REVIEW ARTICLE | JUNE 28 2024

Roadmap on photonic metasurfaces

Sebastian A. Schulz  ; Rupert. F. Oulton  ; Mitchell Kenney  ; Andrea Alù ; Isabelle Staude ;
Ayesheh Bashiri ; Zlata Fedorova ; Radoslaw Kolkowski ; A. Femius Koenderink ; Xiaofei Xiao ;
John Yang ; William J. Peveler ; Alasdair W. Clark ; George Perrakis ; Anna C. Tasolamprou ;
Maria Kafesaki ; Anastasiia Zaleska ; Wayne Dickson ; David Richards ; Anatoly Zayats ;
Haoran Ren ; Yuri Kivshar; Stefan Maier ; Xianzhong Chen ; Muhammad Afnan Ansari ;
Yuhui Gan ; Arseny Alexeev ; Thomas F. Krauss ; Andrea Di Falco ; Sylvain D. Gennaro ;
Tomás Santiago-Cruz ; Igal Brener ; Maria V. Chekhova ; Ren-Min Ma ; Viola V. Vogler-Neuling ;
Helena C. Weigand ; Ülle-Linda Talts ; Irene Occhiodori; Rachel Grange ; Mohsen Rahmani ;
Lei Xu ; S. M. Kamali; E. Arababi; Andrei Faraon ; Anthony C. Harwood ; Stefano Vezzoli;
Riccardo Sapienza ; Philippe Lalanne ; Alexandre Dmitriev ; Carsten Rockstuhl ;
Alexander Sprafke ; Kevin Vynck ; Jeremy Upham ; M. Zahirul Alam; Israel De Leon ;
Robert W. Boyd ; Willie J. Padilla ; Jordan M. Malof; Aloke Jana ; Zijin Yang ; Rémi Colom;
Qinghua Song ; Patrice Genevet ; Karim Achouri ; Andrey B. Evlyukhin ; Ulrich Lemmer ;
Ivan Fernandez-Corbaton

Appl. Phys. Lett. 124, 260701 (2024)

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Roadmap on photonic metasurfaces

Cite as: Appl. Phys. Lett. 124, 260701 (2024); doi: 10.1063/5.0204694
Submitted: 22 February 2024 . Accepted: 18 May 2024 .
Published Online: 28 June 2024

Sebastian A. Schulz,1,a) Rupert. F. Oulton,2,a) Mitchell Kenney,3,a) ,4,5

Andrea Alu Isabelle Staude,6
6 6 7
Ayesheh Bashiri, Zlata Fedorova, Radoslaw Kolkowski, A. Femius Koenderink,8 Xiaofei Xiao,2
John Yang,2 William J. Peveler,9 Alasdair W. Clark,10 George Perrakis,11 Anna C. Tasolamprou,12
Maria Kafesaki,11,13 Anastasiia Zaleska,14 Wayne Dickson,14 David Richards,14 Anatoly Zayats,14
15 16 15,17 18
Haoran Ren, Yuri Kivshar, Stefan Maier, Xianzhong Chen, Muhammad Afnan Ansari,18
19 20 21
Yuhui Gan, Arseny Alexeev, Thomas F. Krauss, Andrea Di Falco,19 Sylvain D. Gennaro,22
Toma s Santiago-Cruz,23 Igal Brener,23 Maria V. Chekhova,24 Ren-Min Ma,25 Viola V. Vogler-Neuling,26
Helena C. Weigand, 27 €
Ulle-Linda Talts, 27 27
Irene Occhiodori, Rachel Grange, 27
Mohsen Rahmani,28
28 29 30 31 2
Lei Xu, S. M. Kamali, E. Arababi, Andrei Faraon, Anthony C. Harwood, Stefano Vezzoli,2
2 32 33
Riccardo Sapienza, Philippe Lalanne, Alexandre Dmitriev, Carsten Rockstuhl,34,35
Alexander Sprafke,36 Kevin Vynck,37 Jeremy Upham,38,39 M. Zahirul Alam,38,39 Israel De Leon,40,41
Robert W. Boyd,38,39 Willie J. Padilla,42 Jordan M. Malof,43 Aloke Jana,44 Zijin Yang,45 Re mi Colom,46
45 44 47 48,49
Qinghua Song, Patrice Genevet, Karim Achouri, Andrey B. Evlyukhin, Ulrich Lemmer,50,51
35
and Ivan Fernandez-Corbaton

For affiliations, please see the end of the Reference section.

12 April 2025 [Link]

a)
Authors to whom correspondence should be addressed: sas35@[Link]; [Link]@[Link];
and [Link]@[Link]

ABSTRACT
Here we present a roadmap on Photonic metasurfaces. This document consists of a number of perspective articles on different applications,
challenge areas or technologies underlying photonic metasurfaces. Each perspective will introduce the topic, present a state of the art as well
as give an insight into the future direction of the subfield.
V
C 2024 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (https://

[Link]/licenses/by/4.0/). [Link]

TABLE OF CONTENTS C. Future directions and outlook. . . . . . . . . . . . . . . . . . 10

1. Materials and their integration . . . . . . . . . . . . . . 10
EDITORIAL . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3 2. Fabrication challenges . . . . . . . . . . . . . . . . . . . . . 11
I. PERSPECTIVE ON PHOTONIC METASURFACES . . . . 4 3. Emission stability . . . . . . . . . . . . . . . . . . . . . . . . . 11
A. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4 4. Magnetic dipole transitions . . . . . . . . . . . . . . . . . 11
B. State of the art . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4 5. 2D materials and valleytronics . . . . . . . . . . . . . . 11
C. Future directions and outlook. . . . . . . . . . . . . . . . . . 5 6. Emerging trends in metasurface design . . . . . . 11
II. METASURFACES FOR CONTROLLING LIGHT 7. High-power applications . . . . . . . . . . . . . . . . . . . 12
EMISSION. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7 8. Tunable light sources . . . . . . . . . . . . . . . . . . . . . . 12
A. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7 9. Topological, non-Hermitian, and temporal
B. State of the art . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8 effects . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
1. Emission enhancement . . . . . . . . . . . . . . . . . . . . 8 D. Concluding remarks . . . . . . . . . . . . . . . . . . . . . . . . . . 12
2. Shaping the emitted light . . . . . . . . . . . . . . . . . . 9 III. NONLINEAR OPTICAL METASURFACES . . . . . . . . . . 12
3. Dynamic tuning of emission. . . . . . . . . . . . . . . . 10 A. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
4. Chiral light control . . . . . . . . . . . . . . . . . . . . . . . . 10 B. State of the art . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
5. Methods: Design and fabrication . . . . . . . . . . . . 10 1. Local resonance—surface plasmons . . . . . . . . . . 14

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2. Local resonance—Mie and multipolar modes . 14 2. System architectures and technological

3. Local resonance—Fano interference . . . . . . . . . 14 platforms . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38
4. Collective resonance—bound states in the C. Future perspectives . . . . . . . . . . . . . . . . . . . . . . . . . . . 39
continuum . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15 X. METASURFACES FOR QUANTUM STATES
5. Collective resonance—surface lattice GENERATION . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 40
resonance . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15 A. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 40
6. Material resonance—epsilon near zero B. Single-photon generation . . . . . . . . . . . . . . . . . . . . . . 41
materials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15 C. Biphoton generation . . . . . . . . . . . . . . . . . . . . . . . . . . 43
7. Integrating metasurfaces with nonlinear D. Future directions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 45
materials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15 XI. METASURFACE LASERS. . . . . . . . . . . . . . . . . . . . . . . . . . 46
8. Nonlinear metasurface selection rules . . . . . . . . 15 A. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 46
C. Nonlinear generation rate and efficiency. . . . . . . . . 15 B. Key performance parameters . . . . . . . . . . . . . . . . . . . 46
D. Future directions of nonlinear optical C. Eigenmode engineering in a single microscale
metasurfaces. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17 laser cavity . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 47
1. Metasurfaces for nonlinear wave-front 1. Enhance laser performance . . . . . . . . . . . . . . . . . 47
control . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17 2. Enhancing local field . . . . . . . . . . . . . . . . . . . . . . 47
2. Metasurfaces for modulation and switching. . . 17 3. Controlling radiation field . . . . . . . . . . . . . . . . . . 47
3. Reduced power non-perturbative nonlinear D. Eigenmode engineering in arrayed lasers . . . . . . . . 47
optics. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17 1. Large area single mode . . . . . . . . . . . . . . . . . . . . 47
IV. METASURFACES FOR BIOSENSING. . . . . . . . . . . . . . . 17 2. High dimensional radiation. . . . . . . . . . . . . . . . . 49
A. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17 3. Reconfigurable phased array nanolasers . . . . . . 49
B. Biosensors: Plasmonic vs dielectric . . . . . . . . . . . . . . 18 E. Future directions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 49
C. Biosensing. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18 F. Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 50
D. Refractometric sensors . . . . . . . . . . . . . . . . . . . . . . . . 18 XII. SOLUTION-DERIVED NANOFABRICATION FOR
E. Plasmonic refractometric sensors . . . . . . . . . . . . . . . 18 NONLINEAR METASTRUCTURES . . . . . . . . . . . . . . . . 50
F. Dielectric refractometric sensors . . . . . . . . . . . . . . . . 19 A. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 50
G. Chiral sensors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19 B. Nanoimprint and solution derived principles and

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H. Enhanced vibrational spectroscopy . . . . . . . . . . . . . 19 advantages. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 50
I. Nanoholes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 20 C. The challenges of solution-based processing of
J. Future directions and outlook—cross-reactive metasurfaces . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 51
metasurface biosensors. . . . . . . . . . . . . . . . . . . . . . . . . 20 D. Roadmap towards high-performing solution-
V. METASURFACES FOR PASSIVE RADIATIVE based metasurfaces . . . . . . . . . . . . . . . . . . . . . . . . . . . 52
COOLING. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 22 E. Future directions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 53
A. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 22 1. Exploration of other materials and processes. . 53
B. State of the art . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 23 2. Nonlinear applications with high scalability,
C. Future directions and outlook. . . . . . . . . . . . . . . . . . 25 transparency ranges, robustness, and
VI. METASURFACES FOR PHOTOCATALYSIS. . . . . . . . . 26 dimensionality . . . . . . . . . . . . . . . . . . . . . . . . . . . . 53
A. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 26 3. Unexplored properties and more fundamental
B. State of the art . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 27 aspects. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 54
C. Future directions and outlook. . . . . . . . . . . . . . . . . . 29 XIII. SEMICONDUCTOR METASURFACES:
D. Concluding remarks . . . . . . . . . . . . . . . . . . . . . . . . . . 30 MATERIALS AND NANOFABRICATION
VII. ORBITAL ANGULAR MOMENTUM AND APPROACHES. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 54
WAVEFRONT CONTROL . . . . . . . . . . . . . . . . . . . . . . . . 30 A. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 54
A. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 30 B. Semiconductor metasurfaces and fabrication
B. State-of-the-art . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 30 challenges . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 54
C. Future directions and outlook. . . . . . . . . . . . . . . . . . 32 C. Group IV semiconductor metasurfaces . . . . . . . . . . 55
VIII. METASURFACES FOR HOLOGRAPHY AND D. Group III–V semiconductor metasurfaces . . . . . . . 55
STRUCTURAL COLOR . . . . . . . . . . . . . . . . . . . . . . . . . . 33 E. Multi-layered semiconductor metasurfaces . . . . . . . 56
A. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 33 F. Metasurfaces made of hybrid and emerging
B. Optical field manipulation in polarization-based materials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 58
holography . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 33 G. Conclusions and future perspectives . . . . . . . . . . . . 58
C. Toward 3D polarization structures: challenges XIV. CONFORMAL AND FLEXIBLE METASURFACES:
and future directions. . . . . . . . . . . . . . . . . . . . . . . . . . 35 A BRIEF PERSPECTIVE . . . . . . . . . . . . . . . . . . . . . . . . . 58
IX. META-OPTICS FOR AUGMENTED REALITY A. Introduction and brief history . . . . . . . . . . . . . . . . . 58
APPLICATIONS . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 37 B. Design, fabrication, and applications . . . . . . . . . . . . 61
A. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 37 1. Optical design . . . . . . . . . . . . . . . . . . . . . . . . . . . . 61
B. State of the art . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38 2. Fabrication techniques . . . . . . . . . . . . . . . . . . . . . 61
1. Parameters . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38 3. Applications . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 62

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C. Challenges, opportunities, and future perspectives 63 2. Numerical implementation . . . . . . . . . . . . . . . . . 91

XV. TIME MODULATED METASURFACES . . . . . . . . . . . . 64 3. Analytical investigations . . . . . . . . . . . . . . . . . . . 92
A. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 64 C. Future directions and outlook. . . . . . . . . . . . . . . . . . 93
B. Time-varying metasurfaces. . . . . . . . . . . . . . . . . . . . . 64 1. A description using polarizabilities . . . . . . . . . . 93
C. Time-modulation in spatial metasurfaces . . . . . . . . 65 2. Multipolar interface conditions . . . . . . . . . . . . . 94
D. Space-time metasurfaces . . . . . . . . . . . . . . . . . . . . . . 66 3. Further developments. . . . . . . . . . . . . . . . . . . . . . 94
E. Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 67 D. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 95
XVI. DISORDERED OPTICAL METASURFACES:
PHYSICS, THEORY AND DESIGN . . . . . . . . . . . . . . . 67 EDITORIAL
A. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 67
B. State-of-the-art . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 67 Sebastian A. Schulz, Rupert F. Oulton,
1. Diffuse (incoherent) vs. specular (coherent) and Mitchell Kenney
light . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 68
2. Full-wave analysis . . . . . . . . . . . . . . . . . . . . . . . . . 68 sas35@[Link]

3. Approximate models . . . . . . . . . . . . . . . . . . . . . . 69 [Link]@[Link]

4. Fabrication . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 69 [Link]@[Link]
C. Future directions and outlook. . . . . . . . . . . . . . . . . . 70
1. Prospective applications . . . . . . . . . . . . . . . . . . . . 71 Over the last decade, the topic of metasurfaces has flourished like
2. Metasurfaces on curved substrates . . . . . . . . . . . 71 no other field in optics. This is primarily due to the appeal of compact
3. Striving for ultra-low costs with augmented flat optical components with wide design flexibility inherent to these arti-
resilience to fabrication imperfections . . . . . . . . 72 ficial two-dimensional materials. As can be seen in this roadmap, meta-
XVII. FROM PRINCIPLES TO PERFORMANCE: surfaces can be made from a wide range of materials, from metals and
EPSILON-NEAR-ZERO METASURFACES FOR other plasmonic materials to dielectrics and even flexible and conform-
NONLINEAR OPTICAL DEVICES . . . . . . . . . . . . . . . 72 able platforms. In all cases, a metasurface’s overall properties follow not
A. Introduction: The physics of ENZ . . . . . . . . . . . . . . 72 only from the those of the constituent materials but also from the shape
1. Materials with ENZ properties . . . . . . . . . . . . . . 73 and arrangement of meta-atoms, engineered on nanoscopic dimensions.
2. ENZ induced behavior in TCOs. . . . . . . . . . . . . 73 The broad range of metasurface applications available stem from the rich

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3. Incorporating metasurfaces with ENZ physics that emerges from the arrangement and geometry of the meta-
materials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 75 atoms; by arranging these into periodic or disordered distributions, that
4. Metasurfaces exploiting the nonlinear ENZ display local or non-local responses, as well as exhibiting conventional or
response . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 75 topological characteristics, these “design parameters” allow us to influ-
5. Future of applications . . . . . . . . . . . . . . . . . . . . . 77 ence light’s amplitude, phase, polarization, and nonlinearity.
a. Speed of modulation . . . . . . . . . . . . . . . . . . 77 This document offers a comprehensive overview of the physics
b. Absorptive losses . . . . . . . . . . . . . . . . . . . . . 77 and applications of photonic metasurfaces which sets the context for
c. Saturation and damage threshold . . . . . . . 77 discussion of future research directions. As commissioning editors, we
d. Alternative modulation mechanisms . . . . 77 have invited 20 perspectives from the community, where each has given
e. Pushing back technical limits. . . . . . . . . . . 77 equal importance to reviewing the historic development of the field,
B. Perspective on future work . . . . . . . . . . . . . . . . . . . . 77 presenting highlights of current research and then pointing to future
C. Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 78 challenges and outlook. Andrea Alu sets the scene with a general intro-
XVIII. DEEP LEARNING FOR PHOTONIC duction (I). The roadmap is then organized into three sections of per-
METASURFACES. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 78 spectives: ten perspectives on the applications of photonic metasurfaces;
A. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 78 three perspectives on the fabrication and material platforms; and finally,
1. State of the art. . . . . . . . . . . . . . . . . . . . . . . . . . . . 80 six perspectives on the emerging topics and the theory of metasurfaces.
2. Future directions and outlook . . . . . . . . . . . . . . 81 The roadmap explore several key application areas for metasurfaces,
XIX. COMPLEX-VALUED SINGULARITIES FOR including metasurfaces for: the control of light emission (II); nonlinear
METASURFACE DESIGNS . . . . . . . . . . . . . . . . . . . . . . . 83 optics (III); biosensing (IV); passive radiative cooling (V); photocataly-
A. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 83 sis (VI); orbital angular momentum and wavefront control (VII);
B. Designing metasurfaces according to the position holography and structural color (VIII); augmented reality (IX); quan-
of complex-plane zero singularities . . . . . . . . . . . . . 84 tum state generation (X); and finally metasurface based lasers (XI). The
C. Asymmetric full 2p phase engineering based on section on fabrication and material platforms includes solution derived
exceptional points in metasurfaces . . . . . . . . . . . . . . 87 metasurface fabrication (XII); semiconductor based metasurfaces
D. Concluding remarks and future perspective . . . . . . 88 (XIII); and flexible metasurfaces (XIV). The final six perspectives
XX. MULTIPOLAR DESIGN METHODS FOR explore metasurfaces for or with time modulation (XV); disorder
METASURFACES . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 89 (XVI); epsilon-near-zero characteristics (XVII); deep learning (XVIII);
A. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 89 complex-valued singularities (XIX); and, last but not least, multipolar
B. State of the art . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 89 characteristics (XX).
1. Theoretical framework of a multipolar In contrast to previous reviews (e.g., Refs. 1–3) and roadmaps,4
description . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 89 which focus exclusively on either past or future development of the

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field, we have aimed instead to provide a comprehensive overview that truly impressive, leveraging the combination of theoretical advances in
gives equal weight to past, present and future of the selected topics. our understanding of the interactions of light with nanostructures, and
This gives the necessary context for the discussion of future research progress in nanofabrication of a wide range of materials, also over large
directions and outlook whilst also providing a valuable up to date area. In turn, the discoveries driven by photonic metasurface research
resource by indexing the rapidly amassed literature in this field. have also translated back to lower frequencies, where the fields of
This roadmap is truly the culmination of a world-wide effort of reflect- and transmit-arrays, as well as frequency-selective surfaces,
leading contributors from across the metasurface community. We are originally demonstrated wavefront and spectrum control for radio-
grateful for their time, effort, and dedication to this compilation of per- waves, driving the interest in a new wave of hardware platforms known
spectives. We hope that this Roadmap on Photonic Metasurfaces will as reconfigurable intelligent surfaces for wireless communications.19
provide you—the reader—with an up to date reference of the current
status, understanding, and direction of photonic metasurface research; B. State of the art
whether you are already an experienced researcher looking for a con-
The first demonstrations of optical metasurfaces, e.g., Fig. 1(a),
temporary summary of the research and direction of the field or
were limited in terms of efficiency and of functionalities, due to a vari-
whether you are looking for a comprehensive introduction to this fas-
ety of challenges. For the most part, they relied on metallic resonant
cinating area.
elements, associated with significant absorption, and on polarization
I. PERSPECTIVE ON PHOTONIC METASURFACES conversion mechanisms, which tend to be inefficient and limited by
symmetries, to control the amplitude and phase of the scattered fields.

Andrea Alu The overall efficiency and the type of transformations that could be
implemented on the incoming wavefront were significantly limited in
aalu@[Link] these first demonstrations.14 By contrast, over the years new genera-
tions of photonic metasurfaces have flourished into a plethora of excit-
A. Introduction ing functionalities for holography,20 multi-functional and multi-
The field of photonics relies on gaining control over light flows to wavelength operation,21 lensing and imaging,22 and several other
advance a wide and rapidly growing range of technologies, including impressive demonstrations of complex wavefront shaping using ultra-
energy, sensing, imaging, and computing. Photonics research has been thin optical devices, becoming competitive with bulky optical technol-
recently unveiling exciting opportunities both in the context of basic ogies in terms of several performance metrics. Figure 1 shows a few

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science and of its engineering and technological impact. A major role demonstrations of the state of the art of this technology, in which tai-
in this recent progress has been played by ultrathin surfaces engineered lored nanostructured apertures are able to imprint the desired wave-
at the nanoscale, known as metasurfaces,5 which have been enhancing front to the electromagnetic fields at the wavelength of interest. Figure
the way we tailor optical wavefronts over an ultrathin platform, open- 1(b), for instance, shows high-efficiency holograms created by tailored
ing a paradigm of compactification of photonic devices for extreme nanostructured surfaces, and Fig. 1(c) an ultrathin metalens that can
light control. In turn, metasurfaces have also been unveiling unique focus light at multiple frequencies.
forms of light–matter interactions emerging from their subwavelength Several design principles have been explored to tailor the optical
light confinement and extreme light control at the nanoscale. The wavefront, spanning from coupled resonances locally tuned to control
recent surge of interest for metasurfaces in the photonics community the amplitude and phase23 to polarization conversion5 and geometric
has been driven by the introduction of the “generalized Snell’s laws of phase concepts,24 each coming with their own advantages and trade-
refraction,”5,6 according to which a transverse gradient of phase dis- offs. For instance, coupled resonances tend to introduce unwanted fre-
continuities imparted by a tailored array of nanostructures can offer quency dispersion, modulating the scattering amplitude as we tailor
enhanced control over wave transmission through a planar interface. the local phase of each metasurface elements. Polarization conversion
These concepts have been building on well-established technologies in can powerfully tailor the phase of the scattered fields, but its efficiency
the realm of microwave components7,8 and “flat” diffractive optical is typically limited. Geometric phase concepts can partially address
elements,9,10 established fields of research for several decades. Over the these challenges, but they are conventionally limited to circularly
years, more sophisticated metasurface designs have been demonstrat- polarized responses.
ing further mastery over all properties of light, enhancing efficiency, While all these design principles offer a powerful playground for
bandwidth, polarization, and wavefront control through metasurfa- wavefront control, metasurfaces often face fundamental constraints in
ces,11–16 which, in turn, have been translated into ultrathin devices for terms of efficiency and bandwidth of wavefront manipulation, which
lensing, holograms and lasing, among many other applications. stem from their ultrathin footprint and inherent symmetry constraints.
While the early demonstrations of metasurfaces were mostly Over the years, several of these bounds have been unveiled,11,14,25,26
based on plasmonic nanostructures, which enable field enhancement indicating that extreme compactification of optical devices comes at a
and light focusing at deeply subwavelength scales, the associated mate- price, which needs to be taken into account when compared to other
rial loss have driven the field toward alternative materials, including more bulky solutions. For instance, it is hard to imagine that a fully
high-index dielectrics and doped semiconductors. Today, the possibili- metasurface-based approach may be able to compete with a sophisti-
ties offered by metasurfaces to efficiently control light with nanoscale cated EOS camera lens, but metasurfaces may be able to replace spe-
resolution over an ultrathin platform have translated into myriads of cific components. Hybrid approaches leveraging metasurfaces appear
opportunities, not only limited to high-profile academic research, but to be certainly competitive, and metasurfaces may be excellent at spe-
also to commercial companies.17,18 The progress in this area has been cific tasks, or for targeted wavelengths of operation.

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FIG. 1. Metasurfaces for wavefront control. (a) Generalized laws of refraction for beam steering through phase gradients (reproduced with permission from Yu et al., Science
334, 333 (2011). Copyright 2011 AAAS;5 (b) metasurface holograms with high efficiency (from Ref. 20); (c) multi-wavelength, polarization-insensitive metalenses (from Ref. 21).
All images are reprinted (adapted) with permission from the respective Journal and copyright remains with the original publisher.

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While the conventional approach to metasurface design has C. Future directions and outlook
been the one of locally patterning the aperture with nanoscale reso- The opportunities for photonic metasurfaces have been growing by
nators that control point by point the response, a few more recent the day, fostered by continuous progress on multiple fronts, which drives
approaches have been opening new design degrees of freedom. For the future of this research area. From the modeling perspective, enhanc-
instance, metagratings27,28 have been demonstrating that extreme ing the ultimate performance of metasurfaces requires sophisticated
control over the optical wavefront can be achieved with high effi- modeling tools that can capture and optimize their design. Given that
ciency, for instance yielding near-grazing beam steering. most metasurfaces are non-periodic, rational design tools, fast simulation
Metagratings are based on grating resonances that stem from an and optimization techniques have been emerging as exciting prospects,
overarching long-range periodicity of the structure, while the indi- for instance in the context of adjoint methods, topology optimization
vidual metasurface elements are designed to control the way the and machine learning. Physics-driven design and optimization
incident wavefront locally couples to the available diffraction approaches, such as the use of singularities in the complex frequency
orders. These principles have been further empowered by nonlocal plane, topological concepts, bound states in the continuum (BIC) and
metasurfaces, in which the coupling among distant elements across exceptional points are emerging directions that unveil new optical phe-
the metasurface aperture is not fought against, but rather leveraged nomena and add new designer tools for photonic metasurfaces.37–40
through more sophisticated design principles that exploit lattice Emerging applications of nonlocal metasurfaces include the pos-
resonances locally perturbed by symmetry-breaking defects.29 sibility of filtering and processing images in momentum space, realiz-
Nonlocal metasurfaces provide a more sophisticated control over ing Fourier and even nonlinear operations over an ultrathin, efficient
the spectral response, and open new opportunities for wavefront platform. The idea is to leverage the engineered nonlocality in meta-
manipulation, including wavefront selectivity,30 and multi- surfaces to perform mathematical operations on the incoming
functionality.31 images,41–43 and even realize optical analog computers that can solve
The recent progress in metasurface design principles, fabrication complex mathematical problems44–46 [Figs. 3(a) and 3(b)]. Tailored
and also tunability of their response has led to a surge of exciting appli- nonlocalities in metasurfaces can also add spatial and temporal coher-
cations. Figure 2 summarizes a few relevant highlights of metasurfaces ence, ideally suited to pattern and control thermal emission and photo-
that realize complex structured wavefronts, relevant for e.g., optical luminescence. These ideas are paving the way to the realization of
communications and holography,32 for eye tracking applications,33 for ultrathin surfaces that emit tailored wavefronts with desired amplitude,
quantum technologies,36 for catalysis and chemical reactions,34 and for phase, and polarization without the need for an external coherent
augmented reality (AR).35 These breadth of applications holds the source driving them.47,48 Figure 3(c) shows a thermal metasurface,
promise of a vibrant future for metasurfaces, opening exciting pros- based on an underlying periodic lattice that can control the degree of
pects for the near future. temporal and spatial coherence endowed to thermal emission, and

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FIG. 2. (a) Metasurface for complex wavefront shaping to impart orbital angular momenta to the impinging light (reproduced with permission from Ren et al., Nat. Commun. 10,
2986 (2019). Copyright 2019 Springer Nature Publishing Group;32 (b) nonlocal metasurface for eyetracking applications (from Ref. 33); (c) concept of metasurfaces to facilitate

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chemical processes (from Ref. 34); (d) metasurface for augmented reality applications (from Ref. 35). All images are reprinted (adapted) with permission from the respective
Journal and copyright remains with the original publisher.

whose local perturbations control the polarization and wavefront On the material front, the use of two-dimensional (2D) materials
shape of thermal emission. Future efforts may be able to demonstrate integrated with metasurfaces, such as graphene51 and transition metal
ultrathin patterned surfaces that embed their own optical sources and dichalcogenides49 [Fig. 3(d)], and even direct patterning of bulk 2D
pattern them with extreme flexibility. materials, holds the promise for exciting opportunities both in the

FIG. 3. (a) Edge detection metasurfaces for image processing and biomedical applications (from Ref. 42); (b) analog optical computing based on nonlocal metasurfaces (from
Refs. 44 and 46); (c) nonlocal metasurface to manipulate thermal emission (from Ref. 47); (d) metasurfaces integrating 2D materials (from Ref. 49); (e) spatiotemporally modu-
lated metasurface to extend the degree of control over wavefront manipulation to space-time diffraction (from Ref. 50). All images are reprinted (adapted) with permission from
the respective Journal and copyright remains with the original publisher.

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context of basic science and applications. These materials offer inter- engineered scattering properties. In contrast to the passive metasurfa-
esting forms of light–matter interactions in the form of plasmon, exci- ces discussed in most other sections of this Roadmap, which manipu-
ton, phonon polaritons, in which light and matter are so intertwined late the light propagating from a distant light source, light-emitting
to form quasi-particles. Combined with metasurface concepts, these metasurfaces incorporate nanoscale light sources in their architecture,
phenomena can further boost light control, and impart exotic photonic allowing the coupling of the emission from the sources to the far-
features to polaritonic responses. Polaritonic materials can be also ide- field.57 Light-emitting metasurfaces offer various functionalities
ally suited to boost optical nonlinearities, opening exciting opportuni- including photoluminescence enhancement,58 tailored emission direc-
ties to extend metasurface operations and wavefront control to tionality,48,59,60 improved quantum efficiency,61 color conversion,62
nonlinear optical processes, such as wave mixing, frequency genera- and controlled degree of coherence,63 thus offering important opportu-
tion, limiting, up- and downconversion.52,53 These materials can also nities for compact and efficient light sources such as lasers (see also
be exciting prospects to efficiently integrate and pattern optical gain in Sec. XI), LEDs,64 and single-photon sources65 for quantum technolo-
metasurfaces, paving the way to a plethora of interesting non- gies (see also Sec. X). Other applications range from displays and opti-
Hermitian wave phenomena.38,39,54 cal communication to biomedical applications, and energy harvesting.
Nonlinearities can also offer powerful tools to reconfigure and Note that, in this section, the term “light emission” specifically refers
modulate in time the metasurface response, which becomes crucial to the fluorescent and photoluminescent sources, while thermal emis-
to make an impact in many technologies. Beyond the importance sion is addressed in Secs. I and V.
of manipulating in real-time the spatial degrees of freedom of the Light-emitting metasurfaces can be categorized into two main
incoming wavefront, creating enhanced forms of spatial light mod- platforms: plasmonic and high-refractive-index all-dielectric.
ulators,55 but also their temporal and frequency content. Suitable Plasmonic metasurfaces are composed of metallic meta-atoms, where
temporal modulation schemes can break reciprocity and efficiently the large confinement of electromagnetic fields in their surroundings
mix frequencies,56 as well as induce nontrivial parametric phenom- can result in a strong reduction of the radiative lifetime of the emitters
ena, including Doppler shifts, and active beam steering,50 largely coupled to the metasurface.66 However, the applicability of these meta-
expanding the reach and opportunities offered by optical metasur- surfaces is limited due to their intrinsic Ohmic losses. All-dielectric
faces, as schematically shown in Fig. 3(e). For various applications, metasurfaces, on the other hand, can exhibit low absorption losses and
real-time dynamic programmability may become necessary moving support both electric and magnetic multipolar Mie-type modes with-
forward the field of metasurfaces, for instance in the context of out demanding complex geometries.67 Multipolar superposition then
image processing, dynamic scene creation, and holograms. The

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allows for tailoring directional properties, e.g., through the Kerker
integration of 2D and polaritonic materials may enable faster and effect, which facilitates applications in beam steering, lensing, and
more efficient forms of modulation.
beam shaping.
Finally, photonic metasurfaces may truly flourish once its realiza-
Various types of emitters have been considered as active compo-
tion becomes fully compatible with large-area and inexpensive fabrica-
nents of light-emitting metasurfaces, such as quantum dots (QDs),
tion techniques, pushing metasurfaces from proof of concept
dyes, and semiconductors. Recently, many studies concentrated on the
implementations to foundry-level production. Roll-to-roll, nanoim-
coupling of optical metasurfaces with 2D materials. In the family of
printing, and self-assembly techniques appear promising in this con-
2D materials, layered systems of transition metal dichalcogenides
text, and efforts to develop design principles compatible with the
(TMDs)68 have attracted special attention due to their unique opto-
constraints of these techniques in terms of materials and disorder tol-
electronic properties, including strong photoluminescence, excitonic
erance are becoming necessary. Overall, photonic metasurfaces have a
response at room temperature, and circular dichroism caused by their
bright future ahead, continuously evolving along the years with new
valley-selective optical transitions.69
concepts, new material playgrounds and a highly interdisciplinary
The key mechanism for controlling light emission by metasurfa-
broad research community. As the field continues to mature, the exotic
wave phenomena at the basis of photonic metasurfaces are empower- ces is the engineering of the local density of photonic states (LDOS)
ing photonic technologies and exciting several industries. through either the localized resonances provided by individual meta-
atoms or the collective resonances originating from their overall
ACKNOWLEDGMENTS arrangement or both. In periodic metasurfaces, collective resonances
Our work on these topics has been supported by the Simons can be regarded as photonic Bloch bands (as in photonic crystals)
Foundation and the Air Force Office of Scientific Research. transformed by the resonant meta-atoms into surface lattice resonan-
ces (SLRs).70 They also include dark modes and quasi bound states in
II. METASURFACES FOR CONTROLLING LIGHT the continuum (quasi-BICs), in which radiative loss is suppressed by
EMISSION destructive interference.71 Collective resonances can provide high
LDOS at the band edges, together with control of spatial coherence
Ayesheh Bashiri, Zlata Fedorova, Radoslaw Kolkowski, and directivity of emission.59,72 Engineering the individual meta-atoms
A. Femius Koenderink, and Isabelle Staude allows to further tailor the light emission properties, employing both
local and nonlocal effects. For example, asymmetric meta-atoms may
[Link]@[Link] allow a controlled fraction of the light to be radiated away by turning
the perfectly nonradiating BICs into quasi-BICs.73 Moreover, spatial
A. Introduction variation of the meta-atom design can allow for the emission of light
Optical metasurfaces are two-dimensional (2D) arrangements of fields with shaped wavefronts through metasurface defined spatially
subwavelength scale building blocks known as meta-atoms with varying phase or amplitude profiles.48,60,74

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Although most of the light-emitting metasurfaces demonstrated different types of emitters. For applications like, e.g., AR glasses, it is
so far facilitate tailoring of spontaneous emission in the weak coupling not overall emission power output that matters, but the combination
regime, their potential for strong coupling and lasing has also been of emissive behavior with transparency for most of the ambient light.
demonstrated.75,76 The latter is discussed in detail in Sec. XI. Some factors are relevant for multiple applications, e.g., brightness,
Semiclassical strong coupling (ensemble of many emitters) is achieved photostability, power efficiency, fabrication reliability, scalability,
when the coupling rate of emitters to the photonic resonances exceeds and cost. In addition, a frequently desired property is post-
the photonic loss rate, and the rate of spontaneous decay is gauged by fabrication tunability. Modulating the emission and/or achieving
the emission spectral bandwidth. This can be achieved by aligning the multiple and adjustable functionalities in one design are the key fea-
active material’s emission bandwidth with metasurface resonances fea- tures of light-emitting metasurfaces that can bring them closer to
turing sharp line widths while aiming to maximize the oscillator real-world applications.77
strength of the dipole transition. Low-threshold lasers, on the other Figure 4 summarizes many of the aspects of light-emitting meta-
hand, require high-quality (high-Q) optical cavities and precise spatial surfaces discussed in this section.
and spectral overlap of their modes with the gain material. This can be
achieved by engineering the parameters of the metasurface integrated B. State of the art
with the gain medium.
1. Emission enhancement
The relevant performance factors for light-emitting metasurfa-
ces depend on the specific target application. For instance, to impact The emission from nanoscale light sources incorporated into
high-power LED lighting one must contend with 0.5–1 A/mm2 cur- metasurfaces can be tailored through a modification of excitation rate
rent density (blue emitting LEDs), or equivalently for phosphor con- (for optical pumping), of radiative decay rate, and of directionality of
verting layer of order 1 W/mm2 emitted power, and 1 W/mm2 the emission.78 Metasurfaces can strongly confine the excitation field
thermal load due to the Stokes shift. This places huge challenges on in the emissive layer, resulting in an efficient incoupling and further
photostability and absorption coefficients. Another application is enhancement of the emission. Radiative decay rate enhancement is
light sources for projection or image-projecting metasurfaces. In associated with the Purcell effect and achieved through modifications
contrast to general lighting, such applications require a small eten- of the LDOS by resonant metasurfaces. For classical cavities, it is well
due. Metasurface-based displays must emit a set of selected wave- known that the Purcell factor scales approximately with the ratio of
lengths, which can be achieved, e.g., by energy transfer between the quality factor Q and the mode volume V. Simple Mie-resonant all-

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FIG. 4. Summary of the key aspects of light-emitting metasurfaces discussed in this chapter including material platforms, physical mechanisms, desired functionality, perfor-
mance requirements, as well as future goals.

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dielectric metasurfaces exhibit Q-factors on the order of 10–100 and been demonstrated, e.g., in a plasmon-exciton-polariton laser, exhibit-
moderate Purcell factors.79 However, they contribute effectively to the ing a reduced threshold in the strong coupling regime.82
radiative decay rate enhancement due to their negligible absorption
losses. This is especially beneficial for emitters with intrinsically high
quantum yields. In contrast, plasmonic metasurfaces can offer much 2. Shaping the emitted light
smaller mode volumes, resulting in larger Purcell factors,80 at the cost
of enhancing both the radiative and nonradiative decay rate, thus Other crucial enabling features of metasurfaces are their areal
reducing the quantum yield for highly efficient emitters. Hence, they nature and the diversity of far-field spatial character that their modes
can only be usefully employed for boosting the quantum yield of rather can be engineered to support, in particular for spatially varying archi-
inefficient emitters78 or should be operated in the regime of high-Q tectures. As such, the radiative decay rate enhancement can also serve
SLRs, where the hybridization between plasmon and diffraction reso- to tailor the emission directionality by channeling the emitted light
nances is tuned to trade in plasmonic confinement for the quality fac- into carefully tailored spatial modes. This is usually achieved by adjust-
tor. Indeed, collective metasurface resonances such as SLRs or quasi- ing the meta-atom geometry or their arrangement,83 which can span
BICs generally support significantly high Q-factors (in particular for from a basic periodic lattice to a complex, spatially inhomogeneous
low-loss dielectric implementations) at the cost of relatively high mode distribution, as well as the substrate/superstrate material. Tailoring
volumes. The high Q-factors make them suitable for lasing, entangled- directionality is key for realizing light-emitting devices with efficient
photon generation, and luminescence enhancement.71 For example, a outcoupling,84 emission into a reduced solid angle for augmented/vir-
40-fold enhancement by quasi-BIC for color centers in silicon meta- tual reality (AR/VR) applications35 and generating arbitrary emission
surfaces has been reported81 [see Figs. 5(a)–5(d)]. For germanium patterns,48,60,85 e.g., for projectors or light-field displays. The combina-
QDs, over three orders of magnitude luminescence enhancement was tion of the high Q-factors and topological properties of quasi-BICs can
obtained in dielectric Fano-resonant metasurfaces.58 Efficient lasing also be harnessed for beam shaping, e.g., for generation of vortex laser
and strong coupling enabled by collective metasurface resonances have beams.86

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FIG. 5. (a) Schematic illustration of a silicon metasurface supporting high-Q quasi-BIC resonances; (b) SEM images of the fabricated metasurface; (c) illustration of the carbon
G-centers on the side walls of the etch holes; (d) emission from the carbon G-centers resonantly enhanced by the quasi-BIC [(a)–(d) from Ref. 81]; (e) illustration of chiral emis-
sion due to circularly polarized states (CPS) originating from BIC in a metasurface with broken symmetry; (f) distribution of polarization vectors in the momentum space, with a
pair of CPS shown as red and blue dots (topological charges 61/2); (g) SEM images of the fabricated metasurface; (h) enhanced circularly polarized emission from polycar-
bonate (PC) film doped with 2-methyl-6–(4-dimethylaminostyryl)-4H-pyran (DCM) deposited on the metasurface [(e)–(h) from Ref. 87]; (i) schematic of a single layer TMD inte-
grated with an achiral dielectric metasurfaces for controlling valleytronic emission; (j) detected valley resolved photoluminescence of excitons and trions upon left-handed and
right-handed circularly polarized laser excitation for structure shown in (i); (k) measured trion and exciton degree of polarization, for structure shown in (i) [(i)–(k) from Ref. 69)];
(l) schematic of a polymer layer containing Eu3þ compound integrated with a broken symmetry TiO2 metasurface for tailoring directionality and fluorescence enhancement of
MD transitions; (m) measured fluorescence spectra for the metasurface scheme shown in (l) (red curve) normalized to the spectra of the substrate (blue curve); (n) measured
back focal plane images of (n) MD and (o) ED transitions coupled to the metasurface shown in (l) [(l)–(o) from Ref. 72]. All images are reprinted (adapted) with permission from
the respective Journal and copyright remains with the original publisher.

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3. Dynamic tuning of emission for near-field reconstruction. FEM and FDTD can simulate both peri-
odic structures with plane wave excitation and finite structures with
Many envisioned applications of light-emitting metasurfaces
open boundary conditions. Importantly, for light-emitting metasurfa-
require dynamic, controllable, and reversible modulation of light emis-
ces, point dipole excitation mimicking a nanoscale emitter is possible
sion. Such post-fabrication tunability can be achieved using active
for these techniques.96 Emission calculations for infinite periodic sys-
materials, which change their optical properties under electrical, opti-
tems are not as straightforward, since periodic boundary conditions
cal, or thermal stimuli. Recently, sub-picosecond modulation of photo-
replicate a single emitter in the unit cell to an infinite coherent periodic
luminescence has been achieved in semiconductor metasurfaces
set. For such systems a Floquet transformation is required, also known
through optically induced free-carrier effects,88 which constitutes the
in the RF antenna community as the so-called “array scanning
current state of the art in modulation speed. On the other hand, large
method.”97 Alternatively, reciprocity-based methods that relate fluo-
modulation depths can be provided by liquid crystals (LCs) or chang-
rescence to absorption can be used, which are particularly powerful to
ing the metasurface geometry, e.g., by stretchable deformation or using
simulate extended ensembles of incoherent emitters.98
micro-electro-mechanical systems (MEMS). The use of both
Among the nanofabrication techniques, electron beam lithography
approaches for actively tuning spontaneous emission has already been
(EBL) and focused ion beam milling (FIB) provide state-of-the-art nano-
demonstrated,89,90 making them promising future platforms for
scale precision while preserving high flexibility, and were generally
dynamic light-emitting metasurface devices.
empowering research on metasurfaces over the last decade.99 The key
challenge for the fabrication of light-emitting metasurfaces is the integra-
4. Chiral light control
tion of nanoscale emitters into the metasurface architecture. Typically,
Moreover, an important area of application for light-emitting this is achieved either by fabricating the metasurfaces directly from
metasurfaces is the creation and manipulation of circularly polarized light-emitting materials or by hybridizing passive metasurfaces with
light—a property that is often desired in classical and quantum optical active materials post-fabrication. A typical materials choice for the first
information processing, communication, sensing, and displays. Several approach are direct bandgap semiconductors, including epitaxially
strategies have emerged in this field. In one scenario, circular polariza- grown structures incorporating quantum wells or quantum dots.100 The
tion of the emission is enforced by the metasurface design, while the latter approach can be achieved, e.g., by spin-coating the metasurfaces
emitter can be arbitrary. This can be achieved, e.g., by using chiral meta- with nanoemitter or dye-containing polymers100,101 or by depositing or
atoms, photonic spin-valley locking91 or optical Rashba effect, where chemically binding emitters such as QDs on the surface. 2D or layered

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lack of inversion symmetry causes splitting of optical spin-polarized active semiconductors are obtained from bulk crystals via exfoliation or
states in momentum space. Alternatively, the utilization of chiral quasi- grown directly by chemical vapor deposition (CVD). Among the inte-
BICs was introduced as a compelling method for narrowband direc- gration techniques, one distinguishes dry and wet transfer as well as vari-
tional chiral light emission87 [see Figs. 5(e)–5(h)]. In the second sce- ous strategies of direct integration.68
nario, chiral metasurfaces are combined with emitters of circularly
polarized light. Prominent examples include the usage of chiral metasur- C. Future directions and outlook
faces for circular dichroism enhancement or selective coupling with
valley-polarized excitons in 2D TMDs. The latter is often motivated by While the field of light-emitting metasurfaces has witnessed sig-
the demands of valleytronics. As to the valleytronic applications of chiral nificant progress to date, several challenges remain to be overcome to
metasurfaces, they, however, face notable limitations as they often pro- further develop the metasurface platforms for future practical applica-
mote only one specific valley and would require nanoantenna geometry tions. Here, we provide some suggestions for progress in this regard.
changes for switching. This leads us to the third scenario, where achiral
metasurfaces enable control over the circularly polarized emission. 1. Materials and their integration
Specifically, achiral metasurfaces were proven to allow for control of the
As light-emitting metasurfaces consist of two primary compo-
lifetime, the degree of valley polarization, and the spectral shape of chiral
nents, namely the metasurface itself and the nanoscale emitter, robust
2D TMD emission.69,92 An example of chiral 2D TMDs coupled to the
material platforms for both, as well as effective integration techniques
achiral metasurfaces is shown in Figs. 5(i)–5(k). However, a comprehen-
are required. Importantly, high radiation efficiencies can only be
sive understanding of the coupling mechanisms in such complex hybrid
obtained by using dielectric materials with minimal losses. With much
systems, which would be essential for testing their applicability for val-
leytronics, is still missing. Notably, coherent coupling between excitons of the recent research on passive metasurfaces resorting to a conve-
and meta-atom resonances offers new avenues for the tunability of chiral nient implementation in silicon, metasurfaces made from wide-
properties, including via the magneto-optical effect.93 bandgap materials such as titanium dioxide (TiO2), gallium phosphide
(GaP), zirconium dioxide (ZrO2), or lithium niobate (LiNbO3) can be
game-changers for the visible spectral range, which is of particular
5. Methods: Design and fabrication
interest for applications of light-emitting metasurfaces.
Various numerical methods, including rigorous coupled-wave Regarding the emitters, high quantum efficiency along with
analysis (RCWA), finite element method (FEM), and finite-difference strong optical and thermal stability is desired. Importantly, for both
time-domain (FDTD), are used to simulate light-emitting metasurfa- metasurface and emitters, fitting the industrial needs and compatibility
ces.94,95 RCWA is well-suited for periodic metasurfaces with low with electrical devices must be considered. Here, electrical driving
refractive index contrast excited by plane waves, and directly computes schemes are of particular interest, considering that most research
reflected and transmitted diffraction orders, but requires extra steps works on light-emitting metasurfaces still rely on optical pumping.

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As such, many hybrid material platforms and integration consequence of a selection rule forbidden ED transition.107 Due to a
schemes remain to be explored. For example, fluorescent ions such as strong optical magnetic response, all-dielectric metasurfaces were sug-
trivalent lanthanides could be doped into the constituent materials of gested as exquisite candidates for tailoring the fluorescence properties
the metasurface during the fabrication process or implanted afterwards of MD transitions, opening an exciting pathway toward exploring
using ion implantation. magnetic light–matter interactions at the nanoscale57,72 [see Figs. 5(l)–
5(o)]. A particular challenge associated with commonly studied MD
2. Fabrication challenges transitions is their slower radiative decay rate and consequently lower
emission intensity compared to their ED counterparts. However, in a
Apart from materials and integration, important challenges recent study, a significantly bright and fast optical-frequency MD radi-
remain in terms of nanofabrication. First, Q-factors in low-loss quasi- ation is identified in 2D hybrid organic-inorganic perovskites (HOIPs)
BIC metasurfaces are currently limited by fabrication imperfections such as butylammonium lead iodide (BA2PbI4).108 It is shown that the
such as roughness.102 Thus, it is highly desirable to further improve MD radiative rate in such systems is up to 3 orders of magnitude faster
the structure quality to unlock a range of effects dependent on high Q- than previously established MD transitions. Additionally, similar to tri-
factors. Second, another grand challenge in terms of fabrication, espe- valent lanthanides, 2D HOIPs exhibit spectrally separated ED and MD
cially regarding application perspectives, is scalability. While this holds radiations. MD radiation properties, e.g., emission directionality of
for most metasurface applications, the challenge is even greater for such emitters, can be engineered by integrating them with suitable
light-emitting metasurfaces due to the need to integrate the active nanophotonic platforms. Particularly, metasurfaces supporting high-Q
material. For example, although deep-UV photolithography has been resonances are elegant tools for enabling directional color and/or
proposed as a viable solution for complementary metal–oxide–semi- polarization routing of the emission from MD and ED transition
conductor (CMOS)-compatible wafer-scale metasurface production,103 channels. This opens new perspectives on realizing spectrometer-free,
light-emitting materials are usually not CMOS-compatible, requiring low-loss, and CMOS-compatible nanophotonic devices for imaging,
new approaches to be developed. For example, a combination of nano- sensing, and probing.
imprint lithography and selective area sublimation has been proposed
for large-scale production of GaN light-emitting metasurfaces.104 5. 2D materials and valleytronics
Other alternatives may include, e.g., laser-induced transfer, suitable for
creating large-scale periodic arrays of light-emitting nanoparticles.105 When dealing with 2D materials as active components, their
Third, the precise and deterministic placement of the active material ultrathin nature presents both advantages and drawbacks. Notably, it

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only at desired locations within the metasurface geometry still presents entails limited overlap with the excitation field, resulting in a low signal
a challenge. This can be, e.g., the gap between two meta-atoms where in absolute units. To address this, employing high-Q metasurfaces is
the fields are significantly enhanced, asymmetric locations within the needed to boost local pump field enhancements, while also being key
unit cell for beam-steering effects, or positions featuring specific local for superior Purcell enhancements. A significant limitation of all val-
field characteristics such as chiral density. Suitable placement strategies leytronic devices is the cryogenic temperature requirement due to the
may be adopted from the field of nanoantennas, with approaches rely- presence of phonon-assisted intervalley scattering that prohibits valley
ing on two-step electron-beam lithography showing particular poten- polarization under normal conditions. A promising avenue toward
tial for metasurfaces. The large areas that the metasurface spans also realizing non-zero valley polarization at room temperature involves
suggest that nanoimprint methods may be used to print emissive the utilization of TMD-containing van-der-Waals heterostructures.
materials in a registry with meta-atoms if sufficiently precise spatial These artificial materials can support a flurry of interesting effects and
registration can be achieved. applications, one of them being that valley polarization can be aug-
mented through mechanisms such as charge or spin transfer and other
3. Emission stability proximity effects. Adding to the general fabrication challenge, for real-
istic device applications methods for scalable and high-quality fabrica-
A critical issue concerning a wide range of emitters, spanning tion of 2D materials and heterostructures have to be developed. Here,
from fluorescent dyes to QDs and perovskites is photobleaching, where the CVD-based phase engineering techniques can pave the way for
the excess energy delivered during the excitation process results in the novel heterostructures and junctions with unique electronic phases
reduction of the emitted light intensity from the emitters over time. and customized properties.
Photobleaching is attributed to both pumping conditions and intrinsic
properties of the emitters. Therefore, an adequate emitter choice is cru- 6. Emerging trends in metasurface design
cial for minimizing sample photodamage. In this regard, interesting
opportunities may be offered by highly stable emitters like nitrogen Regarding the design of light-emitting metasurfaces, a grand chal-
vacancies and nanodiamonds.106 lenge is posed by the high computational demand of suitable
approaches like those based on the reciprocity principle. These
4. Magnetic dipole transitions demands are typically higher than for other metasurface applications:
the emission process needs multi-wavelength (optically pumped) and
The light–matter interaction in the optical frequency range multi-physics analysis (including, e.g., electrical and thermal effects),
mainly refers to the interaction of the electric field with electric dipolar coherent or incoherent summing over many source positions, and
(ED) electronic transitions. However, certain solid-state emitters, such when translated by reciprocity into a scattering problem it involves a
as trivalent lanthanides and transition-metal-doped crystals, exhibit continuum of wave vectors. Finally, emissive devices such as LEDs
robust magnetic dipolar (MD)-dominated electronic transitions as a often rely on metasurfaces in complex vertically stratified stacks.

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Generally in metasurface research, there is a growing preference for mode lasing.113 Photonic systems with gain and loss can support non-
optimization algorithms over human-driven approaches due to their Hermitian features known as exceptional points (EPs), which can be
capability of efficient systematic investigation of parameters, as detailed used to control the directionality and polarization of emitted light.54 In
in Secs. XVIII and XX. New, highly performing algorithms may thus temporal photonics, sufficiently fast time modulation can give rise to
prove especially useful for active architectures and help to come up exotic physical phenomena related to light emission and lasing, such
with spatially variant architectures of unprecedented complexity or as new mechanisms of light amplification.114 Currently, the concepts
help to tackle specific design issues associated with the integration of of topological, non-Hermitian, and temporal photonics remain mainly
emitters. For example, quasi-BICs can be engineered to suppress at the level of fundamental research. However, in the future, some of
absorption losses, enabling, e.g., plasmonic-dielectric metasurfaces these concepts may revolutionize the field of light-emitting metasurfa-
with theoretically arbitrary high Q-factors,109 which can potentially ces, enabling unprecedented performance and novel functionalities.
lead to high-performance metasurface designs incorporating light-
emitting and thus inevitably also absorbing materials. D. Concluding remarks
Light-emitting metasurfaces represent a cutting-edge area of
7. High-power applications
research in nanophotonics, offering dynamic control over the proper-
To be competitive as commercial light sources, metasurfaces ties of emitted light from the incorporated nanoscale light sources.
must reach specific performance values. A challenge for high power Furthermore, thanks to recent developments in the field of nanofabri-
applications, such as LEDs is the required combination of high emitter cation and material processing, light-emitting metasurfaces hold great
density, high emitter efficiency, and resistance to photobleaching and promise for a wide range of practical applications from advanced dis-
thermal load. Inherent to the process of emission is that the Stokes plays and communication systems to imaging devices, sensors, and
shift energy is dissipated as heat, often meaning 0.5–1 eV of dissipated beyond. Although challenges such as energy efficiency and integration
energy for every emitted photon. For example, a metasurface-based with existing technologies need to be addressed to reach their full
LED should withstand of order 1 A/mm2 input current while main- potential, the ongoing research and development in this area lead us to
taining power-to-photon conversion and power handling capacity suf- expect a bright future for advanced light-emitting metasurface devices
ficient for providing 1 W/mm2 emission intensity. These goals require with novel functionalities as well as their integration into real-world
proper material engineering to obtain sufficiently bright and photosta- applications. Finally, metasurfaces also offer a unique platform for
ble emitters—the associated dissipated power, or in the case of a color future scientific applications investigating fundamentally new direc-

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converting layer, the Stokes-energy loss in such systems is also of order tions in the area of light emission.
1 W/mm2. For metasurface lasers, it is important to realize that a very
high benchmark is set by III–V surface-emitting lasers that provide ACKNOWLEDGMENTS
continuous-wave output power on the level of 100 W and brightness I.S., A.B., and Z.F. acknowledge financial support from the
>1 GW/cm2/sr at power-to-photon conversion >0.5 W/A, while Deutsche Forschungsgemeinschaft (DFG, German Research
maintaining decent beam quality (M2). This typically requires large- Foundation) through the International Research Training Group
area single-mode operation, which is particularly challenging for meta- (IRTG) 2675 “Meta-ACTIVE,” Project No. 437527638, and through
surfaces. However, the above figures have recently been approached by the Emmy Noether Program, Project No. STA 1426/2-1. The work
photonic crystal surface-emitting lasers.110 of A.F.K. is part of the Dutch Research Council (NWO) and was
performed at the research institute AMOLF. R.K. acknowledges the
8. Tunable light sources support of the Research Council of Finland (Grant Nos. 347449 and
353758).
In addition to simple light sources, many of the emerging applica-
tions of light-emitting metasurfaces, such as LiFi, LIDAR, AR/VR, III. NONLINEAR OPTICAL METASURFACES
require a reliable way of tuning the emission. In that regard, LCs and
MEMS are the most mature technologies, which are also CMOS- Xiaofei Xiao, John Yang, and Rupert. F. Oulton
compatible and therefore suitable for large-scale and low-cost produc-

tion.89,90 Both approaches can offer a large modulation depth while [Link]@[Link]
providing a modulation speed that is sufficient for most commercial
uses. However, direct integration of MEMS and LCs for specific appli- A. Introduction
cations of light-emitting metasurfaces remains to be developed.
The field of nonlinear optics, emerging in the 1960s alongside
lasers, explores light–matter interactions under extreme light intensi-
9. Topological, non-Hermitian, and temporal effects
ties.115 Effects, such as harmonic generation, three- or four-wave mix-
In addition to the real-world applications, the research on light- ing and parametric amplification, have expanded the operational
emitting metasurfaces continues to explore unconventional directions bandwidth of coherent light sources from the extreme ultraviolet to
such as nontrivial topology,111 non-Hermitian physics/parity-time terahertz and produced methods to measure and control light on ultra-
(PT) symmetry,112 and temporal photonics.50 Topological robustness fast time scales. Applications extend to quantum optics, where para-
enables various systems (including, e.g., photonic topological insula- metric downconversion and spontaneous four-wave mixing produce
tors, BICs) to exhibit fragile properties regardless of imperfections, correlated and entangled photon pairs for quantum enhanced sensing,
which has been studied especially in the context of large-area single- imaging and computing.116–121

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FIG. 6. The variety of mechanisms used in nonlinear optical metasurfaces. (a) Comparison of nonlinear optical medium based on conventional bulk crystals and meta-optics.142
(b) Representative nonlinear optical processes where meta-optics may have unique advantages.142 (c) Illumination of strong enhancement of SHG based on plasmonic reso-
nances in an aluminum nanoantenna array.143 (d) Illustration of the continuous geometry-phase-controlled nonlinear harmonic responses of individual metal nanostructures in
plasmonic metamaterials.144 (e) Schematic of enhanced THG in Silicon nanoparticles driven by magnetic response.145 (f) Enhanced THG in individual Ge nanodisks excited at
an anapole state.146 (g) Illustration of THG in Si nanodisk trimers and its SEM image.147 (h) Schematic of efficient THG enhanced by metal-dielectric hybrid nanoantennas.148
(i) Enhanced high-harmonic generation from an all-dielectric metasurface made of dipolar bar antennas and disk resonators on a sapphire substrate. Inset: level scheme for the
mode coupling in a schematic three-level Fano-resonant system.149 (j) Illustration of the Fano-assistant THG from silicon quadrumers of four a-Si:H nanodisks with SEM image
of the sample in the bottom left corner.150 (k) Illustration of continuous wave SHG enabled by quasi-BIC on gallium phosphide metasurfaces.151 (l) Illustration of the BIC-
assisted SHG in a single nanoresonator under azimuthally polarized vector beam excitation. Inset: SEM and schematic of an individual dielectric nanoresonator.152 (m)
Illustration of enhanced SHG based on SLR in plasmonic nanoparticle arrays. Inset: SEM image and dimensions of each structure.138 (n) Schematic of high-harmonic genera-
tion from an ENZ-assisted sample composed of a MgO substrate, CdO thin film and gold capping layer.153 (o) Large optical nonlinearity in ENZ material (A 23-nm-thick indium
tin oxide (ITO) layer) enhanced by coupling with plasmonic (gold) nanoantennas.154 (p) Schematic of efficient four-wave mixing based on nanofocusing in a silicon hybrid gap
plasmon waveguide. Inset: electromagnetic mode distributions and the chemical formula for MEH-PPV.124 (q) Illustration of dual-wavelength antenna and frequency upconver-
sion using BPT molecules in a 1.3 nm nano-gap between Au nanoparticle and disk. Inset: schematic of upconversion process, AFM (disk) and SEM (nanoparticle) images.155
(r) Schematic of radial BIC-enhanced SHG in a MoSe2 monolayer covering the ring structures.156 (s) Illumination of SHG in a leaky cavity by considering the input (output) cou-
pling coefficient and the spatial overlap between the dominant modes.157 (t) The interplay of symmetry and scattering phase in SHG from gold nanoantennas.158 All images are
reprinted (adapted) with permission from the respective Journal and copyright remains with the original publisher.

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Nonlinear processes such as harmonic generation and four-wave generation, due to their ability to provide strong local light field
mixing can be remarkably efficient when beams being mixed propa- enhancement. Wavefront control has also been shown [Fig. 6(d)] using
gate in phase over many millimeters of interaction in a nonlinear crys- the globally varied local nonlinear harmonic response of gold nanoan-
tal. Phase-matching brings material and technical restrictions as it tennas of C3 and C4 rotational symmetries, respectively.144 Although
comes at the cost of reduced tuning range and material flexibility. For metal provide excellent confinement, the high nonlinearity of the metal
example, phase-matching may only be achieved at specific wavelengths is difficult to use, since metals do not easily admit electric fields—this
and temperatures and the large interaction lengths require low absorp- means interaction volumes are relatively small. Simple plasmonic reso-
tion. For some photonic applications, new nonlinear materials that nances also provide relatively weak local field enhancement and struc-
can be integrated with the most relevant photonic platforms are tures with sharp features and gap that do enhance fields have low
important, such as polymers122–124 and 2D materials.125–128 Nonlinear damage threshold.132,161 For example, typical quantum efficiencies of
optical metasurfaces also hold promise for addressing these challenges SHG are 109 .
[Figs. 6(a) and 6(b)]. First, optical nanostructures can be designed at
the nanoscale to enhance local fields and meet symmetry requirements 2. Local resonance—Mie and multipolar modes
to produce strong nonlinear effects, as we discuss in detail below.
Second, nonlinear metasurfaces do not use phase-matching but instead Metasurfaces made of high refractive index dielectrics, such as sil-
rely on their high intrinsic nonlinearity to produce a useful nonlinear icon, germanium, and gallium phosphide, have emerged recently as a
effect. This alleviates tuning, bandwidth and material absorption competitive alternative to plasmonic metasurfaces, due to low material
restrictions. Third, nanostructured metasurfaces can be integrated with loss, larger interaction volumes and the capability to engineer their
a wide variety of nonlinear materials to further strengthen their intrin- magnetic response. Their efficiencies compared to plasmonic metasur-
sic nonlinearity. Finally, their engineered nature allows for nonlinear faces show improvement by several order of magnitude, mainly due to
wavefront control. These design features have led to a burgeoning field the higher damage threshold (see Sec. III C).151,162 These metasurfaces
of nonlinear metasurfaces. use Mie resonances to control the nonlinear interaction. Although
In this perspective, we present the state-of-the-art in nonlinear they exhibit some ability to enhance optical fields, the larger interac-
photonic metasurfaces, by reviewing the rich variety of mechanisms to tion volume provides the largest benefit.
engineer a nonlinear response at the nanoscale. Before considering Individual Mie resonance modes,132,135,145 such as electric, mag-
future directions for this field, we present a short study of how the netic dipoles, and higher-order Mie resonances, have been explored
individually to enhance nonlinear conversion efficiency beyond plas-

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metasurface interaction area affects nonlinear mixing efficiency as a
function of incident beam powers and areas. To conclude, we identify monic metasurfaces.132,133,163,164 For example, Fig. 6(e) shows that
THG conversion efficiency in silicon nanodisks is enhanced by mag-
the most useful metrics for assessing nonlinear metasurface perfor-
netic dipole resonances by two orders of magnitude compared to bulk
mance and future direction this field might take.
silicon.145
To increase the performance further, resonant coupling is often
B. State of the art used. Interference of multiple Mie resonances may result in far-field
Resonances play a crucial role in nonlinear optical metasurfaces, destructive interference, consequently enhancing the nonlinear effect.
since the linear optical response often dictates the nonlinear one.129 For example, the anapole state, associated with the destructive interfer-
The relationship between linear and nonlinear susceptibilities is well ence of dipole and toroidal moments, suppresses scattering to produce
known,115 but are not often utilized in phase-matched processes due to near-field enhancements.165 Both fundamental and a higher-order
the constraints of absorption on interaction length. However, thin anapole states in individual all-dielectric nanodisks have been imple-
metasurfaces can utilize resonance to produce strong nonlinearities. mented.146,166,167 Figure 6(f) shows a fundamental anapole state in a
Through structural resonances, metasurface can also enhance the elec- single Ge nanodisk for THG.146 Here, a minimum in extinction cross
tric and magnetic fields of incident light. These are usually categorized section corresponds to a maximum electric energy within the material,
into local and collective resonances.130 Local resonances, such as sur- producing THG quantum efficiencies as large as 106 . Coupled reso-
face plasmons,131 Mie modes of metallic and dielectric nanopar- nators also provide stronger nonlinear responses through their mutual
ticles,132,133 and Fano resonances,134,135 utilize nanostructures that coupling.168–171 For example, Fig. 6(g) shows a nanotrimer of three sil-
operate independently across the metasurface, while collective reso- icon nanocylinders that improves THG via the interference of electric
nances, such as guided-mode resonances,136,137 surface lattice reso- and magnetic dipoles.147
nance,70,138,139 and bound states in the continuum140,141 (BIC), access The nonlinearity of nanostructures can be further improved by
mutual coherences between nanostructures. combining the confinement capabilities of metallic resonances and the
interaction volume and radiative control of dielectric resonances.172,173
1. Local resonance—surface plasmons For example, the plasmonic resonance of a Au nanoring around a Si
nanodisk supporting an anapole state148 [Fig. 6(h)] shows THG quan-
Localized surface plasmon resonances (LSPR) are collective oscil- tum efficiency as high as 104 .
lation of free electrons in metal nanoparticles (typically gold or silver)
excited by incident light, where resonance is controlled via size, shape,
3. Local resonance—Fano interference
and particle composition. When integrated into metasurfaces, these
resonances enhance second harmonic generation (SHG)143 [as shown Fano resonance arises from the interference between a broad con-
in Fig. 6(c)] as well as a range of mixing effects53,158–160 including third tinuum of states and a narrow discrete resonance.134 In metasurfaces,
harmonic generation (THG), four-wave mixing, and sum frequency this can be realized through the coupling of plasmonic elements with a

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continuum of modes, leading to asymmetric line shapes and sharp electric field of incident light diverges when the imaginary part of the
spectral features. The intense and localized electromagnetic fields asso- permittivity approaches zero. This produces field enhancements
ciated with Fano resonances can greatly boost nonlinear frequency inversely proportional to ENZ film thickness189 that boost nonlinear
mixing processes.149 Figure 6(i) shows enhanced high-harmonic gen- effects.184–188 Their unique nonlinear optical response and the required
eration from an all-dielectric metasurface,149 where non-perturbative deep sub-wavelength thickness of the ENZ film also makes them
high-harmonic generation is enhanced in a Fano-resonant Si metasur- appealing for high-harmonic generation.153 Indium-doped cadmium
face. Figure 6(j) shows magnetic-Fano-resonance enhanced THG sig- oxide thin films (75 nm) show harmonic generation up to the ninth
nal via interplay between collective and individual optically induced order,153 as shown in Fig. 6(n). More on these materials is presented in
magnetic responses in quadrumers made of identical dielectric nano- Sec. XVII of this roadmap. Figure 6(o) shows a metasurface combining
particles.150 Plasmonic nanostructures show similar nonlinear plasmonic antennas with an ENZ material.154 Here, the narrow spec-
enhancements.169,174 We note nonlinear generation enhanced by Fano tral range and ENZ position of the underlying ENZ material could be
resonances are usually anisotropic with respect to the excitation polari- engineered to significantly boost the nonlinear optical response.
zation and have narrow operation bands due to their resonant nature.
7. Integrating metasurfaces with nonlinear materials
4. Collective resonance—bound states in the continuum
In attempts to maximize the nonlinearity of metasurfaces,
Collective high-Q resonances in all-dielectric metasurfaces, such researchers have integrated nonlinear materials with metasurfaces to
as bound states in the continuum (BICs) can offer large improvements exploit both material and structural resonances. For example, a 100-
in nonlinear metasurface response. BICs are eigenstates of a system path spontaneous parametric downconversion photon-pair source was
that exist within the continuum but do not radiate energy into the sur- created by integrating a metalens array (10 10 array of GaN nanopil-
rounding space. They were initially introduced in quantum mechanics lars) with a b-barium borate (BBO) nonlinear crystal.190 Another
and later extended to photonics.71,140,141,175,176 Mathematical BICs example uses low-loss nonlinear polymer within nanoplasmonic sys-
may have vanishing resonant linewidths. In practice, due to finite sam- tems.124,191–193 Figure 6(p) shows efficient four-wave mixing over
ple size, material absorption, small amount of radiation leakage, and micrometer-scale interaction lengths at telecommunications wave-
structural imperfections, BICs manifest with reasonably large Q fac- lengths on silicon can be achieved by combining an integrated plas-
tors, known as quasi-BICs. The long lifetimes of quasi-BICs are highly monic gap waveguide with a nonlinear organic polymer. Similar ideas
desirable for concentrating light in time and thus the nonlinear optical have been used to focus light into a nanoscale cavity to enable fre-

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process.177,178 Figure 6(k) shows SHG in a dielectric (gallium phos- quency upconversion from Mid infrared to visible,155,194 via molecular
phide) metasurface enhanced by two asymmetric cylinders with quasi- vibrations [Fig. 6(q)]. Highly resonant BIC metasurfaces may also be
BIC resonances.152 integrated with highly nonlinear materials. Figure 6(r) shows a radial
Quasi-BICs can also be engineered as individual local resonators BIC was used to boost SHG from monolayers of transition metal
by exploiting the interference of several Mie modes, similar to the ana- dichalcogenide.156 This brings two advantages: the two-dimensional
pole state discussed earlier.146,166,167 For instance, AlGaAs cylinders materials are straightforward to integrate within metasurfaces and
placed on an engineered three-layer substrate (SiO2/ITO/SiO2) show their atomic thickness minimizes the deformation of the resonance.
suppressed radiative losses, as shown in Fig. 6(l), boosting SHG
efficiency.151 8. Nonlinear metasurface selection rules

5. Collective resonance—surface lattice resonance Finally, we briefly consider the tensorial nature of non-linear
interactions and their corresponding selection rules. Local field
Surface lattice resonances (SLR) also achieve high Q-factors. enhancement and resonances are not alone sufficient for strong non-
When a grating Rayleigh anomaly condition crosses a LSPR, a sharp linear effects to be achieved. The non-linear polarization created by
spectral feature occurs, due to the hybridization of the surface and pump light in a metasurface must also be able to radiate to the far field
localized resonances.70 The SLR feature is controlled via nanostructure to complete the nonlinear process. This requires that the nonlinear
shape and lattice parameters. The effect of SLRs at the fundamental139 tensor components of the metasurface be matched to the desired input
and the generated nonlinear modes138 has been studied for boosting and output beams. Moreover, the interaction of the input and output
the nonlinear optical response.179 Figure 6(m) shows SLRs used to beams with the metasurface should be optimized by both impedance
enhance SHG from a plasmonic nanoparticle array made of split-ring matching, and spatial mode overlap at the various interacting frequen-
resonators138 where the SHG intensity improved more than a thirty- cies.151,195,196 Ideally, the suppression of all radiation channels apart
fold. Nonlinear metasurfaces based on both localized and collective from those for power injection and extraction has been proposed to
plasmonic resonances have also enabled the generation of controllable increased coupling to and from the metasurface,157 as schematically
terahertz waves,180,181 using mechanisms like ponderomotive accelera- shown in Fig. 6(s). Indeed, this has been experimental investigated
tion of photo-ejected elections182 and optical rectification.183 both in plasmonic158 [as shown in Fig. 6(t)] and all-dielectric145,197,198
metasurfaces.
6. Material resonance—epsilon near zero materials
At the boundary between metals and dielectrics, the nonlinearity C. Nonlinear generation rate and efficiency
of materials with epsilon-near-zero (ENZ) points have also been stud- Conventional nonlinear materials produce large conversion effi-
ied184–188 (see Sec. XVII). Where ENZ occurs, the surface normal ciencies by mediating nonlinear processes over a large interaction

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FIG. 7. Nonlinear generation rate and efficiency. (a) Schematic of a nonlinear process at a metasurface involving multiple incident beams and a generated output beam. The
conversion process is determined by incident beam powers and the peak intensities that can be achieved at the metasurface. (b) Map of SHG quantum efficiency in log scale
as a function of normalised pump power and mode area. Linear contours passing through origin have gradient of intensity. The broken line represents the damage threshold
intensity. (c) Map of SHG average power as a function normalised power and mode area. SHG power is maximised at the highest powers along the damage threshold intensity
line. The SHG efficiency and average power are normalised to the maximum value.

volume.115 Thus, large area metasurfaces should produce the fwm ¼ pffiffiffi a3
P 2p P
P s; (3)
highest nonlinear generation rates. To elaborate on this, con- 3 3½A0 Xs0 2
sider the following analysis of nonlinear frequency mixing at a p and P s are average powers in the pump and signal beams,
where P
metasurface.
respectively. Average photon pffiffiffi generation is improved for pulsed pump-
An nth order nonlinear process is affected by up to n input
ing over CW by a factor ½ nXs0 1n , but the advantage does not apply
beams. The ith Gaussian optical pulse intensity in time (t) and space
to peak powers. In this analysis, we assume that Xs0 is fixed, and we
(r) at a metasurface (z ¼ 0), Ii ðr; tÞ ¼ Pi =Ai epr =Ai t =si , where Pi is
2 2 2

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instead concentrate on the influence of beam power and area. We also
the peak power, Ai ¼ pwi =2, is the beam area (wi is beam waist) and
2
focus on SHG for simplicity. SHG efficiency is assessed against two
si is the pulse duration. This arrangement is shown in Fig. 7(a). The
Q common metrics in the literature. The first efficiency, gp ¼ P shg =P
20 , is
process generates a nonlinear polarization, P n ¼ v ðnÞ ni¼1 E i ðr; tÞ, chosen since pffiffiitffi is independent of pump power by definition, where
gp ¼ an =½2 2A0 Xs0 . The second efficiency, gq ¼ P shg =P
0 ¼ gp P 0,
where v ðnÞ is the nth order nonlinear susceptibility tensor and E i ðr; tÞ
is a power dependent quantum efficiency.
are the mixed electric fields.115 In most optical metasurfaces, the These SHG efficiencies are both influenced by mode area, A0, and
Q length is k, so that the generated beam intensity is
interaction pulse duration, s0. Clearly, the best conversion rates occur when the
In ¼ an ni¼1 Ii ðr; tÞ, where an is introduced to represent the intrin- incident average pump power is high and the mode area and pulse
sic nonlinearity of the metasurface. Here, we assume only simple duration are small. Inevitably, SHG is limited by the damage threshold
in-plane tensor connections between the input and output beams. intensity of a metasurface, ID. In our experiments with plasmonic
(Out-of-plane components generate non-Gaussian beams.) metasurfaces using near diffraction limited beams from either mode-
Substituting for the intensities of the mixing and output beams, locked oscillators (X ¼ 80 MHz, s0 ¼ 150 fs) or continuous wave
we find, lasers, we have found damage occurs at about 5 mW average power.
Yn For a diffraction limited area of 0:25 lm2 ; ID 1011 W cm–2 for
Pn pr2 =An t2 =s2n Pi pr2 =Ai t2 =s2i
e ¼ an e : (1) pulsed operation and ID;cw 106 W cm–2 for CW. Damage here is due
An A
i¼1 i to sample heating, and so the lower repetition rates of amplified laser
To simplify further, we assume the incident beams systems can allow higher intensities. Dielectric metasurfaces have
pffiffiffihave compa- slightly higher damage threshold intensities than plasmonic one, but
rable mode area, A0, and pulse duration, s0, so that nsn ¼ s0 and
nAn ¼ A0 at the metasurface. Since we assess nonlinear generation are not immune to damage at intensities ID > 1012 W cm–2 where ion-
with time averaging detectors, we use the average beam power as a ization effects occurs. We note that at these intensities, non-
measure of nonlinear conversion, P n ¼ Pn Xsn , where X is the laser perturbative nonlinear process start to emerge, and the preceding anal-
repetition rate. Thus, we find the average emission power in terms of ysis requires reevaluation.
the average incident beam powers, P i, The quantum efficiency and average SHG power are plotted in
Figs. 7(b) and 7(c) as a function of normalized power and mode area.
Yn
Along the power axis, normalization against both ID and diffraction lim-
n ¼ pffiffiffi an
P i:
P (2)
n n½A0 Xs0 n1 ited mode area, AD, leaves the axis dimension-less. Likewise, we have also
i¼1
normalized the beam area against AD. [We assumed a pump wavelength,
This expression
Q is valid for nth-harmonic generation k ¼ 1lm with a diffraction limited mode area: AD ¼ pð0:41kÞ2 .]
(nHG), where ni¼1 P n0 . In the case of four wave mixing, for
i ¼ P The power independent efficiency, gp, might seem like the most
example, appropriate metric, but it predicts optimal conversion efficiency at low

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beam area. Indeed, this is where the nonlinear effect is strongest, since include but are not limited to thermo-optic effects, free-carrier effects,
the beam intensity is maximized. However, the scaling of SHG with and phase transitions.209 The electrical modulation of a nonlinear
pump power squared suggests that large mode areas and high pump response based on electric-field-induced SHG or optical rectification has
powers should produce optimal SHG. The quantum efficiency proves been investigated in both plasmonic or dielectric metasurfaces.210–214
to be a more useful metric; although it varies with pump power, it can While this research direction is in its infancy, there are clear opportuni-
be evaluated in a way thatpisffiffiffiindependent of both
pffiffibeam
ffi area and pulse ties that play to the strengths of metasurfaces: thin films can be electri-
duration, gq ¼ an P 0 =½2 2A0 Xs0 ¼ an I0 =½2 2. As shown in cally accessed and modulated and resonant nonlinearities are more
Fig. 7(b), contours of gq are linear and pass through the origin, so the amenable to tuning with stronger modulations in material parameters.
gradient gives the intensity. If the damage threshold of the metasurface
is known, its limiting performance can be completely specified at any 3. Reduced power non-perturbative nonlinear optics
power and beam area.
The intrinsic nonlinearity of materials is measured by the nonlin-
Figure 7(c) shows a plot of average SHG power as a function of
ear susceptibility,115 vðnÞ . For example, SHG is governed by the value
average pump power and beam area. The plot confirms that optimal
of vð2Þ and naturally transparent crystals have vð2Þ 1–100 pm V–1.
SHG occurs when the pump power is maximized and the mode area is
When multiplied by incident electric fields of light, the dimensionless
minimized to operate at the damage threshold intensity. This power-
product indicates nonlinear strength. For an n-order process, the
area scaling presents challenges for applications of metasurfaces. The
dimensionless parameter vðnÞ jEjn1 is a metric of nonlinearity. For
write field of electron beam lithography is typically 100 100 lm2 ,
example, SHG with 1 W of CW light over a 104 lm2 beam area, has
representing an upper limit on metasurface area. A beam area of
vð2Þ jEj 108 –106 . Meanwhile, strong nonlinear effects occur for
104 lm2 , at damage threshold intensity requires an average beam vðnÞ jEjn1 1, where the perturbation description of the nonlinear
power of 100 W! polarization breaks down. Achieving this condition requires either
more intense light or a more nonlinear material. For example non-
D. Future directions of nonlinear optical metasurfaces perturbative effects such as high harmonic generation occur at intensi-
Metasurfaces cannot compete with phase-matched nonlinear ties I > 1013 Wcm2 in gases, and slightly lower in solids. While
processes in terms of efficiency, and the power-area analysis above sug- amplified pulsed lasers can access non-perturbative intensities, lower-
gests there are a few routes forward. Metasurfaces offer strong resonant ing the intensity at which non-perturbative effects begin is appealing
nonlinearities, wave-front control and the possibility to integrate new for reducing cost, complexity, size, weight and power. The increased

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materials. In this final section, we review applications in wave-front nonlinearity of metasurfaces are a promising route.
control, optical switching, and accessing non-perturbative nonlinear Nanostructures have been used to control non-perturbative high
physics at reduced power. harmonic generation effects both in isolated structures215–219 and
metasurfaces.149,220–224 High-harmonic generation has also been
1. Metasurfaces for nonlinear wave-front control shown in ENZ based metasurfaces.165 Such applications play to the
strengths of metasurfaces and would enable an expansion of research
The capability to locally engineer optical nonlinearity in metasurfa- teams able to study non-perturbative nonlinear physics across different
ces provides the means to engineer local nonlinear phase. Here, sub- disciplines by mitigating the need for expensive and bespoke laser sys-
wavelength nanostructures are tailored to control the phase and ampli- tems. Metasurface nonlinearity can be extremely large: to our knowl-
tude and direction of the nonlinear polarization.2,199,200 Recently, nonlin- edge, vð2Þ ¼ 1:2 lm V–1 is the highest nonlinear response reported for
ear wavefront control has been demonstrated using plasmonic144,201,202 a metallic metasurface coupled to inter-sub-band quantum well transi-
and all-dielectric203,204 nanostructures with specific structural symmetries tions in the mid-infrared,52,225 yielding vð2Þ jEj 1 under CW illumi-
from the extreme ultraviolet to terahertz.53,180,181,205 Beam shaping based nation. Such giant nonlinear responses have been seen in metasurfaces
on binary nonlinear phase and holography based on continuous nonlin- combining both electromagnetic and material resonances.
ear phase have been demonstrated by nonlinear optical wavefront engi-
IV. METASURFACES FOR BIOSENSING
neering techniques.144,206,207 Currently, there are a few studies in this area
and with the attention being dedicated to controlling local nonlinear
William J. Peveler and Alasdair W. Clark
phase, conversion efficiencies are relatively low. Additionally, wavefront
engineering techniques for various optical beams,53,208 such as multiple
[Link]@[Link]
optical vortex beams (Sec. VII), have been realized using linear optical
metasurfaces. Transferring these techniques developed for linear optical
A. Introduction
metasurfaces into the nonlinear regime will open a new avenue for the
realization of compact and ultrafast nonlinear optical devices. The advancement of technologies for the rapid and sensitive
detection of biological macromolecules (e.g., nucleic acids, proteins,
2. Metasurfaces for modulation and switching glycans) and whole organisms (e.g., viruses, bacteria, and other patho-
gens), are crucial to furthering our understanding of biological systems,
Although nonlinear metasurfaces open new avenues in flat nonlin- to the development of new diagnostic tests and healthcare tools, to
ear optics, the majority cannot be actively tuned post-fabrication despite improved drugs and therapeutics, and for ensuring the safety of our
this being a key feature in some linear metasurfaces (see Secs. II, XIV, food and water supplies. Therefore, as new developments are made in
and XV). Dynamic control over nonlinear metasurfaces under external materials science, one of the first application areas of these new materi-
stimuli is highly desirable in future. The mechanisms of the tunability als is often sensors. This is also true of nanophotonic metasurfaces.

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Indeed, metasurface biosensors have emerged as one of the most nota- surroundings228—i.e., bound molecules, not molecules in the bulk),
ble success stories in the field of nanoscale metamaterial research, tran- meaning they are not thrown off by environmental fluctuations
sitioning quickly from an academic curiosity to practical, commercial (e.g., temperature). While plasmonic nano-resonators are decades
sensing devices that are having impact in medical diagnostics, environ- old, new research into dielectric resonators is revealing key advan-
mental monitoring, and pharmaceutical research. The term “nanopho- tages. Metallic metasurfaces suffer from high losses, strong disper-
tonic metasurface” relates to devices comprised of two-dimensional sion, and poor magnetic response, whereas dielectric resonance,
arrangements of nanoscale building blocks (meta-atoms), whose col- the result of Mie resonances which generate oscillating displace-
lective optical properties are derived from their rational design and ment currents in response to the driving field polarization, exhibit
engineered array properties, rather than purely from their chemical low loss, sharper bandwidths, little heating, and can support strong
composition.199 These surfaces can be constructed using metallic or magnetic dipoles.229 Despite their different resonance mechanisms,
dielectric meta-atoms which have optical resonance properties defined the outcomes are similar: nanostructures, resonantly driven by
by their size, shape, composition, spacing, and crucially for biological light, with properties tunable by altering their geometry, and which
detection, the refractive index of their local surroundings.226 are either sensitive to their surroundings (i.e., the presence of a bio-
Therefore, their resonances properties can be altered by individual bio- molecule), or that produce a highly localized electric field that can
molecules interacting with their surface. The nanoscale nature of the be used to enhance existing sensing techniques. In terms of sensor
meta-atoms mean they are often of comparable size to these biomole- production, both wide-area, relatively inexpensive techniques, like
cules, meaning that even single-molecular localization on a meta-atom colloidal lithography, and smaller-area, relatively slow, more
surface can produce resonance shifts easily measurable in the far-field expensive techniques like electron-beam lithography are com-
by simple white light illumination; shifts that can also provide infor- monly used in the research space. However, advances in rapid
mation on interaction kinetics between molecules.227 Resonant meta- nanolithography techniques, such as nano-imprint lithography
atoms are also able to confine light to extremely small volumes, pro- and extreme UV photolithography, mean that, even for e-beam-
ducing many orders of magnitude enhancement to the electric field developed geometries, there is a clear path to practical, high-
around certain facets of the nanostructure (e.g., at sharp corners and throughput production of metasurface biosensors.
inside small gaps). Since many vibrational spectroscopy techniques
have efficiencies that scale with electric-field strength, the signals C. Biosensing
recorded from molecules within these enhanced regions is greatly
The resonances that unlock applications in biosensing pro-
improved. These two aspects of resonant meta-atoms make them

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duce highly confined field enhancements at the meta-atom surface.
excellent candidates for applications where label-free, hyper-sensitive
Therefore, only molecules resident within this near-field (typically
detection is required, and for applications where the interaction
in direct contact with the meta-atoms) are going to influence, or be
strength between pairs of molecules is being assessed. It has been possi-
influenced by, the resonance, and be detected. So, to function as a
ble to produce structures with bespoke optical properties for decades,
sensor, mechanisms are required to ensure that analytes are located
but recent strides in fabrication technology have greatly improved the
within the sensing volume long enough to measure. As a result, in
efficiency, speed, and cost-effectiveness of producing metasurface sen-
almost all the following biosensor examples, bio/chemical modifi-
sors. Coupled with their ease of excitation (e.g., illumination with
cation of the metasurface is required, usually with a receptor mole-
incandescent light bulbs, LEDS, laser diodes, etc.) and the low com-
cule that is complementary to the target analyte (e.g., nucleic acids,
plexity of their optical measurement, these advancements pave the way
proteins, antibodies, etc.). Once located there are several techni-
for portable, low-power, point-of-care, and field-deployable sensing
ques that allow molecular presence to be confirmed, some of
solutions. In this brief roadmap we will cover a small number of
which can also provide information about molecular structure and
research developments in the field of metasurface biosensors (some of
binding strength of those analytes. The examples below include
which appear in Fig. 8), and provide our outlook on what the future of
technologies developed to detect biomarkers of specific diseases. In
this fast-moving field may hold.
those cases, the detection limits achieved are within the range of
clinical relevance.
B. Biosensors: Plasmonic vs dielectric
Metasurface biosensors can be broadly categorized in two D. Refractometric sensors
groups: plasmonic (where meta-atoms are metallic) and dielectric
The most widely employed sensing modality involves monitoring
(where meta-atoms are, typically, silicon). Plasmonic metasurfaces
the resonance frequency of the metasurface as it interacts with its sur-
exploit localized surface plasmon resonances (LSPR), a nanoscale
roundings—operating on the principle that this frequency is linked to
variant of the long-established biosensor technology of surface
the refractive index immediately adjacent to the nanostructure.
plasmon resonance (SPR).1 Instead of generating surface plasmons
Therefore, when biomolecules bind to or approach the nanostructure’s
that propagate along the air-metal interface of bulk, thin-film met-
surface, they induce an easily observable resonance shift that provides
als (as in SPR), LSPR is generated by the oscillatory interaction of
a quantitative measure of molecular presence, binding events, and
light with the free electrons in the metal nanostructures. These
interaction kinetics.230
structures are smaller than the wavelength of the exciting light,
producing resonantly driven, highly localized electric fields. In
contrast to SPR devices, LSPR metasurfaces require no special cou- E. Plasmonic refractometric sensors
pling schemes, meaning they are trivial to excite, and produce As a widely used technique, there are thousands of examples of
fields with very short decay lengths (only probing their immediate different geometries, materials, and operating frequencies that have

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been explored. What follows is a small selection of recent examples. G. Chiral sensors
Gold is the most popular material for these sensors because of its Chirality is a fundamental property of many biomolecules,
chemical stability, simplicity of modification with bio-receptors, and including amino acids and nucleotides, where molecules exist in two
the ease by which visible resonances can be excited using white light.231 forms that are mirror images of each other, known as enantiomers.
For over two decades, the most popular surface geometry has been cir- This characteristic is crucial in biochemistry and pharmacology
cular nanodisks, a geometry that can be produced using many different because enantiomers of the same substance can exhibit vastly different
fabrication techniques. Since controlled array spacing is not necessarily biological activities, with one form potentially beneficial and the other
required for many biosensing tasks, a number of wide-area fabrication harmful. Chiroptical spectroscopic techniques can identify and charac-
examples (e.g., colloidal fabrication) exist. Examples include hole-mask terize chiral biomacromolecules, but their sensitivities can be greater
colloidal lithography and photolithography to produce gold nanodisks than six orders of magnitude lower than refractometric plasmonic sen-
for multiplexed measurement of diagnostic-relevant protein-protein sors,252 meaning they are largely unsuitable for detection of enantiom-
binding affinity at pM concentration.232 Similar fabrication techniques ers at diagnostically relevant concentrations (which can be pg/ml). The
have been used to detect single-base DNA mutations,233 and others enhanced fields exhibited by resonant metasurfaces can significantly
have shown that by coating the nanodisks with molecularly imprinted enhance the chiroptical response, enabling more sensitive detection of
polymers (MIPS) instead of traditional “complementary” receptor chirality. By using geometrically chiral plasmonic structures, so-called
molecules, label-free quantification of many polyphenol-protein inter- superchiral fields can be generated,253 optimizing the selective absorp-
actions can be made.234 Other examples of wide-area fabrication for tion of light by chiral molecules and enhancing CD signals. This pro-
scalable sensor production include nanosphere lithography to produce vides a more efficient means for the detection, analysis, and separation
Au nanopyramids to measure real-time protein (a–Synuclein)-small of enantiomers, offering improved sensors for pharmaceutical develop-
molecule interactions,235 and the use of nanoimprinting to create ment and diagnostics. The quest to generate superchiral fields for these
indented gold structures (“nanocaves”) for detecting tumor markers in purposes has led to a number of plasmonic metasurfaces which exhibit
human serum (carcinoembryonic antigen at 5 ng/ml).236 Electron- complex meta-atom geometries. Notable examples include the use of
beam lithography enables greater metasurface control, providing more gold shuriken indentations, fabricated by injection molding, to detect
options for geometry and layout variation (e.g., multi-layered biosen- pg quantities of helical biopolymers,252 perform multiplexed sensing of
sors with internal self-referencing),237 and receptor localization (e.g., proteins and virions,254 and record the chiro-optical response of type
receptor “patches” adjacent to the meta-atoms for biomolecule- II dehydroquinase.255 Another example of a chiral metasurface sensor

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mediated metasurface reconfiguration).238,239 As such, periodic arrays demonstrated the use of a 3D core-shell nanohelix structure, con-
of e-beam produced gold structures have been used to detect prostate structed via ion beam deposition of a Pt core, surrounded by the con-
specific antigen (PSA), in serum, at 500 pg/ml.240 In a variation of the ductive polymer P-oPD, to achieve detection of DNA binding protein
periodic nanodisk structure, Shen et al. demonstrated gold mushroom 43 (relevant for neurodegenerative disease) at a concentration of
10 fM.256
arrays with high-intensity coupled resonance modes (between a gold
film and elevated gold disks) for detecting alpha-fetoprotein (a liver
cancer and fetal development marker) at 15 ng/ml.241 Similarly, high- H. Enhanced vibrational spectroscopy
intensity fields can be produced in small gaps between discrete struc- The ability to confine light to incredibly small volumes make
tures, as demonstrated with IR-resonant nanorods for detecting metasurfaces ideal for increasing the efficiency of vibrational spectros-
human antibody IgG down to 30 pM,242 and to monitor peptide- copy techniques. Many techniques can benefit from these properties,
induced neurotransmitters from synaptic vesicle mimics.243 with Infrared Absorption Spectroscopy, Surface-Enhanced Infrared
Absorption (SEIRA), and Terahertz spectroscopy, having benefited
F. Dielectric refractometric sensors from metasurface enhancement (using IR resonating microstruc-
tures).257,258 However, the most common use of metasurface-
Recently, as the benefits of dielectric resonators has become enhanced vibrational spectroscopy is seen in Surface Enhanced Raman
apparent, similar functionality has been demonstrated with dielectric Spectroscopy (SERS).259,260 When light passes through a molecule
metasurfaces. Silicon nanodisks have been used to monitor biotin- with certain attributes, it may undergo Raman scattering; inelastic scat-
streptavidin interaction at 1010 M,244 to detect breast cancer bio- tering that produces a fingerprint of molecular vibrations from that
markers at 0.7 ng/ml,245 and to identify PSA at 1.6 ng/ml (below diag- molecule, elucidating chemical composition and structure. However,
nostic requirements).246 Low-cost fabrication has also been explored in Raman scattering is inefficient; large concentrations are required to
this space, with PSA detection shown using silicon disks produced via obtain signals. SERS amplifies scattering from molecules adsorbed on
colloidal lithography,247 and, in efforts to produce cost-effective meta- nanostructured surfaces, enabling detection of individual molecules
sensors with CMOS camera compatible readouts, Triggs et al. demon- and events. Since SERS enhancement scales with electric-field, meta-
strated chirped silicon-nitride gratings for characterizing antibody atoms are engineered to exhibit sharp edges or small gaps to concen-
binding.248 More complex shapes are also emerging, with crescent trate the electric-field. Sensing requires the excitation laser line cross-
structures supporting quasi-BIC (bound states in the continuum)140 over with the (typically broad) meta-atom plasmon, making surface
having achieved 0.16 nM protein detection,249 and where, notably, tuning simple, even with less-controlled techniques (e.g., colloid-
Altug’s laboratory have manipulated the angles and spacings of germa- mediated lithography). Indeed, the vast majority of SERS work is per-
nium and silicon nano-ellipse structures, and combined them with formed using cheap, effective, metal colloid. However, commercial and
hyperspectral imaging, to fingerprint various biomolecular events at research examples of metasurface SERS systems do exist when signal
high sensitivities.250,251 reproducibility or more sophisticated functionality are required. One

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such example used coupled gold triangular trimer structures designed approaches are well established and many methods of engineering
to exhibit multiple resonance modes spanning the visible and mid- metasurfaces with suitable chemistries attached have been achieved.
IR.261 With tip separation of a few nanometers, the trimers promoted However, there are also drawbacks to such an approach that are now
large field in these volumes. The authors demonstrated that these becoming more widely recognized.
multi-resonant structures were multi-functional, and could be used as The first consideration is one of multiplexing and the number of
SERS substrates for detecting DNA hybridization, and as surface targets that need to be detected. In the paradigm considered above,
enhanced fluorescence and SEIRA substrates.261 DNA hybridization assuming perfect receptor or sensing element specificity, “n” functional
has also been detected via SERS using metasurfaces consisting of sensing elements are required for n different targets. As the under-
polarization-sensitive silver split-ring resonators262,263 and by using standing and appreciation of multi-biomarker solutions for disease
the hybridization events to drive individual nanoparticle localization detection or biological systems measurement grows, particularly with
into the center of gold bowtie structures.239 Combining SERS with chi- advances in “omic” technologies, n can approach a very large number,
ral nanostructures has led to chiral discrimination of amino-acids via rendering it impractical or impossible to build such a large number of
SERS.263 Recent work on dielectric metasurfaces has shown that, much sensors.280 Second, again led by the increased amount of -omic data
like for refractometric sensing, these surfaces may hold advantages available, there is an understanding that not all biomarkers or target
over plasmonics for SERS biosensing. While plasmonic meta-atoms molecules are actually known at the outset. These “unknown-
can require high laser intensities, leading to heating and molecular unknowns” might enable greater insight or more accurate diagnosis
damage, dielectric meta-atoms exhibit little absorption, minimizing but simply have not yet been linked to the condition in hand. Finally,
heat, while retaining nanoscale light confinement. However, although there is a question of just how specific a sensor can be, particularly
there is activity in dielectric SERS,264 and some examples of dielectric when targeting small molecules or macromolecules with few features
SERS metasurface substrates do exist (e.g., silicon dimers to detect to bind.
b-carotenal molecules)265 the enhancement factors that can be Thus, the idea of cross-reactive arrays is now gaining traction.
achieved in Si systems are significantly lower than those seen in plas- Such arrays contain multiple sensing elements, sensitive to multiple or
monic systems (103 for Si vs 106 –101 4 in metal systems),260 meaning many different targets, and, rather than generating a single target
that their impact in biosensing may be limited. response, generate a pattern or fingerprint when exposed to a sample.
The sensing fingerprint is then tied back to the sample contents by sta-
I. Nanoholes tistical analysis and pattern recognition. This cross-reactive approach

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breaks the n for n paradigm and enables a holistic approach to sample
Surfaces that exhibit structured “negative” features, such as
measurement where all biomarkers in the sample have a chance to be
engineered holes and voids, also make for effective biosensors.266
measured, not just those known about at the outset.281 The sensor tar-
Extraordinary Optical Transmission (EOT) through plasmonic nanoa-
geting chemistry can be tuned to be more specific or more cross-
pertures is a phenomenon where light passes through holes in metal
reactive as the user desires, and a “training and testing” model is used
films at efficiencies higher than classical theories predict. A combined
to gather representative data that informs a statistical model or
effect of propagating and localized surface plasmon resonances, EOT
machine learning for further “unknown” sample analysis.282
acts to concentrate and funnel light through the nanoapertures, signifi-
Incorporating this approach with metasurfaces allows optically
cantly enhancing the transmitted light intensity, in doing so generating
addressable arrays to be created where changes in absorbance, reflec-
enhanced fields within the aperture itself. Thus, if molecules can be
tance, optical helicity, or other outputs are transduced to create a fin-
located inside these holes, refractometric and enhanced spectroscopy
gerprint, with spatial or wavelength based multiplexing possible for
sensors can be created. Gold nanohole arrays have been shown to be
each individual part of the sensor array.227
highly sensitive to antibody binding events,267 capable of responding
There are many examples of the method using plasmonic nano-
to PSA in a 96-well plate compatible metasurface format,268 used for
particles in solution, deposited inside well-plates, or drop-cast onto
detecting numerous exosomes for cancer diagnostics (measurements
surfaces as discrete sensing areas that display differential reactivity
that can also monitor treatment efficacy),269,270 for detecting pancre-
directly with target compounds or biomarkers to alter their plasmonic
atic cancer,271 and for identifying virus-like particles and assessing viri-
color.283 For example, Hormozi-Nezhad and co-workers have made
cidal drug candidates.272 Hole structures also bring the possibility to
extensive studies in this area, differentiating pesticides,284 measuring
create nanofluidic flow-through systems, where the apertures serve
urinary biomarkers for neurology,285 and also amyloid proteins among
dual roles as both optical modulators and liquid delivery channels.
many other bio-targets.286 Biogenic amines as markers of food spoilage
Examples of these systems include circular gold apertures for label free
can also be detected in this manner,287 as well as the different bacteria
DNA detection,273 single base DNA discrimination using gold nano-
themselves.278 In each case, the growth, etching, and aggregation of
pores and electro-plasmonic trapping,274 and bowtie shaped gold pores
metallic nanomaterials that leads to their color change, is influenced
to detect DNA275 and beta-amylase protein translocation.276
by the different reactive chemistry included in each part of the array
(typically a well in a 96 well plate), and the chemical interactions with
J. Future directions and outlook—cross-reactive the sample under test. It is clear that a reactive plasmonics approach
metasurface biosensors such as this could be further integrated into arrays of plasmonic mate-
In all the above examples, recognition of the target and retention rials as part of a metasurface, however, this would likely have to be a
in the sensing volume has been achieved using a specific binding part- single-use sensor, so may have limited utility in practical applications.
ner or interaction. For example, complementary base pairing of DNA, A second approach is to functionalize the metasurface elements
or a specifically chosen antibody or affinity protein for the target. Such with different cross-reactive chemistries, less specific than an antibody

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FIG. 8. Metasurface biosensing examples. (a) Gold mushroom nanostructures.241 (b) Quasi-BIC mode supporting silicon crescent nanostructures.249 (c) Flow-through nanohole

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sensor for DNA sensing.273 (d) DNA-directed nanoparticle localization inside gold bowties, as a sensing system.239 (e) Cross-reactive metasurfaces for monitoring water treat-
ment sites.277 (f) Multi-responsive, array-based nanoparticle sensor for micro-organism detection.278 (g) Barcode-based biosensing with elliptical dielectric resonators.251 (h) A
SERS-based artificial nose sensors.279 (a) Reprinted with permission from Shen et al., Nat. Commun. 4, 2381 (2013). Copyright 2013 Macmillan Publishers Limited.241 (b)
Reprinted with permission from Wang et al., Adv. Funct. Mater. 31, 2104652 (2021). Copyright 2021 Wiley-VCH GmbH.249 (c) Reprinted with permission from Shi et al., Nano
Lett. 18, 8003 (2018). Copyright 2018 Authors, licensed under a Creative Commons Noncommercial License (CC-BY-NC-ND).273 (d) Reprinted with permission from Clark
et al., Adv. Mater. 26, 4286 (2014). Copyright 2021 Wiley-VCH Verlag GmbH & Co.239 (e) Reprinted with permission from Sperling et al., Environ. Sci. 10, 3500 (2023).
Copyright 2020 Authors, licensed under a Creative Commons Attribution 3.0 Unported License.277 (f) Reprinted with permission from Li et al., Anal. Chem. 89, 10639 (2017).
Copyright 2017 American Chemical Society.278 (g) Reprinted with permission from Yesilkoy et al., Nat. Photonics 13, 390 (2019). Copyright 2019 Springer Nature Limited.251
(h) Reprinted with permission from Kim et al., Nat. Commun. 11(1), 207 (2020). Copyright 2020 Authors, licensed under a Creative Commons Attribution 4.0 International
License.279

but still imparting a degree of selective binding to nearby biomolecules. metamaterial created strong SERS hotspots between the elements, and
We have already exemplified this approach with cross-reactive meta- the interaction of the SAM with the targets (small biomolecules, extra-
surface arrays applied to the sensing of small molecules in whiskey and cellular vesicles, cell lysates) ensured different molecules could enter
water.277,288 In each case, a sensor was produced that consisted of an the hotspots, driving differential SERS spectra across the array. Two
array of plasmonic metasurfaces (many separate metasurfaces on the companion cell lines (one cancerous, one not) were easily identified
same substrate) that were each modified with a self-assembled mono- based on their differential SERS spectra across select array elements,
layer (SAM) of a different small molecule, imparting varying local coupled with PCA and LDA analysis.
charge, acidity, nucleophilicity and hydrophobicity to each metasur- The coupling of this approach with the exquisite sensitivity of
face. The metasurfaces were then exposed as an ensemble to different metasurfaces, their greatly improved multiplexing capacities, and
samples, reacting with molecules in solution to alter the local dielectric advanced fabrication methods should make metasurface sensing arrays
environment of each metasurface differently, creating a varying plas- a hugely powerful tool in bioanalaysis of the future, capable of operat-
monic fingerprint based on color shift across the array. These finger- ing in both liquid and gas sensing modes to deliver pattern recognition
prints were analyzed with principal component analysis (PCA) and of a wide variety of targets. Key to this success will be the choice of
linear discriminant analysis (LDA) to create tools capable of either dis- interfacial cross-reactive chemistries to deliver the best interactions
criminating whiskeys based on their chemical content, or treated and with the analytes under study, as well as exploitation of novel transduc-
untreated water samples based on their mineral and organic carbon tion modes possible with advanced metasurfaces, to increase the data
content. It is clear how such an approach can now be extended to density that can be collected. As more and more metasurface-based
direct biosensing, and is an area of ongoing research. tools become portable, thanks to their compatibility with simple opti-
In a similar approach, but with a different transduction method, cal platforms and even smartphone read outs, there is huge potential
Stevens et al. demonstrated a gold nanopillar metamaterial, where here for delivering ultra-sensitive biomolecule detection with specific
each region (sensing element) again featured a different SAM.279 The or cross-reactive sensing, at the point of need.

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V. METASURFACES FOR PASSIVE RADIATIVE COOLING human infrastructure elements like buildings, for instance, may lead to
lower indoor temperature and alleviate the need for excessive air con-
George Perrakis, Anna C. Tasolamprou, and ditioning, with potential for energy savings and improved efficiency.290
Maria Kafesaki Many other devices and technologies, such as solar cells, thermal tex-
tiles, and thermophotovoltaics, can highly benefit from PRC.291,292

gperrakis@[Link] Despite the practical benefits and high potential impact, PRC has
three main limitations.293–298 First, peak cooling demand occurs dur-
A. Introduction ing daytime, when incident sunlight heats the objects, Fig. 9(a).
Therefore, one will need a structure that reflects the entire solar spec-
From a thermodynamic point of view, exploiting a 3 K heat trum, Figs. 9(b) and 9(d).296 Second, PRC technology may be counter-
sink (ultra-cold universe) of infinite heat capacity, earth objects can productive in year-round assessments, due to provision of undesirable
reach temperatures below the ambient air temperature ( 300 K). cooling during cold days. Therefore, adaptive PRC may be required,
This is the principle behind passive radiative cooling (PRC). i.e., based on dynamic modulation techniques to tune thermal emis-
Specifically, PRC technology aims to exploit the coldness of the sion depending on the ambient air temperature.297 Third, current PRC
Universe for cooling purposes without any electricity input technology is highly unstable, strongly affected by climate or varying
required.289 It relies on Earth’s atmosphere transparency between weather conditions (e.g., humidity or clouds, resulting to reduction of
8 and 13 lm. This transparency window coincides with the peak of the atmospheric transparency) and by surrounding constructions [e.g.,
black-body thermal radiation spectrum of earth objects at typical tem- high-rise buildings, providing additional heat or obstructing the heat
peratures ( 300 K). Thus, any earth object facing the sky can release release, Fig. 9(c)], causing drop of the radiative cooling power. These
heat to the outer space, in the form of thermal electromagnetic (EM) limitations are a direct consequence of the symmetry of absorption-
radiation, lowering its temperature. emission met in most thermal emitters, owing to the fact that PRC con-
Such a passive strategy (i.e., that cools without any electricity figurations are made of reciprocal materials. Specifically, reciprocal
input) could significantly impact global energy consumption (15% materials, characterized by symmetric permittivity and permeability
decrease).290 The use of PRC as a passive cooling mechanism in tensors, satisfy Kirchhoff’s law of thermal radiation, which states that

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FIG. 9. (a) Solar absorption and thermal radiation properties of conventional surfaces (without metasurfaces cooler). Sub-optimal thermal emission (for k > 4 lm) and strong
parasitic solar absorption are observed resulting to object’s temperature larger than the ambient (300 K). (b) With a metasurface cooler on top (yellow layer), the radiative cool-
ing is enhanced, by enhancing emissivity at 8–13 lm and reducing atmospheric absorption, and the unwanted solar radiation is strongly reflected, leading to sub-ambient sur-
face temperatures, T< 300 K. Note that the object is insulated in (b) to minimize non-radiative heat gains from conduction and convention (e.g., wind), i.e., besides avoiding the
radiative heat gains. (c) Illustration of obstruction effect of high-rise buildings on the access of coolers to the sky. The black and purple arrows indicate top and sidewalls emis-
sion, respectively. In (b) and (c), sun and outer space are omitted for clarity. (d) Ideal reflectivity (R, green), emissivity (e, blue), and transmissivity (T, red) in ultraviolet (UV), vis-
ible (VIS), near-infrared (NIR), short-wave-infrared (SWIR), and mid-infrared (MIR) spectra, together with the normalized AM 1.5G solar irradiance spectra (gray, <4 lm) and
the infrared transmission of the atmosphere (gray, > 4 lm).

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their spectral, directional emissivity (e) equals their spectral, directional non-beneficial parts of the EM spectrum, Figs. 9(b) and 9(d). In 2015,
absorptivity (a). To this end, the two main existing strategies to stabilize Hossain et al.301 fabricated an anisotropic, conical-shaped waveguide-
PRC (i.e., avoid fluctuations in the radiative cooling power) are (i) high metamaterial emitter composed of 14 alternating layers of alumi-
spectral selectivity [maximizing the thermal radiation in the atmo- num (Al) and germanium (Ge) (size 2 lm, i.e., thickness and
spheric transmission window and keeping it minimum everywhere bottom diameter) to realize polarization-insensitive, highly selec-
else, Figs. 9(b) and 9(d)]299 to mitigate the sensitivity to humidity, and tive PRC, Fig. 10(a). They demonstrated ultra-high emissivity
(ii) enhanced directionality, also to a limited solid angle (beaming), to (>0.85) and broadband operation at 8–13 lm, owing to the
avoid additional heat gains from the surrounds, Fig. 9(c).300 slow-light modes at different wavelengths (with peaks’ emissivity
Conventional approaches to meet these stringent requirements, >0.9) and the tapered shape. They measured a remarkably high
however, come with large space demands, often requiring complex cooling power, of 116.6 W/m2, at ambient air temperature and a
shelter and shading systems, and therefore limit applicability, often temperature of 12:2 C below ambient.
reducing also the emission power.293 For real objects in local thermal Apparently, fabrication feasibility, scalability, and cost-
equilibrium, Kirchhoff’s law of thermal radiation still holds at every effectiveness are also vital for promoting PRC as a viable energy tech-
combinatorial specific set of wavelength (k), angle (h), and polarization nology. With this in mind, Zhai et al.,302 two years later, demonstrated
(p).300 The field of photonics though, which explores the use of light a highly transparent hybrid metamaterial cooler composed of resonant
molding techniques in the visible and infrared, assisted by the recent polar dielectric (silica) microspheres ( 4 lm diameter) randomly dis-
advances in nano-fabrication, is capable of engineering e at selected k, tributed in a polymeric matrix (50-lm-thick), Fig. 10(b). By accessing
h, and p, i.e., using the concepts of photonic crystals (PCs), metasurfa- the high-order Fr€ ohlich resonances of the polar silica spheres, the
ces, and metamaterials. Metasurfaces and metamaterials, for instance, metamaterial provided larger than 0.93 and broadband infrared emis-
involve structuring the material at a subwavelength scale. Relying on sivity across the atmospheric window. When backed with a silver coat-
local and non-local resonant phenomena (as a result of proper ing to reflect solar radiation, the metamaterial showed a noon-time
structuring, i.e., of suitably designed building-blocks, known as meta- radiative cooling power of 93 W/m2 under direct sunshine. The high
atoms), metamaterials and metasurfaces provide unique optical prop- significance of this work is related to the high-throughput and eco-
erties and enable novel ways to tailor light. The careful engineering of nomical roll-to-roll manufacturing of the metamaterial combined with
shape, size, and arrangement of meta-atoms can imprint the desired the high PRC performance.
response, such as enhanced directionality,300 or tune the spectral band- Although the impact of PRC on emitters’ surface temperature
width of operation,301 also offering extra advantages, such as ultra-low

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was early highlighted, its impact on cooling inner (enclosed) spaces
thickness and weight,305 and flexibility. Therefore, metamaterials/ (that trap heat by the greenhouse effect) remained unclear until 2020.
metasurfaces have been employed as coatings for PRC applications in In 2020, Heo et al.299 presented a Janus thermal emitter for cooling
recent years [see Fig. 9(b)].305–307 Additionally, to date, considerable enclosed spaces, consisting of an Ag-coated quartz grating and a poly-
attention has been paid to utilizing metasurfaces and metamaterials dimethylsiloxane (PDMS) layer on quartz substrate’s front and rear
also to relax the constraints coming from space-reversal symmetry or side, Fig. 10(c). The Janus emitter acted as selective emitter on the top
by reciprocity (connected to time-reversal symmetry) via (i) breaking side, to dissipate heat to outer space, and as broadband emitter on the
the time-reversal symmetry with non-reciprocal materials and gra- bottom side, to draw heat from the inner space, Fig. 10(c). The selec-
tings, e.g., magneto-optic materials, time-modulated systems, or Weyl tive emitter showed a sub-ambient cooling of 6 C, obtained by
semimetals,308 or (ii) breaking the space-reversal symmetry of trans- exploiting spoof surface plasmon polaritons (sSPPs) to achieve near-
mission with reciprocal but anisotropic or bi-anisotropic systems, such ideal selectivity. Notably, the temperature of an object inside the enclo-
as metallic gratings with subwavelength slits, gradient metasurfaces, sure was 4 C lower than that achieved when using a conventional
hyperbolic metamaterials, and chiral structures.309,310 Consequently, it radiative cooler with reflective bottom surface. These results demon-
would be of paramount importance to fabricate non-reciprocal ther- strate that metasurfaces and metamaterials can provide high-efficiency
mal emitters (coolers) or asymmetric configurations that would emit PRC (4 12 C) even paired with high-throughput, economical, and
or allow heat in certain directions without absorbing or allowing scalable manufacturing, promoting PRC as a viable energy technology.
incoming heat.293,294 Currently and in recent years, there is significant Tunability. As mentioned also earlier, the ability to tune a cooler’s
research on examining different photonic strategies in terms of appli- thermal emission depending on the environmental conditions allows
cability, feasibility, and potential of enhancing and stabilizing PRC. In for an adaptive PRC system whose cooling power switches off when
this perspective, we provide an overview of the recent and ongoing not needed, e.g., in cold nights or winter times, avoiding overcooling
research on metasurfaces, metamaterials, and PCs as means to control that increases the heating cost. In 2018, Ono et al.311 proposed an one-
the fundamental aspects of thermal radiation for cooling purposes. dimensional (1D)-PC consisting of two components, a spectrally
Such aspects are related to (i) spectral selectivity, (ii) tunability, (iii) reflective filter and a switchable radiative cooler. The on-top spectrally
directionality, and (iv) asymmetric propagation. Finally, we discuss the selective filter was a 11-layer stack of alternating Ge/MgF2 layers,
challenges and potential future directions. which served as a reflector of solar radiation and a passband filter with
high transmissivity at 8–13 lm. The radiative cooler at the bottom
B. State of the art consisted of a VO2/MgF2/W tri-layer, where VO2 (material with phase
Spectral selectivity. As mentioned already, spectral selectivity is a transition hysteresis) was the switching component. The angle and
quite important feature of a radiative cooling system, as it can allow polarization averaged emissivity (0 –90 ) in the wavelength range of
emission/absorption only in the beneficial for cooling 8–13 lm 8–13 lm was 0.64 in the metallic state of VO2. On the contrary, the
spectral window (atmospheric transparency window) and reject the averaged emissivity dropped to 0.05 when VO2 was in insulating

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FIG. 10. Examples of PRC metasurfaces of different geometries and configurations. (a) Array of fabricated conical-shaped metamaterial pillars.301 (b) Polymer-based hybrid
metamaterial with randomly distributed SiO2 microspheres for large-scale PRC.302 (c) Janus emitter applied to an automobile under direct sunlight, where heat is trapped by
the greenhouse effect, allowing broadband absorption of IR waves from the enclosure and selective emission to the ultracold space.299 (d) Structure of the temperature-
adaptive radiative coating and principle of operation.297 (e) Phase change metasurface consisting of periodic VO2/SiO2/VO2 cavities.303 (f) Spectra of the thermochromic smart
window with and without radiative cooling regulation in VIS, NIR, and MIR at 20 C (blue) and 90 C (red).304 (g) Asymmetric transmission periodic micro-structure of inverted
silver trapezoids and relevant forward/backward transmission, reflection and absorption over the atmospheric transparency window range and beyond.294 (h) Schematic of the
asymmetric transmission pyramidal micro-structure and principle of operation.295 (i) Array of fabricated SiO2/AlOx double-shell hollow microcavities for directional thermal emis-
sion.300 All images are reprinted (adapted) with permission from the respective Journal and copyright remains with the original publisher.

phase, leading to a 0.59 modulation performance. At “on” state, the slow-light waveguide mode in the trapezoidal HMM, while with the
radiative cooler reached an equilibrium temperature around 10 C presence of the filter on the top, system’s emissivity peaked (>0.95)
below ambient. At low ambient temperatures ( 25 C, when cooling only at three wavelengths (8.4, 9.7, and 11.8 lm), creating spectral-
is not needed) the system switched off, accompanied by a sudden selective emission (at 8–13 lm). The thermal emissivity modulation
reduction of the cooling power, maintaining cooler’s temperature near performance was 0:67 (from 0:20 to 0.87), leading to a cooling
the critical temperature ( 25 C). The same year (2018), Wu et al.303 power >100 W/m2 (up to 127.8 W/m2) when cooler’s temperature
proposed a phase-change metasurface consisting of periodic VO2/ was 69 C, and 27.9 W/m2 at 68 C. Considering scalability, flexibility,
SiO2/VO2 cavities supporting a thermally switchable Fabry–Perot and low cost, Tang et al.,297 in 2021, fabricated a phase-change meta-
(FP)-like fundamental resonance mode at 8–13 lm, Fig. 10(e). The material consisting of a 2D array of thin WxV1xO2 blocks embedded
thermal emissivity there switched from 0:2 to 0:65 ( 0:45) with a in a BaF2 dielectric layer on an Ag film, in various design configura-
critical (VO2 phase-change) temperature 68 C. The cooling power tions, for production in a roll-to-roll fashion, Fig. 10(d). When
was calculated 118 and 528 W/m2 at device temperatures 67 and WxV1xO2 was in the insulating phase, the metamaterial was mainly
69 C, respectively, compared to 1.3 and 187 W/m2 for a simple 300- transparent to the IR radiation at 8–13 lm and highly emissive when
nm-thick VO2 film. In 2020, Zhang et al.312 proposed a trapezoidal it switched to the metallic state. The thermal emissivity was further
hyperbolic metamaterial (HMM) emitter composed of Ge and VO2 amplified by a designed photonic resonance involving adjacent
for self-adaptive PRC and a MgF2/Ge multilayer filter placed on top WxV1xO2 blocks and by the 14-wavelength cavity formed in BaF2 due
for reflecting solar radiation and allowing selective transparency (at to the bottom ultra-thin Ag layer, Fig. 10(d). This flexible,
8–13 lm). When VO2 was in metallic phase, close-to-unity, broad- temperature-adaptive metamaterial switched its thermal emissivity
band (>4 lm), and angle-insensitive emission was achieved due to the from 0.2 to 0.9 (0.7) at 8–13 lm when the surface temperature raised

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above 22 C. The metamaterial was 2 C warmer than two reference and 0:1 backward, ratio 7). Theoretical predictions revealed that
(non-adaptive) roof coatings when the ambient temperature was below the radiative cooler integrated with the ATS has an insensitive (no
22 C. matter the conditions and terrain) equilibrium temperature 10 C
In addition to modulation of thermal emissivity, the simultaneous below ambient, compared to 2 C of the standalone thermal emit-
modulation also of solar heating (i.e., absorbing/reflecting near- and ter/cooler. As in the previous case, though, the equilibrium tempera-
short-wave-IR radiation and remaining transparent or semi- ture should be reconsidered.314
transparent in the visible spectrum), e.g., in smart and/or thermochro- In 2023, Cho et al.300 reported directional, polarization-
mic windows, may further improve the regulation of heat flow to insensitive thermal emission, which facilitates PRC from the sidewalls
maintain a system’s temperature near a desired set point, increasing of buildings [Fig. 10(i)], see also purple arrows in Fig. 9(c). They fabri-
energy-savings. In 2020, Wang et al.313 proposed a compound meta- cated hexagonally arrayed holes (12-lm pitch, 5.5-lm depth, and 10-
surface of large and small cross-shape resonators for realizing self- lm diameter) realized by sub micrometer-thick SiO2/AlOx double
adaptive PRC and solar heating in one system. The core of the self- shells (100/100 nm), resulting to a hollow cavity film, Fig. 10(i). The
adaptive response is the utilization of a PVP (pNIPAM) spacer below cavity film exhibited average emissivity values of 0.51–0.62 at angles
crosses, which can expand (contract) with heat and contract (expand) (h) 60 –75 and 0:29–0:32 at 5 –20 , yielding a parabolic antenna-
with cold, increasing or decreasing crosses’ spacing. The absorptivity/ shaped distribution. The angular selectivity peaked at four different
emissivity modulation performance in both solar and 8–13 lm spec- wavelengths at 8–13 lm (8, 9.1, 10.9, and 12 lm), identified as
tral regimes was 0:8 (from 0:1 to 0:9) within a narrow band- Berreman modes (only in p-polarization at epsilon-near-zero (ENZ)
width. The results showed that the compound metasurface can remain wavelengths of SiO2) and photon-tunneling modes (at maximum
cool at 35 C and warm at 25 C. In 2021, Wang et al.304 fabricated a negative permittivity wavelengths of AlOx), creating broadband (at
scalable smart window based on W-doped VO2 nanoparticles dis- 8–13 lm), angle-selective emission bands, resulting to superior
persed in a PMMA solution on top of a PMMA spacer for simulta- directional PRC compared to an isotropic black body-like thermal
neous thermal emissivity and solar reflectivity modulation, Fig. 10(f). emitter (up to 4 C). We note that Wang et al.315 proposed the same
Interestingly, the critical temperature was tuned through W-doping year that directional thermal emission can also be realized in a broader
around 27:5 C (i.e., much lower than that of pure VO2, 68 C). The spectrum beyond the previously considered ENZ and Berreman mode
stacking formed a FP resonator with weak resonance (at 8–13 lm) at region. A two-phase metamaterial emitter composed of only two mate-
low temperatures and strong FP resonation effect at higher tempera- rials (material 1 containing subwavelength particles of material 2 on
top of a perfect electrical conductor) was proposed showing numeri-

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ture (due to the insulator-to-metal transition of VO2), enhancing emis-
sivity. The emissivity at low temperatures was 0.21 and at high cally strong (e > 0.8) directional (80 6 5 ) broadband thermal emis-
temperatures 0.61 (0.4 modulation performance), combined with sion, where the bandwidth of directional thermal emission can be
near-IR solar modulation of 9.3%, due to the change of the transmit- controlled through the methods of gradient ENZ and effective medium
tance of VO2 with temperature, Fig. 10(f). The proposed smart win- theory. These results suggest that by utilizing metasurfaces and meta-
dow yielded higher energy-saving performance than a commercial materials, PRC can be less affected by the environmental conditions
low-e window, up to 324.6 MJ/m2, revealing the importance of inte- and the surroundings, which promise all-weather and all-terrain
grating PRC modulation in smart and/or thermochromic windows. applications.
Stabilizing PRC. In 2018, Wong et al.294 proposed an asymmetric Regarding non-reciprocal emitters, where Kirchhoff’s law of ther-
EM transmission structure (ATS) placed on top of a thermal emitter/ mal radiation does not hold, i.e., emissivity is not equal to absorptivity,
cooler to reduce its dependence on humidity and clouds that lower its their impact on PRC is not extensively examined in the literature. Two
radiative cooling power, Fig. 10(g). The proposed ATS, consisting of a recent studies in 2023, by Liu et al.316 and Shayegan et al.,317 demon-
tapered metallic grating, exhibited high-contrast asymmetric transmis- strated direct observation of Kirchhoff’s law violation under a moder-
sion at 8–13 lm ( 0:8 forward and 0:4 backward, ratio 2), ate external magnetic field (<1.5 T). They reported inequality between
Fig. 10(g). Therefore, the ATS, on one hand, permits outgoing trans- emissivity and absorptivity over a broad MIR band, matching also
mission of thermal radiation emitted by the radiative cooler, and, on 8–13 lm.317 In Liu et al. case, they used a photonic design that sup-
the other hand, it reflects incoming radiation from the sky that lies ports a guided-mode resonance coupled to a magneto-optic mate-
within the same wavelengths [see also Fig. 10(h)]. Theoretical predic- rial316 while in the Shayegan et al. case, they employed magnetized
tions under humid, semi-transparent sky revealed 57% (50 W/m2) gradient epsilon-near-zero thin films.317
recovery of cooling power, translating to a radiative cooler’s tempera-
ture 8 C lower than the standalone radiative cooler (without ATS). In C. Future directions and outlook
this case, however, the metallic grating is made of silver, Fig. 10(g), Using concepts coming from metasurfaces, metamaterials, and
which is a reciprocal material, meaning the directional absorption PCs research, recent studies have demonstrated tunable (>0.4) and
must equal the directional emission. Therefore, the amount of recov- high-efficiency PRC ( 4 12 C below ambient) during daytime
ered cooling power should be reconsidered.314 Two years later, Wei under direct sunlight, even combined with high-throughput, economi-
et al.295 proposed an ATS placed on top of a thermal emitter/cooler to cal, and scalable manufacturing, Fig. 10. Here, we emphasize on flexi-
mitigate the combined effects of weather (humidity and clouds) and ble, roll-to-roll processing technologies that earned sufficient attention
terrain [e.g., obstruction effect of high-rise buildings, Fig. 9(c)] on its as a future contender on the PRC industry manufacturing roadmap
radiative cooling power, Fig. 10(h). Using a glass imprinted with prop- [see Figs. 10(b) and 10(d)].297,302 In this case, radiative coolers’ reliabil-
erly designed micro-structures [Fig. 10(h)], a high forward-backward ity should be further examined in relation to integrated polymers’ deg-
transmissivity contrast ratio at 8–13 lm was achieved ( 0:7 forward radation (thermally- or light-induced due to ultraviolet (UV)

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radiation) or to metal reflectors’ oxidation by oxygen and moisture. could be employed, such as two-photon polymerization (2PP), 3D/
Employing chemical additives, coatings, or hybrid organic-inorganic 4D-printing, and laser-induced periodic surface structures (LIPSS)
ultra-thin PRC multilayers306 may improve polymers’ outdoor perfor- with ultrashort pulsed lasers, for nano-structuring a wide range of
mance, although thin polymer films with extended outdoor lifetimes materials (metals, semiconductors, dielectrics, and polymers).
are already available.302 Moreover, a way to avoid the metal layers or Decoupling a and e can lead to novel functions, ranging from reducing
more intricate 1D multilayers (commonly used to reflect sunlight) and losses from solar radiation re-emission in solar energy harvesting sys-
still strongly reflect sunlight (including UV radiation) is by integrating tems (occurring due to reciprocity) to radiative camouflage and opti-
layers with light-scattering pores on the nano- and micro-scale.318 mum PRC.292,317
Porous structures’ durability, though, affected by dust or moisture,
ACKNOWLEDGMENTS
should be further examined. Alternatively, to avoid porosity and effi-
ciently reflect solar light, paints based on a binder (e.g., polymeric) G.P., A.C.T., and M.K. acknowledge support by the Hellenic
with various fillers and high-index pigments to scatter light (such as Foundation for Research and Innovation (HFRI) under “Sub-action
TiO2, SiO2, Al2O3, and BaSO4 nano- and micro-particles) could be uti- 2 for Funding Projects in Leading-Edge Sectors—RRFQ: Basic
lized,318 i.e., “complementary” to porous structures. Finally, minimiz- Research Financing (Horizontal support for all Sciences),” Project
ing non-radiative heat gains from conduction and convention [wind, ID 15117 (MultiCool).
Fig. 9(b)] should also be addressed for efficient PRC below ambient air VI. METASURFACES FOR PHOTOCATALYSIS
temperature (i.e., besides avoiding the radiative heat gains).296 This
could be achieved by tuning metamaterial’s thermal conductivity, Anastasiia Zaleska, Wayne Dickson, David Richards,
which can be achieved by changing its chemistry or micro- and Anatoly V. Zayats
structure.319,320
In addition to the above, great effort has been conducted to [Link]@[Link]
stabilize PRC subject to unideal conditions such as clouds, humid
subtropical climate, and high-rise buildings [Fig. 9(c)].294,295,300,315
A. Introduction
Despite the demonstrated superior directional PRC (up to 4o C
compared to an isotropic black body-like thermal emitter), Chemical reactions facilitated by light are a cornerstone of
enhanced selectivity and directionality come with reduced sky clean energy conversion, environmental remediation and material
access and emission power [Figs. 9(b)–9(d)],296 limiting heat dissi- synthesis. While photochemical transformations can take place

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pation to outer space and, therefore, cooling power. Moreover, inte- when reactants are directly illuminated with light, the use of
grating ATSs composed of reciprocal materials to break the various material systems, often nanostructured, as photocatalysts,
symmetry of transmission as means to stabilize PRC [Figs. 10(g) can enable a broader class of chemical reactions and can offer
and 10(h)]294,295 is still under consideration.314 Theoretical studies enhanced efficiency and selectivity in light-driven processes.
proved that asymmetric transmission is achievable using reciprocal Nanomaterials, particularly nanoparticles, play a crucial role in
materials but without increasing the overall radiative cooling photocatalytic applications by providing large surface areas for
power.314 Therefore, it would be interesting to experimentally molecular adsorption and unique electronic properties, enabling
examine the applicability and potential of this photonic strategy on efficient light absorption and facilitating controlled photochemical
stabilizing PRC compared to conventional approaches for enhanc- transformations. The size, shape, and composition of nanomateri-
ing directionality and selectivity, given also the plethora of photonic als and their surface chemistry can be engineered to optimize pho-
designs for asymmetric transmission proposed in the literature tocatalytic activity and selectivity, thereby enhancing the overall
(e.g., gratings, arrays, and chiral metamaterials) for various applica- efficiency of light-driven reactions. Both semiconductor and metal-
tions, even at 8–13 lm.321 We note that, according to recent stud- lic nanostructures can be used for photocatalysis, exploiting strong
ies,293–295 asymmetric transmission and PRC cannot be enabled in light absorption in the designed spectral range, resulting in elec-
the same component or material (e.g., one grating or metamaterial), tron–hole pair excitation through interband transitions in semi-
which may increase PRC system’s complexity, Fig. 10(h). conductors and metals, or the generation of energetic hot electrons
A promising route to stabilize PRC, maintaining high cooling using surface plasmon resonances in metallic nanostructures. An
power enabled by a single component, is to avoid the reciprocity con- additional side-effect of such electronic excitations is the rise of the
straints with non-reciprocal materials.316,317 Maximal violation of local temperature of the material which influences the reactivity
detailed balance in thermal radiation (absorbed equals emitted) cur- through thermal effects, as in conventional thermal catalysis.
rently faces several challenges, as it requires a temporal or magnetically Overall, the integration of nanostructures with photochemistry
induced modulation.322 The design, simulation, and optimization of and photocatalysis holds significant promise for advancing sustain-
such approaches, though, are inherently complex while the involved able technological solutions.
phenomena are typically resonant.322 Consequently, novel solutions to In this respect, metamaterials and metasurfaces provide a highly
achieve high-contrast asymmetric propagation with broadband opera- flexible platform for engineering enhanced light–matter interactions
tion in MIR are required.316 Moreover, the impact of non-reciprocal which control electric field localization and its polarization as well as
thermal emission on PRC, to our knowledge, has not been experimen- local temperature, while providing large surface areas important for
tally demonstrated yet, also due to limited fabrication feasibility, scal- chemistry.323,324 The planar geometry of metasurfaces also facilitates
ability, and increased cost in standard lithographic techniques. Toward their integration into photo-electrochemical systems, while the use of
this direction, emerging low-cost, robust, and scalable approaches metaparticles—nanoparticles engineered using metamaterial design

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principles325—provides the combination of increased surface area and crystal.332 This approach can be applied to various types of semicon-
engineered optical response with the advantage of scaleable fabrication ductor material systems by varying the active materials, leading to sub-
afforded by nanoparticle synthesis. Furthermore, the opportunity to stantial improvements in air/water contamination, water splitting or
engineer these nanoparticles as a coating on powders is preferred for artificial photosynthetic processes (Fig. 11).
some photocatalytic applications. The engineered enhanced light absorption and planar geometries
of metasurfaces enable their use as a photo-electrode material,333 dem-
B. State of the art onstrating, in the case of a GaP-nanodisk-based metasurface, an over-
Many realizations of metallic (plasmonic) and semiconductor all photocurrent enhancement by more than fivefold compared to a
metasurfaces and metamaterials have been recently developed and planar GaP film under hydrogen evolution reaction conditions
investigated for enhancing and controlling photocatalytic and photo- [Fig. 11(c)].331 Nanoimprint lithography techniques and electrochemi-
electrocatalytic transformations. While plasmon resonances have been cal approaches enable the rapid development of large-area nanopat-
widely employed in metallic catalysts, which provide enhanced light terned surfaces of various materials necessary for industrial
absorption and hot-carrier excitation not limited by a bandgap, semi- applications as a new generation of highly efficient solar meta-
conductor, and dielectric metastructures are also actively considered electrodes.
for enhancing light absorption at sub-bandgap energies and engineer- Dielectric (catalytically inactive) metasurfaces decorated with
ing strong absorption in catalytically inert dielectrics decorated with metal catalytic nanoparticles can be employed as an antenna-reactor
metal or semiconductor catalysts. These often exploit archetypical photocatalyst where the virtually lossless metasurface funnels light to
metasurface designs based on nonradiative high-index nanophotonics, efficiently drive a chemical reaction.334 By combining a Si3N4 metasur-
such as multipolar Mie resonances and bound states in the continuum. face exhibiting strong quasi-bound states in the continuum (quasi-
Photocatalysts based on semiconductor materials, such as tita- BIC) resonances and large electric field enhancements, with Ni nano-
nium dioxide (TiO2) and gallium phosphide (GaP) are traditionally particles as reactors, this hybrid metasurface-based catalytic system
attracting significant attention because of the possibility to utilize solar was demonstrated to efficiently drive H2 dissociation under the reso-
energy directly.326,327 They generally benefit from high chemical stabil- nant illumination [Fig. 11(d)]. The experimental and theoretical analy-
ity and reactivity, are nontoxic and inexpensive. Holes in the valence sis suggest that both photothermal heating and electronic transitions at
band and electrons in the conduction band, excited upon interband the quasi-BIC-Ni surface facilitate catalytic chemistry (the thermal
light excitation, can then interact with molecules on the surface pro- effect also cannot be ruled out in the above-discussed semiconductor

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moting chemical transformations. However, optical absorption in metasurfaces when defect-related transitions are considered). This
semiconductor materials is limited by their bandgap. TiO2 has a rela- approach, based on engineered dielectric metasurfaces combined with
tively large bandgap of about 3.2 eV, which makes this catalyst pre- otherwise weak absorbing metal catalysts, provides a universal plat-
dominantly active under UV light, in the wavelength range shorter form which can be exploited for various combinations of dielectrics
than 400 nm, compared with a bandgap of around 2.2 eV for GaP. and catalytic metals.
This means TiO2 photocatalysts can harvest only a few percent of the In contrast to dielectric and semiconductor materials, plasmonic
solar spectrum energy (about 3%–5%). Additionally, the photocatalytic nanostructures provide the unique possibility to engineer light absorp-
activity of semiconductor materials is limited by the rapid recombina- tion throughout visible and near-infrared spectral ranges with spectral
tion of photogenerated electron–hole pairs and insufficient charge car- selectivity as well as strong electromagnetic field enhancement. Surface
rier transfer. Extensive research efforts have been dedicated toward the plasmons excited in metal nanostructures by light absorption decay
improvement of their photocatalytic performance through material either radiatively through re-emission of photons or non-radiatively
modification and incorporation or doping with other functional mate- via, e.g., Landau damping on a femtosecond timescale, resulting in hot
rials for visible light utilization. carriers with energies comparable to the energy of the exciting pho-
Metasurfaces patterned on TiO2 and GaP have been designed to tons.337 These highly energetic hot carriers generated from the non-
increase the absorption of light and broaden their working spectral radiative decay of surface plasmons can either directly interact with
range.328–331 For TiO2 metasurfaces, doping can be first used to intro- molecular adsorbates on the metal surface or be transferred into adja-
duce defect states near the bandgap edges, and the associated absorp- cent semiconductor or metal co-catalysts efficiently inducing chemical
tion is then increased at selected wavelengths of visible light by transformations.
engineering nonradiative modes via the interplay between electric and Plasmonic hot-electrons can be harvested in metal-
magnetic dipoles of the individual nanostructures forming the meta- semiconductor Schottky barriers, by combining the semiconductor
surface (meta-atoms), lattice modes, or the effects of bound states in catalyst with plasmonic nanostructures to achieve efficient electron–
the continuum. While the defect related excitation of electron–hole hole pair separation to prevent their direct recombination, thus
pairs may have its drawbacks, primarily in lower carrier mobility, the increasing the lifetime of the hot-carriers and prolonging their
enhanced absorption at the resonances in the visible spectral range can opportunity to interact with adsorbed molecules. One drawback of
be sufficient to demonstrate photocatalytic transformations at wave- metal–semiconductor heterostructure catalysts is the low charge
lengths where reactivity would be negligible without the metasurface. mobility from the Schottky contacts. Many designs use a combination
The impact of patterning also increases the surface area available for of plasmonic metasurfaces on or in a catalytic semiconductor layer
photocatalytic activity, which may be the dominant effect, as was dem- simply to increase the local temperature and enhance thermal
onstrated for NO degradation, when a 20-nm-thick TiO2 film was con- catalysis.
formally coated onto a photonic crystal, with some contribution also Alternatively, by incorporating strong plasmonic effects from
from the waveguided mode excitation enabled by the photonic metallic (Au, Cu, Al, etc.) nanostructures with highly catalytic active

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FIG. 11. (a) SEM images of the TiO2 metasurfaces for the photoreduction of Ag nanoparticles and the dependence of the obtained mean particle size as a function of illuminating time

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for the black TiO2 metasurface (red square line), the black TiO2 film (blue triangle line), and the conventional TiO2 metasurface (green dot line). Scale bar: 200 nm. The insets show the
corresponding structural colors under a bright-field microscope. A schematic of the electron transfer process is shown on the left.328 (b) An active metasurface based on a periodically
patterned SiNx coated with TiO2 photocatalyst. The spectra of the photochemical efficiency for the flat sample and the two different structured samples.332 (c) Enhancement of hydrogen
evolution reaction (HER) under simulated solar illumination from a dielectric metasurface made of amorphous a-GaP on an ITO-covered glass slide, compared to that with a 100 nm
thick continuous a-GaP film.331 (d) Wavelength-dependent reactivity for photocatalytic H2 dissociation using a quasi-BIC metasurface with and without Ni nanoparticle loading.334
Adapted with permission from.334 Copyright 2024 American Chemical Society. (e) Photo-electrocatalytic HER performances of core–shell Cu/Pt lattices combining individual LSPs and
collective plasmonic SLRs under different illumination wavelengths.335 Adapted with permission from Deng et al., Nano Lett. 21, 1523 (2021).335 Copyright 2021 American Chemical
Society. (f) Plasmon-enhanced visible-light-driven hydrogen production from water using a TiN plasmonic metasurfaces (blue line) and compared with a TiN film (black line).336 Adapted
with permission from Yu et al., ACS Photonics 8, 3125 (2021).336 Copyright 2021 American Chemical Society.

materials, core-shell or decorated nanostructures can be employed for nanocavities act as plasmonic “nanofurnaces” capable of reaching tem-
various types of reactions. Plasmonic metasurfaces decorated with peratures above 600 C under moderately concentrated solar irradia-
transition metals (Pd, Pt) can enable efficient coupling of light energy tion (20 Suns). Upon decoration with catalytic Rh nanoparticles, the
into a catalyst through strong electromagnetic field enhancement, hot- obtained photothermal metasurface achieved a high rate of CO2 pro-
carrier generation and photothermal effects. Such metaparticles (or duction under solar-spectrum-simulated light intensities342 as well as
hetero-nanoparticles) have demonstrated a significant increase in pho- in the reverse water gas shift reaction.343
tocatalytic activity over monometallic particles by efficient transfer of Metasurfaces based on arrays of strongly coupled bimetallic
hot carriers to the catalytic surface for various reactions.338–341 core–shell nanoparticles were also exploited to enhance photo-
As an alternative to conventional plasmonic metals, titanium electrocatalytic activity for hydrogen evolution reactions.335 Large-area
nitride (TiN) has started attracting significant attention for photocatal- Cu–Pt nanoparticle lattices fabricated by combining top-down lithog-
ysis. TiN metasurfaces can be designed to exhibit broadband optical raphy and solution-based chemistry support two different types of
absorption in the visible range (i.e., an average of more than 92% in plasmon modes, localized surface plasmons from individual particles
the 400–750 nm spectral range).336 When coated with a polymeric and surface lattice resonances (SLRs) from the 2D lattice, that
photocatalyst, plasmon-enhanced hydrogen production from water increased the catalytic activity under white-light illumination up to
under visible-light illumination was achieved, with the hydrogen evo- 60% [Fig. 11(e)].
lution rate increased by 300% compared to a smooth TiN film In addition to optical excitation by light illumination, hot elec-
[Fig. 11(f)]. The increased efficiency is attributed to a combination of trons can also be generated electrically by excitation with tunneling
enhanced light absorption, carrier separation, hot carrier transfer and electrons in tunnel junctions.344 Recent realization of an electrically
thermal effects induced by the plasmonic metasurface. Refractory plas- driven plasmonic nanorod metamaterial provides the opportunity to
monic TiN metasurfaces were also used for driving heterogeneous use an electron tunneling effect for the simultaneous excitation of hot
photothermal catalytic reactions. Self-assembled TiN cylindrical electrons and surface plasmons, providing the means to realize a new

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kind of hot-electron-activated nanoreactor. By constructing a high- The quality of semiconductor and plasmonic materials is of utmost
density array of plasmonic tunnel junctions at the top surface of a plas- importance. For plasmonic photocatalysts, different applications in
monic metamaterial composed of vertically oriented gold nanorods, photocatalytic metadevices may favor either rough or monocrystalline
the efficient electrical excitation of the plasmonic modes of the meta- and ultrasmooth interfaces depending on the requirements of hot elec-
material by inelastic electron tunneling can be realized. During the tron transfer to either molecules or semiconductor co-catalysts.345
tunneling process, the majority of electrons (99.9%) tunnel elastically In this regard, geometries and constituent materials can be opti-
in the electrically driven nanorod metamaterials, appearing as ener- mized by using numerical simulations to tailor the desired engineering
getic hot electrons in the nanorod tips. The highly efficient and con- optical response for reactions that require specific energies.
fined hot-electron generation makes the tunnel junctions highly Furthermore, advanced ab initio numerical methods could help
reactive and opens up opportunities for the precise activation of chem- deepen understanding of reaction mechanisms under specific light illu-
ical reactions in the junctions, which can be further detected with high mination conditions (intensity, light polarization) and optimize optical
sensitivity by observing the light emission from the tunnel junction or properties to create a database of photonic metasurfaces suitable for
by observing changes in the tunneling current due to the extreme sen- photocatalysis. Electron and thermal effects of the metasurface illumi-
sitivity of this highly confined tunneling process to any changes in the nation under both solar and pulsed laser illumination, as well as hot-
junction. electron transfer processes to reactants, need to be optimized. Machine
learning and deep neural networks (DNNs) have recently been dem-
C. Future directions and outlook onstrated to be powerful tools for designing efficient light-harvesting
metasurfaces due to their extraordinary capability to find solutions
Photonic metasurfaces have emerged as a promising platform for from a large data set or parameter space.346
driving photocatalytic reactions. To develop a highly efficient photoca- Product selectivity is a crucial aspect of any photocatalytic reac-
talyst with a photonic metasurface, several key design concepts need to tion that remains an ongoing concern and challenge. By engineering
be considered (Fig. 12). First of all, scalability of the fabrication the synergetic effects of electron transfer and temperature, as well as
method. For commercial exploitation, high durability, low unit cost, the choice of the materials for adsorption, there is an opportunity to
and efficient use of materials are undoubtedly the most appealing crite- explore the prescribed modification of the energy reaction landscape
ria for economic viability and sustainable chemical/energy production. to steer reactions toward the desired products. Many tests of the cata-
Most of the aforementioned metasurfaces were fabricated using EBL lytic properties of plasmonic metastructures are performed under
or lithographic techniques which are relatively expensive fabrication pulsed laser illumination which favors plasmonically derived hot-

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processes and do not offer a large catalytic surface area. Nanoimprint electron generation, and the peculiarities of CW illumination need to
lithography and self-assembled techniques can be used instead to be taken into account. Selectivity in the synthesis of chiral molecules is
reduce the fabrication cost. the utmost challenge for pharmaceutical industries, and chiral meta-
To justify the use of metasurfaces, it will be advantageous to move surfaces may play an important role in steering the chiral reactions
from expensive noble metals and employ sustainable earth-abundant under circularly polarized light illumination.
materials. For example, plasmonic metasurfaces made of transition Significant attention has been paid recently to the control of the
metal nitrides and phosphides, CuS, MXenes, copper, and aluminum chemical reactions through optical cavity modes, addressing specific
nanostructures need to be further investigated as a platform for engi- vibrational modes of the molecules to influence selectivity.347 These
neering light absorption for photocatalysis and photo-electrocatalysis. studies have been performed until now in optical cavities which select

FIG. 12. Challenges (left) and requirements (right) for practical applications of optical metasurfaces in photocatalysis.

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the spectrum of the electromagnetic modes available for strong- A. Introduction

coupling to vibronic modes of the reactants. Metasurfaces and Structuring light in multiple degrees of freedom, from spatial to
metaparticles may play an important role in these photochemical trans- temporal, holds great promise for advancing modern photonics
formations as they can be engineered to provide high quality-factor from both fundamental and applied aspects. In particular,
vibrational modes for coupling to molecular vibrational states.348 structured-light fields have proven useful for numerous photonic
applications, including super-resolution microscopy,349 optical trap-
D. Concluding remarks ping,350 multimode imaging,351,352 and holography,32,208,353 optical
Metasurfaces and metamaterials providing precisely designed communications,354,355 nonlinear light conversion,356 chiral sens-
light–matter interactions offer an exquisite platform for understanding ing,357,358 and quantum information processing.359–361 Conventional
the mechanisms of light-induced chemical transformations, hence generation of structured light typically relies on multiple cascaded
revealing routes to optimization. Through targeting either electron- phase and wave plates in bulky form, imposing major challenges for
induced and/or thermal effects via the design of the composition and their practical applications. Over the past decade, flat optics, also
structure of metamaterials, understanding of the role and interplay known as ultrathin metasurfaces,5 have become a new topic in the
between electronic and thermal contributions in the reaction can be photonics community. Recently, such metasurfaces have been largely
achieved, and their relative weight can be adjusted to control reaction developed for the generation, manipulation, and detection of struc-
pathways. Beyond fundamental research, metasurfaces can be readily tured light. Here we summarize the key physical concepts demon-
applied in synthesis of high-value chemicals where small quantities of strated for generation of various kinds of structured light with
metasurfaces. Apart from the generation, we highlight some exciting
products, cost and femtosecond laser illumination are not prohibitive
applications of metasurface manipulation of structured light, includ-
issues. Similarly, they provide an excellent platform for multiplexed
ing but not limited to metasurface lasers with tailored spatial modes,
functionalities, such as sensing and photochemical transformations,
metafibres capable of transforming arbitrary vector beams, vectorial
useful for environmental applications and pollution remediation.
metasurfaces that can create optical skyrmions, high-bandwidth
In order to advance metamaterial-based catalysis concepts into
twisted light holography, vortex metalens for edge enhancement,
mainstream photocatalysis, the problem of scalable production must
and metasurface-structured quantum emission. We also discuss
be addressed together with a reduction of the associated costs, which
some of the major challenges that lie ahead for the large deployment
can be achieved by moving away from top-down approaches toward
of structured-light metasurfaces. Finally, we provide some insights
self-assembly, electrochemistry, laser printing, or nanoimprint lithog-

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into recent new advances in metaphotonics that could potentially
raphy for roll-to-roll fabrication. The planar nature of metasurfaces mitigate these challenges and push the field forward by creating
and metamaterials is advantageous for photo-electrochemical reactors more research impact.
and generally for photochemistry, where light-management issues are
important considerations. Beyond these, the transfer of the light-
B. State-of-the-art
harvesting properties designed for metasurfaces into a metaparticle
platform holds much promise for the application of these designs in a In meta-optics, both plasmonic antennas and dielectric pillars
scaleable manner compatible with chemical industry standards. have been used for the metasurface generation of different structured
Harnessing metasurfaces and metamaterials as photocatalysts light fields in real space. For instance, a helical phase profile that car-
has emerged in the catalysis community because of their ability to ries the orbital angular momentum (OAM) has been imprinted by a
harvest sustainable solar energy to promote chemical reactions. phase-only metasurface, with the use of a set of meta-atoms that
It is a comparatively new area of photonics and metamaterial offer a complete phase modulation (from 0 to 2p). Ultrathin plas-
research that is growing rapidly and showing promising results. monic metasurfaces based on near-field mode hybridization have
Due to the ongoing climate and energy crisis, much research effort been designed to implement the OAM phase [Fig. 13(A-a)].5 High-
is currently focused on finding catalysts to combat environmental index dielectric nanopillars with strong mode confinement, operat-
problems such as CO2 reduction, NOx decomposition, and ammo- ing as truncated waveguides, have also been used to realize different
phase vortices [Fig. 13(A-b)].85 Huygens’ metasurfaces of high trans-
nia production to name but a few, and to provide renewable and
mission efficiency offer an alternative platform to realize phase vorti-
clean energy with sustainable input through water splitting, etc.
ces through spectrally overlapping electric and magnetic Mie
Metasurfaces, metamaterials and metaparticles have an important
resonances [Fig. 13(A-c)].362,363 Apart from the use of phase-
role to play in achieving net-zero pollution.
sensitive elements for creating phase vortices, plasmonic and dielec-
tric nanostructures can be designed to possess strong polarization
ACKNOWLEDGMENTS birefringence, exhibiting different phase accumulations for the polar-
This work was supported by the UK EPSRC under Project No. ization along the long and short axes [Fig. 13(B)].16,20,364 Geometric
EP/W017075/1. metasurfaces based on the Pancharatnam–Berry phase principle
have been used to create polarization-encoded phase vortices
VII. ORBITAL ANGULAR MOMENTUM AND through the in-plane rotation of an identical asymmetric nanostruc-
WAVEFRONT CONTROL ture. Meta-atoms with both varying orientation and size have been
further developed to control arbitrary orthogonal polarizations in an
Haoran Ren, Yuri Kivshar, and Stefan Maier independent manner.365 As such, the output phase response for
orthogonal polarization incidence can be decoupled from each other,

[Link]@[Link] leading to the generalized spin-to-OAM conversion of light that

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FIG. 13. Illustration of the metasurface generation of structured-light fields and their use for various photonic applications. (A) Spiral phase metasurfaces directly imprint a spiral
phase profile via phase-sensitive elements made of (a) hybrid plasmonic antennas, (b) high-aspect-ratio dielectric nanopillars, and (c) flatter dielectric nanopillars satisfying the
first Kerker condition. (B) Geometric phase metasurfaces encode the spiral phase profile onto the cross-polarization component from the metasurface by using birefringence (a)
plasmonic and (b) dielectric nanostructures. (C) J-plate metasurfaces exploit the complete and independent phase and polarization control, capable of creating different OAM
modes at arbitrary orthogonal polarization outputs. (D) An intracavity metasurface enables coherent laser emission with tailored structured-light modes. (E) Structured-light
metafibres interfaced on the fiber end-faces can transform the fiber output into arbitrary selected structured-light fields on the hybrid-order Poincare sphere. (F) Vectorial meta-
surfaces enable the creation of free-space optical skyrmions carried by topologically nontrivial 3D vectorial textures. (G) Metasurface OAM holography allows the multiplexing
of a range of OAM-selective holographic images. (H) A spiral metalens can perform a 2D spatial differentiation operation and achieve isotropic edge detection under ambient
sunlight illumination. (I) A polarization-beam-splitting metalens has been used for structuring quantum emission in multiple degrees of freedom from ultra-bright defects in hex-
agonal boron nitride at room temperature.

creates different OAM modes at orthogonal polarization outputs.366 transformations370 along the optical path, which may inspire new
Such metasurfaces are designed by exploiting the complete and inde- directions in singular optics toward 3D space. In addition, temporal
pendent phase and polarization control by single meta-atoms based shaping of light, especially in the ultrafast domain, has benefited wide-
on the Jones calculus, named as J-plate metasurfaces [Fig. 13(C)]. ranging photonic applications.50,371 Spatio-temporal metasurfaces
Notably, J-plate metasurfaces pave the way of using a single metasur- have thus been created by combining a frequency comb source with a
face for creating arbitrary structured light on the hybrid-order passive metasurface, capable of steering optical beams with a wide
Poincare sphere.367 steering angle in just a few picoseconds.50 In addition, metasurface-
Unlike traditional refractive or diffractive optics constrained from enabled pulse shapers have been demonstrated by embedding a dielec-
a limited access to multi-dimensional wavefront shaping, meta-optics tric metasurface in the focal plane of a Fourier-transform pulse shaping
has offered an unprecedented opportunity for structuring light fields setup.371 Such a Fourier-transform pulse shaper has recently allowed
in multiple degrees of freedom, from transverse to longitudinal (propa- the generation of spatiotemporal optical vortices carrying previously
gation direction) planes, as well as from spatial to temporal domains. unexplored transverse OAM modes.372,373
Propagation-invariant or non-diffracting light beams, such as caustic Over the last decade, structured-light metasurfaces have found
beams whose transverse intensity distribution remains invariant over a many applications in the optics-related fields. Here we present only a
significant propagation distance, exhibit high robustness and a self- few highlights, including but not limited to intracavity metasurface
healing behavior.368 This has inspired metasurface generation of lasers, metafibers harnessing structured-light fields, generation of opti-
multiple phase vortices369 as well as on-demand polarization cal skyrmions in free space, metasurface holography using twisted light

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modes, vortex metalenses for edge detection, and the manipulation of emission from ultra-bright defects in hexagonal boron nitride (hBN),
quantum emission. Incorporating structured-light metasurfaces in a as well as enable simultaneous manipulation of multiple degrees of
solid-state or fiber laser cavity has enabled coherent light emission freedom of a quantum light source, including directionality, polariza-
with tailored spatial mode profile, such as high-purity vortices374 and tion, and the OAM of light. Dielectric metasurfaces can also be used
vortex arrays,375 in a compact form factor [Fig. 13(D)]. This paves the for the manipulation and even direct generation of entangled photon
way for the development of the next generation of miniaturized laser pairs.383 A geometric metasurface was first used in a spontaneous para-
sources with tailored spatiotemporal mode control. The current use of metric downconversion setup for the nonlocal spin and OAM correla-
structured light in optical fiber science and technology is limited by tions on entangled biphoton states.361 In this context, quantum state
mode mixing, and hence generation of structured light is most usually engineering mainly relies on the nonlinear optical effects, including
handled outside the fiber via bulky optics in free space. A new meta- spontaneous parametric downconversion and four-wave mixing,
fiber platform has been introduced for implementing ultrathin meta- where one or two pump photons spontaneously decay into a photon
surfaces directly on the end face of optical fibers.376,377 Polymeric pair. These nonlinear effects typically require the use of bulky nonlin-
metasurfaces, with unleashed height degree of freedom, were 3D laser ear crystals by matching the momentum of the participating photons.
nanoprinted and interfaced with polarization-maintaining single- Nonlinear metasurfaces have subwavelength thickness and allow the
mode fibers. Multiple metasurfaces were interfaced on the fiber end- relaxation of this constraint,34 opening new possibilities of quantum
faces, capable of transforming the fiber output into arbitrary selected state engineering. Recently, metasurface generation and manipulation
structured-light fields on the hybrid-order Poincare sphere of entangled photons via spontaneous parametric downconversion
[Fig. 13(E)].377 have been demonstrated by high-quality-factor nonlinear metasurfaces
Allowing subwavelength-scale-digitization of optical wavefronts made of lithium niobate137 and gallium arsenide384 materials. These
to achieve complete control of light at interfaces, metasurfaces are par- results suggest that metasurfaces can offer a versatile platform for cre-
ticularly suited for the realization of planar holograms that promise ating complex photon quantum states toward high-dimensional pho-
new applications in high-capacity information technologies. Recent tonic quantum processing.
advances in metasurfaces and Fourier holography have offered an
unprecedented opportunity to control optical wavefront in the spatial- C. Future directions and outlook
frequency domain. Metasurface holograms have shown the indepen- Structured light, with many millions of spatial modes in a tiny
dent control of both the 3D polarization378 and the OAM cross section area of light, has shown great potential in transforming
states32,208,353 of individual spatial-frequency components, represented

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the landscapes of a wide range of photonic applications, from classical
by different image pixels reconstructed from the metasurface holo- to quantum regimes. Meanwhile, metasurfaces have provided scientists
grams in the Fourier plane. It opens the door to the use of a single and engineers with versatile tools to generate, manipulate, and sculpt
metasurface for creating optical skyrmions with topologically nontriv- optical fields. Although numerous advancements have been made in
ial 3D vectorial textures379 [Fig. 13(F)], as well as for reconstructing both the structured light and metasurface fields, there remain certain
distinctive images from different OAM states [Fig. 13(G)].32,208 challenges in the science and technical aspects of structured-light
Meanwhile, structured light has fueled many photonic applications in metasurfaces. Even though metasurfaces benefit from the use of sub-
imaging, microscopy, and optical communications. For instance, the wavelength meta-atoms to digitize optical wavefronts, the accuracy
donut-shaped OAM beam in the focal region of a microscopic objec- and efficiency of their amplitude, phase, and polarization modulations
tive lens can deactivate fluorophores, minimizing the effective area of still need to be improved. For instance, for a phase-type metasurface,
illumination and leading to super-resolution imaging. In addition, a increasing the number of gray levels is important to reach near-unity
spiral phase metasurface incorporated in a Fourier filtering optical diffraction efficiency, but this is indeed challenging for metasurfaces
setup can perform a 2D spatial differentiation operation and achieve that rely on size-varying meta-atoms to realize the phase modulation.
isotropic edge detection.380 A recent polarization-multiplexed metalens Recent developments in 3D laser-nanoprinted metasurfa-
integrated with a polarization camera has allowed single-shot edge ces,208,376,377,385 multilayer,386 and cascaded metasurfaces,387 as well as
detection of indoor and outdoor scenes under ambient sunlight illumi- in hybrid metasurfaces that combine both refractive and diffractive
nation [Fig. 13(H)].381 Practical OAM communication systems suffer optical elements388 may alleviate this major challenge by unlocking 3D
from turbulence-induced phase distortions to the propagating beams, design degrees of freedom.
decreasing the orthogonality of OAM modes through introduced Current structured-light metasurfaces still require external source
modal crosstalk. An ultrathin OAM mode-sorting metasurface was excitation, making them difficult to be integrated on-chip. Integration
recently used for characterizing the OAM orthogonality breakdown of metasurfaces with on-chip light sources, waveguides, and detectors
under different turbulence conditions.382 It allows the measurement of will provide an exciting opportunity for future metasurface systems-
the whole OAM spectrum at the same time, suggesting that metasurfa- on-a-chip. Recently, generation of free-space structured light with pro-
ces with a small form factor can be integrated with practical communi- grammable integrated photonics was demonstrated.389 More compli-
cation systems for compact, fast, and efficient detection of twisted light cations of using structured-light fields include strong modal coupling
in turbulence environments. and intermodal crosstalk, due to free-space turbulence, large beam
Structured photons in the quantum regime promise enhanced divergence, and misalignment in the detection process. Despite a great
security by harnessing structured light as high-dimensional quantum success has been made in the metasurface generation and manipula-
states. An ultrathin polarization-beam-splitting metalens was demon- tion of structured-light fields, metasurface-based selective detection of
strated for arbitrary structuring quantum emission at room tempera- complex spatial modes, for instance, arbitrary selected states on
ture [Fig. 13(I)].359 The quantum metalens can collect the quantum the hybrid-order Poincare sphere, is still elusive today. Nonlinear

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metasurfaces have been developed to observe high-order nonlinear structures smaller than working wavelengths provided an alternative
optical spin–orbit interactions,390 as well as non-reciprocal asymmetric method to enhance the controllability of birefringence.399,400 The
generation of visible images.391 Owing to the use of subwavelength drawback of materials with subwavelength structures was their
meta-atoms, nonlinear metasurfaces hold tremendous promise for extreme anisotropic requirement with very high aspect ratios.
enhancing the toolkit for structured light–matter interactions beyond
the limits of linear optics. While major challenges still exist on both sci- B. Optical field manipulation in polarization-based
ence and technical aspects of structured-light metasurfaces, we believe holography
these challenges are rather likely the driving forces to inspire more
To tackle the challenges in conventional optics, metasurfaces
innovations and push the field forward.
have provided more degrees of freedom and better performance, par-
ACKNOWLEDGMENTS ticularly manifesting polarization-dependent physical channel multi-
The authors acknowledge financial support from the plexing.401–405 Initial demonstration of polarization multiplexed
Australian Research Council DECRA Fellowship DE220101085 holograms based on plasmonic metasurfaces suffered from poor qual-
(H.R.) and Australian Research Council Discovery Project ity and low efficiency.5,406 Wen et al. proposed and experimentally
DP220102152 (H.R., S.A.M.). S.A.M. additionally acknowledges the demonstrated highly efficient helicity multiplexed metahologram with
Lee-Lucas Chair in Physics. good image quality in the near-infrared and visible range.407 In this
work, the issues of poor image quality and low efficiency were resolved
VIII. METASURFACES FOR HOLOGRAPHY AND by leveraging the high efficiency and broadband property of reflective
STRUCTURAL COLOR metasurfaces.20 Two off-axis holographic images were reconstructed
under the illumination of a circularly polarized (CP) light beam. The
Xianzhong Chen and Muhammad Afnan Ansari images were symmetrically distributed and interchangeable by control-

ling the helicity of the CP light beam as shown in Fig. 14(a).407 The
[Link]@[Link] right panel of Fig. 14(a) shows the change of holographic images (bee
and flower) when the polarization of the input light beam is changed
A. Introduction from left circular polarization (LCP) to right circular polarization
Optical holography has been used for several decades for recon- (RCP). The helicity multiplexed property for CP light was attained by
structing 3D images by shaping the wavefront of a light beam. Unlike interleaving two metasurfaces comprised of plasmonic nanorods.

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multiview parallax and photography techniques, a hologram consists Polarization-sensitive metaholograms for input light beams with ellip-
of complete information of an object. The recording in the holographic tical, linear, and arbitrary orthogonal polarizations have also been
technique is not an image itself, rather it contains random patterns of reported in the literature.365 Helicity multiplexed metaholograms have
varying phase or intensity.392 The holograms can be reconstructed attracted various exciting applications in optical field manipulation
either by the interference of a reference light beam with a scattered such as stimuli-responsive (e.g., pressure, voltage, temperature, and
light beam from a real target or by calculating the phase profile of the gas) and tunable metaholograms.408–410 For example, a volatile gas
light beam at the interface of a hologram. The phase profile can be sensor based on helicity multiplexed metahologram integrated with
encoded into the spatial light modulators or surface structures using liquid crystals was presented to sense isopropyl alcohol gas by generat-
lithography. The process involving the computer-generated phase ing a visual alarm.408 In this work, the response of gas was recorded
information is known as computer-generated holography (CGH).393 with different geometries of the designer liquid crystal (nematic and
In the traditional holography and diffraction optics, the light field is isotropic) by integration with an asymmetric metasurface. The pro-
regarded as a scalar field with two parameters, i.e., intensity and phase posed non-interleaved asymmetric metasurface411–413 employed both
of the light beam.394 With the ongoing advancements in nanofabrica- geometric and propagation phase for the phase modulation. The over-
tion techniques, the last decade has witnessed the rapid development all phase retardation was controlled by controlling the cell order of liq-
of ultrathin and flat optical devices with unique degrees of freedom. uid crystals through the external stimulus, i.e., the presence of gas. The
One degree of freedom is the independent control of polarization dis- tunable phase retardation adjustment of output light beam with
tribution in the engineered light path, which remains the cornerstone desired polarization state using asymmetric metahologram and liquid
for multifunctional holography, e.g., vectorial holography.395 The crystals have opened new avenues to detect chemical and biomedical/
traditional bulky optics were also used to a certain extent to introduce biological substances in real-time for public health and environmental
the concept of polarization holography for two-channel orthogonal monitoring.408,409 Recent studies on optical polarization multiplexing
polarization control using birefringent materials.396 These have further demonstrated the ability of metasurfaces to realize inde-
polarization-dependent computer-generated holograms are sensitive pendent amplitude and phase modulations with non-orthogonal
to the polarization state of the incident light beam and capable of sepa- polarizations, which further expanded the ability of metaholograms for
rating readout light through its polarization to generate distinct holo- the full vectorial holography.407,414,415
graphic images. This led to various novel applications such as multi- Furthermore, holography has been widely used to achieve beam
optical switching and image processing.397,398 However, the conven- shaping,416 surface plasmon holographic displays,417 data storage,418
tional holographic recording medium and diffraction optics suffered optical trapping,419 diffractive laser tweezers,420 and digital holographic
from a limited degree of freedom and were unable to achieve simulta- microscopy.421 Although two-dimensional (2D) holograms were
neous control of polarization state and spatial light field distributions. experimentally reported using metamaterials and metasurfaces, none
The form and magnitude of such type of birefringence were limited to of them have achieved 3D image reconstruction using CGH in the visi-
naturally occurring crystals. On the other hand, materials with ble domain. To fulfill the essence of holography in 3D space, Huang

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FIG. 14. Polarization sensitive metasurface holograms, 2D polarization structures and their combination. (a) Helicity multiplexed holograms. Two central symmetric helicity-
dependent holographic images are reconstructed under the illumination of LCP (bee and flower) and RCP light beams (flower and bee). (b)–(d) Schematic diagram of a 3D
metasurface hologram. (c) A 3D object (jet) and (d) Experimentally obtained a real holographic image of the jet at an observation plane under the illumination of an RCP light
beam. (e)–(g) Schematic for hiding a gray-scale high-resolution image in a laser beam through metasurface based on Malus’ law. (f) The hidden image of James Clerk Maxwell
is revealed with a linear polarizer (analyzer). (g) Detailed information in the eyebrow area (10 10 pixels). The right and left FIGS show the polarization distribution and the cor-
responding intensity profile. (h)–(j) Mechanism of polarization encryption for encoding a color image. (h) The target image of flower (red) and leaves (green). (i) Detailed infor-
mation in the selected region (6 5 pixels) of the target image (top panel) and the corresponding orientation angles and feature sizes of dielectric nanopillars (bottom panel).
(j) Results of metasurfaces for hiding a color image based on color mixing, which is realized with a metasurface consisting of supercells. (k)–(m) A metasurface that can simul-
taneously realize polarization sensitive and insensitive holograms and 2D polarization profiles for hiding a high-resolution image (a castle), which can increase information chan-
nels and information density. Panels (a) reproduced with permission from Wen et al., Nat. Commun. 6, 1 (2015).407 Copyright 2015 Springer Nature. (b)–(d) Reproduced with
permission Huang et al., Nano Lett. 13, 3559 (2013). Copyright 2013 Springer Nature.426 (e)–(g) Reproduced with permission from Yue et al., Light 7, 17129 (2017).423
Copyright 2017 Springer Nature. (h)–(j) Reproduced with permission from Zang et al., Adv. Mater. 30, 1707499 (2018). Copyright 2018 Wiley-VCH.424 (k)–(m) Reproduced with
permission from Intaravanne et al., Adv. Photonics Res. 2, 2000046 (2021). Copyright 2020 Wiley-VCH.425

et al. presented a relatively simpler approach to realizing 3D hologra- incorporation of spatially varying polarization along with the phase
phy using ultrathin metasurface consisting of subwavelength metallic distribution is essential to fully unlock the potential of metasurfaces for
resonators with varying orientation as shown in Fig. 14(b).392 The increased information storage. Yue et al. proposed such a technique to
phase information of the 3D object was calculated using commercially encrypt a 2D grayscale image (of James Clerk Maxwell) in a structured
available CGH algorithm.422 In the CGH algorithm, the 3D target laser beam with inhomogeneous polarization distribution using meta-
object [Fig. 14(c)] was considered as a collection of many point sour- surface based on Malus’ law as shown in Fig. 14(e).423 The result of the
ces. The complex amplitude at the hologram interface was numerically intensity profile of the encrypted grayscale image was revealed with an
calculated through the superposition of the wavefronts of all point analyzer (linear polarizer) as shown in Fig. 14(f). To further explain
sources. Upon the illumination of the CP light beam, the metasurface the technique, a selected portion from the eyebrow area (10 10 pix-
reconstructed a real 3D holographic image within the Fresnel range of els2) is enlarged in Fig. 14(g) to show the intensity and its correspond-
hologram as shown in Figs. 14(b) and 14(d). As explained earlier, the ing pixel-level polarization distribution. It is noted that the resultant

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beam exhibited a subwavelength resolution. Similarly, metasurfaces 3D space. Therefore, a solution is required to address this problem at
can also be used to encode colorful images in inhomogeneous polariza- the fundamental level where new control variables can be incorporated
tion profiles based on Malus’s law. Zang et al. experimentally demon- into the metasurface design procedure. The required control variables
strated simultaneous encryption of intensity and color information for an arbitrary 3D polarization structure include wavelength, wave-
into a wavelength-sensitive polarization distribution.424 This technique front positioning (x, y, z), and dynamic polarization rotation in a 3D
was used to embed high-resolution color images with precisely con- space. Much work has been done to address one control parameter at
trolled contrast and brightness onto a dielectric metasurface as shown a time,407,412,425,426,430 however, simultaneous control of all parameters
in Figs. 14(h)–14(j). The target high-resolution color image of a rose is scarce and challenging. The combinational control of more than one
was selected which encompassed green and red pixels with the varia- parameter is also expected to yield unique optical field manipulation.
tion of spatial brightness as shown in the top panel of Fig. 14(i). The Recently, Zang et al. proposed a metalens with polarization functional-
corresponding wavelength-dependent polarization distributions were ity through the superposition of both RCP and LCP components of
different for both colors and mapped by controlling the orientation the light beam at each focal spot under the illumination of linearly
and the feature size of the dielectric nanopillars as shown in the bottom polarized incident light beam.431 The authors started from a simple
panel of Fig. 14(i). Vivid red petals and green leaves were revealed with lens model by incorporating an additional term for the polarization
the right transmission axis of the analyzer under the illumination of rotation / in the phase profiles of LCP and RCP components. Since a
660 and 550 nm wavelengths. The same method was also used to pro- linearly polarized incident light beam can be divided into LCP and
duce polarization-encrypted colorful images using additive color mix- RCP light components, therefore, a portion of the transmitted wave is
ing of the primary colors as shown in Fig. 14(j). In this work, a converted to LCP light to focus with an additional phase shift /, and
supercell contains nanopillars with different feature sizes, which the other portion is converted to RCP light with an additional shift of
respond to different wavelengths.424 By integrating such high- /. The idea was then extended to realize multiple focal points using
resolution polarization encryption techniques with holography, many the superposition method with independent polarization rotations as
diverse applications can be realized in information security, anticoun- shown in Fig. 15(a). Wang et al. presented an off-axis multi-foci metal-
terfeiting, and high-density data storage. For example, an application ens model to incorporate polarization rotations in four different focal
of optical information security was experimentally demonstrated by points at different locations on the observation plane as shown in
integrating an arbitrary polarization distribution for image conceal- Fig. 15(b).432 Unlike the previous work where only linear polarization
ment and a hybrid CGH as shown in Fig. 14(k).425 The functionality rotations are created, Wang et al. introduced RCP, LCP, and linear
was achieved by simultaneously concealing a high-resolution image in

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polarization rotations for the application of polarimetry to detect the
the polarization distribution and encoding holographic images polarization of arbitrary incident light beams. The ellipticity, handed-
through the superposition of two-phase profiles for orthogonal CP ness, and major axis of the polarization state of the incident light beam
light beams. As a result, a metasurface was used to reconstruct holo- were determined through the measured intensities of the four focal
graphic images at the observation plane either under the illumination points.432 Both designs have provided a unique insight into a pixel-
of linearly polarized light beam without the analyzer or under the illu- level simultaneous control of wavefront along with the independent
mination of RCP light beam as shown in Fig. 14(m). The desired con- polarization rotations. More specifically, both unique ideas of polariza-
cealed image was revealed with a predesigned angle combination of tion rotation at different focal lengths (f1 and f2) along the z-direc-
the analyzer and input linear polarizer as shown in Fig. 14(l). In con- tion431 and the off-axis (xi, yi) multi-foci metalens432 have led to the
trast, the other transmission axis combination of the analyzer and generation of 3D polarization structures. An optical focal curve can be
input linear polarizer could not generate meaningful information. The regarded as a continuous structure if the number of focal points along
work also investigated the simultaneous incorporation of polarization- the curve becomes infinite. Wang et al. started from a muti-foci metal-
sensitive and insensitive holograms with high-resolution image ens with discretized focal points to a continuous optical curve along an
encryption in the polarization distribution, which further enhanced arbitrary trajectory by increasing the number of focal points.433 In the
the information capacity and hence can be utilized for high-level anti- next step, the 2D polarization curve model was transformed to 3D
counterfeiting. polarization knot design by introducing the longitudinal parameter (z)
as an additional control variable in the phase terms using the superpo-
C. Toward 3D polarization structures: challenges and sition method. As a result, 3D light fields along with spatially varying
future directions inhomogeneous polarization distributions and intensity patterns were
2D high-resolution image encryption based on spatially varying generated in the form of 3D optical knots as shown in Fig. 15(c).433
polarization distributions has been realized with metasurfaces.423–425 The predesigned polarization distribution was confirmed through the
However, in addition to the phase, intensity, and color, the encryption modulated intensity patterns with an analyzer (linear polarizer). In
of spatially varying polarization distribution in a 3D space remains a addition to the predefined inhomogeneous polarization distribution,
challenge. To generate the desired wavefront and dynamically manipu- the polarization rotation at each point on the 3D trajectory was
late the polarization distribution in a 3D space, an independent pixel- dynamically modulated by changing the polarization state of the inci-
level control of phase and polarization is simultaneously required dent light beam. The complete evolution of the 3D structure was also
along the light’s propagation. The biggest challenge to achieve such observed and measured using a CCD camera as shown in Fig. 15(d).
functionality is the limited degree of freedom in the current metasur- Intaravanne et al. introduced a new control variable (wavelength k) in
face design. Although few studies have shown unprecedented abilities the design procedure along with polarization rotation / and 3D focal
to break the conventional limits to some extent,415,427–429 they are still position (u, v, f) to demonstrate wavelength selective 3D polarization
unable to address the complete and dynamic control of light fields in a structures as shown in Fig. 15(e).434,435 At a given observation plane,

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FIG. 15. Metalenses for realizing polarization rotation, 3D polarization structure manipulation and a compact spectrometer. (a) A multi-foci metalens with a polarization rotation func-
tionality. (b) Application of multi-foci metalens for the polarization detection in the THz range. (c) Customized 3D polarization structures based on multi-foci metalens. (d) Simulated
and experimental intensity distributions of 3D structures at different observation planes under the illumination of an RCP incident light beam. (e) Metasurface for color-selective 3D
polarization structures. The left panel and right panel show the light intensity distributions without and with an analyzer, respectively,. (f) A compact metasurface spectrometer based
on multi-foci metalens. (g) Light intensity distribution under the illumination of different monochromatic incident light beams. (h) Spectrum detected by the metasurface spectrometer
under the illumination of the polychromatic incident light beam. Polychromatic light beam contains five different wavelengths. Panels reproduced with permission from: (a) repro-
duced with permission from Zang et al., Laser Photon. Rev. 13, 1900182 (2019).431 Copyright 2019 Wiley-VCH. (b) Reproduced with permission from Chang et al., J. Vac. Sci.
Technol., B 21, 2755 (2003). Copyright 2020 Optica Publishing Group (formerly OSA).432 (c) and (d) Reproduced with permission from Wang et al., Nano Lett. 21, 2081 (2021).
Copyright 2021 American Chemical Society.433 (e) Reproduced with permission from Intaravanne et al., Light Sci App 11, e302 (2022). Copyright 2022 Springer Nature.434 (f)–(h)
Reproduced with permission from Intaravanne et al., Adv. Opt. Mater. 12, 2203097 (2024). Copyright 2023 Springer Nature.435

different 3D polarization knots were generated by changing the wave- points at will, the wavelength of the incident light beam can be
length of the incident light beam as shown in the left and right panels detected accurately by mapping the wavelength information to the
of Fig. 15(e). The right panel and left panels present the intensity distri- intensity distribution. A compact spectrometer was realized by tailor-
bution of corresponding 3D polarization structures with and without ing the dispersion based on the model of multi-foci metalens as shown
the analyzer, respectively. in Fig. 15(f).436 The metasurface-based spectrometer can focus and split
The ability to generate arbitrary wavelength-dependent 3D polar- the monochromatic [Fig. 15(g)] and polychromatic light beams
ization structures with ultrathin metasurfaces can be of interest to [Fig. 15(h)] of different wavelengths to desired positions on an observa-
many pragmatic applications such as integration optics for compact tion plane with 1 nm resolution. This unique dispersion control and high
spectrometers, and longitudinally variable structures for 2D and 3D nanometer spectral resolution were achieved over a broadband range in
optical image steganography. For example, motivated by the intrinsic the visible domain. The application of the proposed multi-foci metalens-
dispersion property and ability of metalens to generate multiple focal based spectrometer proved that this technology has clear potential for

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development in on-chip integrated photonics where wavelength detec- the need for a transparent medium precludes the use of conventional dis-
tion, information processing, and spectral analysis are required in a com- plays. This requirement for transparency poses challenges, but it also pro-
pact platform. Like other emerging technologies, further improvements motes widespread acceptance of the technology. It benefits specialized
in the current design are required and new challenges need the attention applications such as assisted surgical operations or equipment mainte-
of the research community. For example, the demonstrated metasurfaces nance, as well as end-user applications such as smartphones.
have a low conversion efficiency, which is associated with the symmetric The main elements of an AR system are the image projector, which
spin–orbit interactions and can be resolved by employing the nanoreso- creates the digital image, and the optical combiner, which blends digital
nators with asymmetric spin–orbit interactions.411–413 Furthermore, the and real images before delivering the combined picture into the user’s
polarization manipulation can be extended to incorporate arbitrary eyes.440 Depending on the system architecture, the image projector con-
polarization states, including linear, elliptical, and circular polarization sists of a light source (laser or LED), a spatial light modulator that mod-
states. The integration of metasurfaces with materials such as 2D transi- ulates the light to create an image, e.g., based on liquid crystals or digital
tion metal dichalcogenides,437 conducting oxides,438 liquid crys- micro-mirrors, and image-forming optics such as lenses and mirrors.
tals,408,409,439 and active materials209 can add the extra degree of freedom The optical combiner has been the subject of intense research over the
and perform complicated optical tasks that are impossible or extremely last few years and is the focus of this paper. Combiners started as bulky
challenging only with passive metasurface design. and irregularly shaped glass elements,440 as shown in Fig. 16(a), they
then evolved into sophisticated photonic devices, usually involving
IX. META-OPTICS FOR AUGMENTED REALITY
nanostructures [Figs. 16(b) and 16(d)].
APPLICATIONS
The most common configuration used for optical combiners to
date is an optical waveguide that delivers light toward the observer via
Yuhui Gan, Arseny Alexeev, Thomas F. Krauss, and
a Holographic Optical Element (HOE)441 or a Surface Relief Grating
Andrea Di Falco
(SRG)442 [Fig. 16(b)]. Both HOEs and SRGs are manufactured using
nanoscale lithographic techniques. Another type of optical combiner
adf10@[Link]
uses metalenses [Fig. 16(c)],443 which are actively being explored for
AR applications due to their low weight and their ability to imprint
A. Introduction any desired phase distribution onto the incoming wave; therefore, met-
Augmented reality (AR) superimposes computer-generated content alenses can replace freeform optical elements due to their advanta-
onto a transparent medium such that the user can perceive the real world geous form factor and functionality. We note that several reviews

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augmented with the artificial content; this contrasts with virtual reality describing AR systems using both waveguide combiners and metal-
(VR), whereby a computer generates all the content. In AR applications, enses are already available,444 which this perspective article aims to

FIG. 16. Four AR architectures: (a) freefrom optical combiners; (b) waveguide combiners with metagratings; (c) prism combiners with a metalens; (d) holographic metasurface
combiners. (a)–(c) use full-color projectors to generate virtual image; and (d) uses plain laser beams and the virtual image is encoded in the metasurface.

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complement. Here, we first introduce the key parameters and figures on the user due to the shape and weight of the freeform mirror and its
of merit of an AR near-eye transparent display and then briefly review tilt. Additionally, this design is fundamentally restricted by the conser-
the state-of-the-art of various meta-optical technologies that are being vation of etendue, as discussed before.
used in consumer-grade AR glasses. Finally, we discuss the perfor- Waveguides—Currently, the most popular implementation of the
mance tradeoffs of each approach, including the use of transparent AR optical combiner function consists of an imaging waveguide with
holographic displays based on metasurfaces. The holographic diffractive elements. In a typical arrangement, three linear diffraction
approach eliminates the need for an image projector, thus achieving a gratings are used, (i) to deliver the image rays created by the projector
minimalistic form factor while delivering superior optical perfor- into the first diffracted order below the angle of total internal reflection
mance, as shown in Fig. 16(d). of the glass-air interface, thus in-coupling image rays into the wave-
guide; (ii) split the image rays into higher diffraction orders, thereby
B. State of the art replicating the image pupil; and (iii) diffract the image rays at multiple
points into the user’s eye, thus, outcoupling the image rays from the
1. Parameters waveguide. The key advantage of this approach is that the waveguide
AR display systems must meet a variety of performance metrics, produces copies of the image pupil, thereby surpassing the fundamen-
which can sometimes conflict one another. For example, the field of tal trade-off between the FoV and the eyebox imposed by the conser-
view (FoV) describes the range of angles at which optical rays are vation of etendue, achieving FoV > 60 and eyebox > 10 mm without
delivered to the human eye to form an image on the retina. The FoV is the need to use bulky free-form optics. The gratings are typically Bragg
critical, as it defines the perceived size of the virtual object generated gratings recorded in holographic media or Surface Relief Gratings—
by the AR glasses. A typical value for heads-on AR displays is around SRGs. The technology of holographic Bragg gratings is very mature
but this solution only offers low refractive index contrast. This intrinsi-
60 (diagonally)444 while, for reference, the human eye’s FoV is
cally leads to a high selectivity of the diffraction process in terms of
approximately 120 ;440 thus, it is desirable to extend the FoV of AR
angle and wavelength, therefore limiting the FoV of the entire sys-
glasses. However, such an extension poses real challenges for the dis-
tem.444 Despite these shortcomings, this approach is well suited for
play brightness and resolution, as the properties of the image are deter-
applications that do not require large FoV (for example, displaying
mined by the luminous source. If the FoV increases, the luminous
notifications or giving instructions for navigation, for automotive
energy must be distributed over a larger range of solid angles, so the
luminous energy per solid angle will suffer. Similarly, for a larger FoV,

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the resolution decreases, as there is only a fixed number of pixels avail-
able. A large FoV also has an impact on the eyebox, which describes
the geometrical region of eye positions that contribute to image forma-
tion without vignetting. AR glasses must have a large eyebox to ensure
tolerance to eye movements and to accommodate different users. The
size of the eyebox is measured in mm in the x and y directions in the
plane coinciding with the plane of the eye hole, where a minimum of
6 mm is required to accommodate inter-pupil distance variations of
95% of the human population. High-performance displays achieve
>10 mm in both directions. The product of the FoV and the eyebox is
comparable to the etendue of an optical system, as it represents the
product of an area and an angle; this product is fixed by the image pro-
jector. For a given projector, an increase in the FoV directly results in a
decrease in the eyebox size. As discussed further below, this conserva-
tion of etendue can be overcome by the method of “pupil replica-
tion”—which replicates the image source over the surface of the
optical combiner, which is why the waveguide approach is so attrac-
tive. Finally, images must be created with good color and brightness
uniformity, irrespective of FoV and eyebox, so this requirement cannot
be traded off.

2. System architectures and technological platforms

Freeform Optics—The simplest way to deliver light from a projec-
tor to the eye is to reflect the projector signal toward the eye by a suit- FIG. 17. (a) Side view of a waveguide combiner consisting of three elements, i.e.,
ably shaped, partially reflective mirror, as shown in Fig. 16(a). This to in-couple, spread, and out-couple the image rays. The inset shows an example
approach has the advantage of requiring minimal image pre- of a Surface Relief Grating (Reproduced with permission from Levola and
processing and results in a relatively simple system architecture while Laakkonen, Opt. Express 15, 2067 (2007). Copyright 2007 OSA Publishing).445 (b)
Top view of a waveguide combiner with two grating elements. The inset shows the
delivering good FoV (90 ) and eyebox (>10 mm) as well as producing cross section of an advanced etched metagrating which constitutes the hybrid ele-
high-quality images. The main disadvantage of this approach is the ment of the waveguide combiner which simultaneously spreads and out-couples the
need for a bulky, inconvenient headset that imposes an unnatural look image rays, with a pitch of 300 nm.

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applications). SRGs are, in turn, fabricated by nano-structuring wave- meta-atoms instead of one.458 This is an elegant solution which, how-
guide surfaces and possess higher refractive index contrast. Therefore, ever, restricts the unit cell size for lithographic reasons, so only a low
SRGs support larger FoVs. Such gratings can now be fabricated with NA or longer wavelength operation can be achieved. Another example
high accuracy and high manufacturing yield because of advances in is the control of aberrations, where in particular, designed phase profiles
nanofabrication, including the use of nanoimprint lithography [see have been used to demonstrate a very large FoV,459 but only for a single
Fig. 17(a)].445 This classical three-element grating scheme was pio- wavelength.
neered by Nokia440 and then adopted by other companies, including When it comes to AR applications, metalenses face the same chal-
Microsoft, Magic Leap, Vuzix, and others. A more advanced version of lenge as standard freeform optical elements in terms of balancing a suf-
the waveguide combiner scheme (e.g., that introduced by WaveOptics ficiently large FoV (>60 ) with a wide enough eyebox (>10 mm),
uses two-dimensional SRGs to combine the expander and the out- while possessing a small form-factor for the convenience of the user.
coupler elements in one hybrid unit). In this configuration, a larger However, the main limitation is that due to the design and
area of the combiner is available for the outcoupling, resulting in an manufacturing challenges we mention above, modern metalenses are
increased eyebox of >10 mm in both directions. Realizing these advan- yet to become suitable for image-forming optical systems. As a result,
tages is, however, a challenging task. The grating must not only have many metalenses are designed for security camera operations that do
minimal dependence of the diffraction efficiency on the wavelength not require multiple colors and that work best in the near-infrared.
and incident angle, but also balance the contributions from the image Holographic Metasurfaces—In the scheme shown in Fig. 16(d),
rays that are incident from different directions, as specific optical rays the microdisplay projector is replaced by a simple laser or an LED.
can reach a given extraction point via multiple routes and not just This choice shifts the physical location of the digital information from
through a single geometrical path as in the classical configuration, see the image projector to the optical combiner, which is much simpler,
Fig. 17(b). In this way, the chromatic and angular aberrations can be but restricts the system to fixed images stored in the hologram.35,460
minimized to produce a uniform virtual image. These requirements While some degree of image multiplexing is possible, the number of
can only be met with the introduction of further degrees of freedom, independent images that can be stored in the combiner is then rather
which has led to the development of 3D metagratings—true nano- limited. A solution would be the deployment of dynamically tuned
photonics objects sculpted into complex 3D shapes.446 Each element of metasurfaces to create AR glasses capable of displaying dynamic
such a 3D metagrating acts as a sub-wavelength antenna. The full images. Such a dynamic holographic display could be achieved using a
response of the grating is then defined by the convolution of the inter- variety of material platforms and actuation mechanisms, as discussed
in Sec. IX C.

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ference pattern of the entire grating with the radiation profile of each
grating element.447 While traditional SRGs are patterned at scales
greater than the wavelength, these advanced metagratings require a C. Future perspectives
lithography resolution below 50 nm and high-precision alignment. Waveguides and Metalenses—Metalenses and metagratings used in
Metalenses—Metalenses utilize subwavelength structures to manip- AR optical combiners exhibit noticeable similarities in terms of control-
ulate light at the nanoscale. With their ultra-thin size, sub-wavelength ling a given wavefront and producing a desired optical response. Both
modulation scale, and ability to imprint any desired phase front onto approaches utilize engineered patterns of sub-wavelength antennas to
the incoming signal, metalenses can be used to make flat versions of tra- create a desired functionality. Likewise, both in metalenses and metagrat-
ditional lenses448 reducing the size, complexity, and cost of the optical ings, the complexity of the meta-atom design is now surpassing initial
system.449,450 Remarkably, metalenses can also be engineered to respond simplistic designs by shaping or substructuring the meta-atoms. By
differently to light with specific polarization, wavelength, or angle of exploiting all the degrees of freedom of metaoptics design, it is now possi-
incidence.451,452 This flexibility makes them very attractive for AR appli- ble to improve the brightness and color uniformity of AR systems.
cations.453–455 In the example of Fig. 16(c), metalenses are used in the While the design complexity of the meta-atoms and the
Maxwellian configuration, whereby the image is focused on the pupil manufacturing of metalenses and metagratings have already merged,
and the virtual image is always in focus, independent of the accommo- these two approaches employ fundamentally different architectures.
dation of the eye lens.456 This approach offers advantages in terms of Given the advanced technology readiness level reached by the
FoV. However, the eyebox for the Maxwellian configuration is very waveguide-style combiner, it is anticipated that waveguide combiners
small.444 While metalenses offer superior control over the wavefront of will be the choice for the next few generations of commercially avail-
the transmitted light, they are characterized by intrinsic tradeoffs.457 The able AR systems. The main advantage that motivates this choice is that
main trade-off is the fact that a typical metalens design strongly depends the waveguide architecture addresses the issue of the FoV—eyebox
on the wavelength. The choice of thin film thickness, meta-atom size trade-off, through the pupil replica mechanism. Importantly, from an
and unit cell, as well as the use of Fresnel zones to accommodate multi- engineering point of view, in metagratings, it is also possible to manage
ple 2p phase shifts, are all wavelength-dependent. Moreover, the unit the extraction efficiency and thus maximize the extracted energy along
cell size depends on the numerical aperture (NA) according to the the propagation path of the image rays. The main challenge for
Nyquist criterion as a <k/(2 NA), which means that the higher NA waveguide-based combiners remains to achieve good color and bright-
required for AR systems to achieve reasonably large FoV also demands ness uniformity. These parameters are still limited by chromatic and
a smaller unit cell size. This quickly becomes very challenging in terms angular aberrations. Regardless of the coupling mechanism, it is
of lithographic requirements, especially for operation in the visible. All extremely challenging to in-couple and out-couple all the image rays
these requirements trade-off against each other; for example, the wave- with the same efficiency, independently of their wavelength and inci-
length dependence can be addressed by controlling the dispersion in dent angle. To this end, the shape of the 3D meta-atoms will require
each meta-atom by substructuring the unit cell and using two further optimization. Importantly, this development will need to

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include consideration of the manufacturing at the scale of the meta- and their shape.470,471 Future solutions would deploy active tuning
gratings, e.g., using nano-imprinting technologies and using materials mechanisms. The most promising solutions include the incorporation
with a sufficiently high index of refraction. Current efforts in this direc- of liquid crystal cells coupled to metasurfaces filters,472,473 metasurfaces
tion tend to fabricate gratings with a refractive index greater than 2.5 based on phase change materials474,475 and variants of transparent
by imprinting patterns into polymers and using them as an etching conductive oxide modulators.476,477 Ideally, the holographic metasurfa-
mask.461 This approach can employ a wide range of conventional opti- ces should be tuned electrically, at the level of the single meta-atom,
cal materials but possesses the challenge of accurately translating com- over a sufficiently wide modulation range, and reversibly over a mean-
plex metagrating shapes into dielectric materials through a single-step ingful number of cycles, cycle number still being an issue with phase
etch process [see, e.g., Fig. 17(b)]. Alternative approaches include change materials. Despite the fast and meaningful progress,478 at the
imprinting into a polymeric matrix with added nanoparticles, which time of writing this article, it is not clear which, if any, of these
have been used to create 3D nano-structures with a refractive index approaches will yield the magnitude in change of the optical response
greater than 2462,463 avoiding the etching step. required by AR applications, with low dispersion and low loss. If this
While waveguide combiners will likely remain the standard important issue could be solved, however, such glasses would be light-
approach, they will improve on their limitations by incorporating weight with a form factor barely different from modern spectacles.
some of the benefits of metalenses. Next-generation combiners will Their frame would be thin yet contain all the electronics and the light
likely exploit the polarization-dependent response of meta-atoms, source. The degree of freedom available in the design would also
implement pupil replica schemes, be achromatic, and offer a high level enable the implementation of pupil replica strategies, thus surpassing
of sophistication of response. In the process, they will also tackle other the etendue constraints. By scanning a laser over various areas of a
key issues like the unwanted scattering of external light, known as the holographic metasurface and dynamically altering the optical response
“rainbow effect,” and the outcoupling of the digital image away from of specific meta-atoms, it becomes possible to generate wavefronts in
the user’s eyes, referred to as “glowing eye.” This will be achieved by any desired shape and direction. This approach could realize the goal
designing metagratings that have an asymmetric optical response of consumer-grade AR glasses that seamlessly integrate digital and
depending on the direction of the incident light. real-world visuals.
While the intrinsic limitations of metalenses make it harder to see To conclude, there have been major developments in AR systems
them prevailing as combiners in AR glasses, we see potential in their over the last few years. Traditional methods have evolved to incorpo-
use as AR technology integrated with LiDAR and Time-of-Flight sen- rate more sophisticated strategies to manage the delivery of light to the
sors, and as optics for facile recognition applications.464 These applica-

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eye, incorporating nanopatterned optical interfaces. In their evolution,
tions have much less stringent achromatic requirements, as they solely these systems have crossed paths and aligned with the progress made
need to operate at a predetermined wavelength and exclusively within in the various areas of meta-optics, which is indeed one of the most
the near-infrared (NIR) spectrum. This has the additional benefit of versatile nanophotonic platforms available to optical engineers. Here,
enabling the use of silicon technology, such as nanolithography, which we have discussed both the differences and the similarities between the
is readily compatible with scaled-up manufacturing processes with different platforms and practical solutions. While some considerations
high precision in extra small feature size.465,466 are unavoidably speculative, and AR systems of the future may look
Freeform combiners with metasurfaces—Another possible direc- very different from current implementations, meta-optics has already
tion in the development of metasurfaces for AR glasses is their use to carved a place for itself in this future.
enhance freeform optical elements.467 This type of hybrid freefrom-
meta optics uses both the controlled phase response typical of metama- X. METASURFACES FOR QUANTUM STATES
GENERATION
terials and the geometry of the freeform elements to fix both the image
quality and the aberrations. Patterning curved substrates is challenging,
s Santiago-Cruz, Igal Brener,
Sylvain D. Gennaro, Toma
but recent results have shown that this is a practically viable solu-
tion.467 Alternative approaches include the use of conformable meta- and Maria V. Chekhova
surfaces, which have the advantage of decoupling the fabrication
[Link]@[Link]
constraints from the shape of the substrate to which they are
applied.468,469 This manufacturing approach could also be used to cre-
ate curved waveguide combiners to mimic curved lenses used in most A. Introduction
modern spectacles by first manufacturing diffraction gratings on a In the early 20th century, the understanding of light underwent a
transparent flexible film and then transferring this film onto a curved significant transformation through the discovery of the photoelectric
waveguide combiner. This type of combiner would be less bulky than effect and the development of quantum theory.479 Pioneering physi-
conventional freeform combiners and have a more natural look, how- cists of the time postulated the existence of quanta of light called pho-
ever, still be constrained by the conservation of the etendue. It is, there- tons—a term coined by the American physicist Gilbert N. Lewis in
fore, more likely that freeform optics enhanced by metasurfaces will 1926 from the Greek word “ph os,” meaning “light.”480 However, it was
find better use in the image projector, working on a broadband range not until the 1970s that physicists learned to generate single photons
with a wide field of view. and even more fascinating states—pairs of such photons that behave
Holographic metasurfaces—Finally, we would like to imagine ulti- as a single quantum object, and exhibit entanglement. Subsequent
mate AR glasses based on holographic metamaterials. Current solu- advancements enriched the toolbox of quantum optics with other
tions only offer static images, at best multiplexed in the same device, quantum states of light, such as squeezed states, Schr€
odinger cat states,
using e.g., polarization, wavelength, the direction of the incoming light, cluster states, and many others, whose description in terms of classical

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electromagnetic theory leads to paradoxes. These quantum states of of states in its environment. As demonstrated by Purcell in 1946,
light are now pivotal instruments for quantum photonic technologies, the spontaneous emission rate in an optical cavity is proportional
including quantum information processing, communication, metrol- to the ratio between the quality (Q) factor of the cavity and the
ogy, sensing, and imaging.481 optical mode volume.540 Consequently, optical resonances with
Over the years, scientists have developed a plethora of single- high quality factors and/or small optical mode volumes are sought
photon sources482 using atoms,483,484 trapped ions,485 single molecules after for this purpose. From a quantum optical perspective, effects
in solids,486 epitaxially grown487 and colloidal488 quantum dots, carbon of spontaneous emission—such as single-photon emission by
nanotubes,489 color centers in diamond,490 and defects in two- atoms or solid-state emitters, and the generation of photon pairs
dimensional materials.491 The most convenient sources of entangled through SPDC and SFWM—can be elucidated as being stimulated
photons are created using nonlinear optical effects: spontaneous by the vacuum field. Despite the vacuum field having an average
parametric downconversion (SPDC) in second-order nonlinear crys- value of zero, it exhibits non-zero fluctuations around this mean.
tals492–497 and spontaneous four-wave mixing (SFWM) in fibers.498,499 The spectral density of these fluctuations is uniform across all
SPDC and SFWM can also produce single photons if one photon of a states in the k-space and is equal to one photon per state (per
pair is used to herald the presence of the other photon. However, the mode).479 A resonance augments the density of states for the reso-
most significant application of these nonlinear effects is to generate nant mode. Given the uniform population of states due to quantum
and engineer entanglement between the two photons, whether in vacuum fluctuations, the resonance intensifies the spectral bright-
polarization or continuous variables, such as time/frequency and posi- ness of these fluctuations at its wavelength and for the correspond-
tion/momentum. With stronger pumping, both SPDC and SFWM ing orientation of the optical field. This explains the enhancement
produce higher fluxes of photon pairs, forming different kinds of of all spontaneous emission effects for resonant modes of optical
squeezed vacuum states. Being brighter than single- or few-photon metasurfaces.
states, squeezed vacuum and other squeezed states are especially useful Similar enhancement of emission can be obtained using plas-
for quantum measurement and sensing. monic nanoantennas and metasurfaces. Plasmonic metasurfaces
In recent years, optical metasurfaces have been developed to harness the power of surface plasmons—collective electron oscil-
manipulate and control the amplitude, phase, and polarization of lations at interfaces between metals and dielectrics—to amplify
light.1,13,500–502 The latter manipulation combined with enhanced effi- single-photon emission. By tailoring light–matter interactions
ciencies due to engineered resonances has been used to promote the within nanoscale mode volumes, these structures improve the
classical process of harmonic generation at the nanoscale.53,130,135,503–519

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efficiency of QEs. For instance, plasmonic metasurfaces were
More recently, metasurfaces have evolved into platforms for the genera- shown to enhance the spontaneous emission rate of embedded
tion and manipulation of quantum light. Thanks to their flexibility in InAs quantum dots, as illustrated in Fig. 18(a).523 The quantum
engineering high-quality optical resonances, metasurfaces can control dot entered a superlinear photoluminescence regime, which was
and amplify various forms of spontaneous emission—from the emission attributed to the excitation of surface plasmon polaritons (SPPs)
of single photons by solid-state emitters58,100,395,489,520–525 to the genera- and the subsequent room-temperature generation of hot elec-
tion of photon pairs through nonlinear optical effects.137,384,526–529 In trons. Plasmonic metasurfaces can also enhance the spontaneous
addition to their compact nature, metasurfaces are multifunctional, emission of isolated defects in 2D materials, such as hexagonal
capable of combining the generation of quantum light with tasks like boron nitride (hBN), that are known to emit single photons at
sorting,530 filtering,531 polarization transformation,532,533 sensing,534 and room temperature. For instance, Fig. 18(b) depicts a metasurface
engineering photon entanglement.535,536 Metasurfaces thus present a composed of gold nanoparticle arrays that support localized sur-
promising avenue to generate and control complex quantum states of face plasmon resonances. The strong confinement of the electric
light at the nanoscale. In this short perspective, we direct our focus field near the nanoparticle surface intensifies the spontaneous
toward the unique abilities of optical metasurfaces at enhancing the emission, aligning with the Purcell enhancement in the weak cou-
emission of single photons or photon pairs through the engineering of pling regime.521
optical resonances. Plasmonic metasurfaces, while offering remarkable opportunities
for enhancing single-photon generation through their ability to con-
B. Single-photon generation centrate light in small volumes, face limitations in achieving high-Q
One of the fundamental building blocks of optical quantum resonances. These limitations arise due to the inherent Ohmic loss of
technologies consists of single-photon sources. A prominent chal- plasmonic materials. Researchers are thus actively exploring alternative
lenge in this field is thus the search for single-photon sources that high refractive index dielectric materials to achieve higher Q-factors.
emit indistinguishable photons with well-defined polarization, All-dielectric metasurfaces offer a promising route to enhance single-
high purity, and high emission rates. Many traditional quantum photon generation at visible and near infrared wavelengths through
emitters (QEs) typically face issues such as low quantum yields and the excitation of Mie-type resonances and high-Q bound states in the
emission rates, a broad emission spectrum, and omnidirectional continuum (BIC). For instance, as depicted in Fig. 18(c), an early
emission.525 experimental demonstration shows an all-dielectric metasurface, made
Recently, metasurfaces have facilitated the enhancement of of arrays of high-index nanoresonators supporting magnetic dipole
spontaneous emission rates,58,100,395,489,520–525 beam steer- modes, modifying the single-photon emission of oxygen-doped single-
ing,48,88,537,538 and polarization control of emitters370,539 using walled carbon nanotubes (SWCNTs), by a moderate factor of
optical resonances. According to the Fermi golden rule, the emis- 0:8 4:0. Moreover, single-dopant polarization experiments show an
sion rate of a QE increases with the local electromagnetic density anomalous photoluminescence polarization rotation due to coupling

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FIG. 18. Single-photon generation in metasurfaces. (a) Super-linear photoluminescence dynamics in SPP- quantum-dot coupling systems in a plasmonic metasurface.523 (b)
Deterministic coupling of quantum emitters in 2D materials to plasmonic nanocavity arrays.521 (c) Solitary oxygen dopant emission from carbon nanotubes modified by dielectric
metasurfaces.489 (d) Mie-resonant GaAs nanocylinders incorporating five layers of InAs quantum dots.100 (e) and (f) All-dielectric metasurface exhibiting quasi-BICs due to (e)
lattice deformation (Si)58 or (f) resonator deformation (GaAs).522 On-chip single-photon sources coupled to (g) concentric dielectric rings539 or (h) anisotropic nanobricks541
enabling linear polarization and OAM control. (i) Dielectric bifocal metalens enabling the emission of single photons along one of the two different directions depending on their
polarization.542 (a) Reprinted with permission from Iwanaga et al., ACS Photonics 5, 897 (2018).523 Copyright 2018 American Chemical Society. (b) Reprinted with permission
from Tran et al., Nano Lett. 17, 2634 (2017).521 Copyright 2017 American Chemical Society. (c) Reprinted with permission from Ma et al., ACS Nano 11, 6431 (2017).
Copyright 2017 American Chemical Society.489 (d) Reprinted with permission from Vaskin et al., Opt. Express 29, 5567 (2021).Copyright The Optical Society.100 (e) Reprinted
with permission from Yuan et al., ACS Nano 11, 10704 (2017). Copyright 2017 American Chemical Society.58 (f) Reprinted with permission from Liu et al., ACS Photonics 5,
1365 (2018). Copyright 2018 American Chemical Society. (g) Reprinted with permission from Kan et al., Adv. Mater. 32, 1907832 (2020). Copyright 2020 Authors, licensed
under a Creative Commons Attribution Noncommercial License4.0 (CC BY-NC).539 (h) Reprinted with permission from Purcell, Proc. Am. Phys. Soc. 69, 674 (1946). Copyright
1946 Authors, Creative Commons Attribution Noncommercial License4.0 (CC BY-NC).540 (i) Reprinted with permission from Bao et al., Sci. Adv. 6, 8761 (2020). Copyright
2020 Authors, Creative Commons Attribution Noncommercial License4.0 (CC BY-NC).542

individual SWCNTs to silicon nanoresonators, showcasing the exciting an unstructured surface. This improvement in the spontaneous emis-
potential of dielectric metasurfaces to control the polarization of sion rate aligns with expectations, given the diminished Q factors asso-
QEs.488 ciated with the resonances involved.
Using optical modes with higher Q-factors, single-photon genera- All-dielectric metasurfaces can capitalize on high-Q optical reso-
tion can be further enhanced. For instance, consider a metasurface nances such as symmetry-protected quasi-BICs.506–508 BICs are
composed of Mie-resonant GaAs nanocylinders embedding five layers discrete-energy modes that do not radiate and possess energy levels
of InAs quantum dots [Fig. 18(d)100]. Although the primary objective that coincide with a continuous spectrum of radiating modes.141
of this study was to modify the photoluminescence polarization and Leveraging their high-Q resonances can lead to increased spontaneous
directionality through the outcoupling of quantum dots emission to emission. For instance, as depicted in Fig. 18(e), a 1000-fold enhance-
the magnetic quadrupolar modes, the authors also observed a note- ment of photoluminescence was observed for four layers of self-
worthy 19-fold enhancement in the emission rate when compared to assembled Ge quantum dots (QDs) embedded within a metasurface

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composed of a periodic lattice of asymmetric air holes in a silicon-on- In contrast to bulk crystals, SPDC at the nanoscale relaxes the
insulator (SOI) slab. This metasurface exhibited quasi-BICs with a Q- requirement for longitudinal momentum conservation,543 resulting in a
factor of approximately 1000.58 broad range of frequencies and angles for emitted photon pairs. For
Similarly, a metasurface employing broken-symmetry GaAs reso- instance, the broad frequency-angular spectrum of SPDC in ultrathin
nators, arranged in a square lattice, showcased a several-hundred-fold nonlinear films [Fig. 19(a)]543 leads to a heightened degree of frequency
enhancement in the photoluminescence of monolithically embedded, and angular entanglement, along with short correlation times and sub-
self-assembled, near-infrared InAs/InGaAs QDs [Fig. 18(f)]. Notably, wavelength correlation distances.116 Moreover, the relaxation of momen-
the symmetry protected quasi-BICs reshaped the emission of the QDs, tum conservation offers the potential for tunable polarization
making it unidirectional along the normal to the metasurface.522 entanglement,544 thereby expanding the possibilities for quantum state
Optical metasurfaces can go beyond the mere enhancement of engineering. However, in optical antennas and metasurfaces, resonances
spontaneous emission and tailor its polarization and orbital angular serve to select the wavelengths, directions, and polarizations of enhanced
momentum properties. Examples are metasurfaces designed in the photon emission. Through meticulous selection and design of optical
configuration of a bullseye target through concentric dielectric rings modes and resonances, the generation of entangled photons with
[Fig. 18(g)]539 or anisotropic nanobricks [Fig. 18(h)],541 allowing the improved efficiency can be achieved with control over their emission
emission of single photons with controllable polarization. Consider direction and creation of intricate quantum states.116,137,384,527–529
a nitrogen-vacancy (NV) center at the center of concentric dielec- Observing SPDC at the nanoscale presents challenges. SPDC is
tric nanoridges positioned above a silver film, as shown in inherently a weak parametric process, and experiments with nanopho-
Fig. 18(g). This arrangement emits single photons with well- tonic samples require prolonged data acquisition to detect a signal. To
defined circular polarization (chirality >0.8) and remarkable direc- find suitable materials and structures, one can use classical processes
tionality (collection efficiency reaching up to 92%), a result of the such as second harmonic generation (SHG) and sum frequency gener-
tailored phase of the field scattered from the QE and the corre- ation (SFG).527 These processes share the same phase matching condi-
sponding excited surface plasmon polaritons.539 Similarly, tion and effective nonlinearity as SPDC. Alternatively, difference
Fig. 18(h) illustrates how a metasurface composed of dielectric frequency generation (DFG) can be employed within stimulated emis-
anisotropic nanobricks, enveloping a room-temperature single- sion tomography (SET) to investigate the efficiency of SPDC and the
photon emitter—germanium vacancy center (GeV-ND) positioned entanglement of biphotons.116,543,545,546
on a silica (SiO2) spacer-covered silver (Ag) substrate—excites For instance, SFG was used to predict the enhancement of SPDC

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radially diverging SPP waves. In this manner, metasurfaces can from a nonlinear plasmonic metagrating made of periodic silver nano-
confer topological charges to emitted single photons, thus enabling strips atop a thin lithium niobate (LiNbO3) film and a silver substrate.
the emission of linearly polarized vortex beams. The authors addi- Through optical excitation, localized surface and gap plasmon reso-
tionally demonstrated the realization of multiplexing single- nances were formed around the edges of the nanostrips and within the
photon emission channels with orthogonal linear polarizations nanogaps. This amplified the optical field in the nonlinear LiNbO3
carrying distinct topological charges and demonstrate their entan- layer.547 However, because plasmonic-based systems have high Ohmic
glement.541 A further application of this concept involves the con- losses, they also emit incoherent light, which would reduce the signal-
struction of a dielectric bifocal metalens atop a SiO2 and gold film, to-noise ratio of the generated biphotons.548
housing a quantum dot within the SiO2 layer [Fig. 18(i)]. The met- Compared to their plasmonic counterparts, metasurfaces crafted
alens is designed with its two foci aligned with the positions of the from materials with high second-order susceptibility, such as
quantum dot and its mirrored image. Consequently, each photon GaAs,509,510,518,549 AlGaAs,503,513,550 and other materials,512,551,552 are
can be emitted along one of the two distinct directions, depending attractive alternatives. The initial endeavor to observe SPDC created
within nanostructures was centered around a single crystalline AlGaAs
on its polarization.542
To conclude, we have surveyed some of the recent work in using nanocylinder, characterized by Mie-like resonances at both the funda-
mental and down-converted wavelengths [Fig. 19(b)].553 The histo-
metasurfaces to improve the performance of quantum emitters embed-
gram of the photon arrival time difference revealed a minor peak
ded within them, achieved through optical resonance engineering. In
above the background of accidental coincidences. However, the
addition, metasurfaces can also tailor the emission direction and polar-
peak-to-background contrast (referred to as CAR, coincidences-to-
ization. Shifting our focus, we will now turn to showcasing how non-
accidentals ratio) was insufficient to confirm the emission of SPDC
linear metasurfaces can facilitate the generation of photon pairs via
pairs. Given that thermal light can also lead to a peak at zero arrival
SPDC.
time difference,554 a signature of two-photon emission is the peak
exceeding the background (CAR > 1). Another hallmark of biphoton
C. Biphoton generation emission is the reciprocal relationship between the CAR and the pump
Quantum state engineering largely relies on SPDC492,493,496,497 power. The first demonstration of nanoscale SPDC using this
and SFWM.498,499 These processes lead to the spontaneous emission of approach emerged in the context of a nonlinear film.116 Very recently,
entangled photon pairs, known as biphotons, while adhering to princi- SPDC was achieved in a single LiNbO3 nanoresonator of height
ples of energy and momentum conservation. SPDC and SFWM serve 500 nm and diameter 1 lm, which is, perhaps, the most compact 3D
as the foundation for generating a diverse range of quantum states, source of biphotons to date.555
spanning from heralded single photons and higher-order Fock states One approach to achieve higher biphoton rates involves using
to squeezed states and multiphoton non-Gaussian states like resonances in optical metasurfaces, which enhance the vacuum field
Schr€odinger cat states or NOON states. and hence the spontaneous emission of photon pairs via SPDC. This

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FIG. 19. Photon pairs generation in optical antennas, metasurfaces, and other nanoscale structures. (a) Relaxed momentum conservation in SPDC for thin crystals (right) com-
pared to thick ones (left).543 (b) and (c) The excitation of electric and magnetic dipole resonances in (b) an AlGaAs nanoantenna553 and (c) a lithium niobate metasurface
enhances the emission of photon pairs.526 (d)–(g) Quasi-BIC optical modes drastically enhance the generation of photon pairs, predicted (d) in meta gratings made of nano-
fins,528 (e) in AlGaAs metasurfaces made of nanocylinders with two holes in them,527 measured in (f) a metasurface made of broken symmetry GaAs nanoresonators,384 and
(g) in tilted ellipses nanoresonators.529 (h) Spatially entangled signal and idler photons from a LiNbO3 nonlocal metasurface with guided-mode resonances.137 Other notable
approaches of photon pairs generations via SPDC in (i) metalens arrays combined with a BBO crystal190 and (j) LiNbO3 microcubes.557 (a) Reprinted with permission from
Okoth et al., Phys. Rev. Lett. 123, 263602 (2019). Copyright 2019 American Physical Society.543 (b) Reprinted with permission from Marino et al., Optica 6, 1416 (2019).
Copyright The Optical Society.553 (c) Reprinted with permission from Santiago-Cruz et al., Nano Lett. 21(10), 4423–4429. Copyright 2021 American Chemical Society.526 (d)
Reprinted with permission from Mazzanti et al., New J. Phys. 24, 35006 (2022). Copyright 2022 Authors, Creative Commons Attribution Noncommercial License 4.0 (CC BY-
NC).528 (e) Reprinted with permission from Parry et al., Adv. Photonics 3, 550011 (2021). Copyright 2021 Authors, Creative Commons Attribution Noncommercial License 4.0
(CC BY-NC).527 (f) Reprinted with permission from Santiago-Cruz et al., Science 377, 991 (2022).384 Copyright 2022 The American Association for the Advancement of
Science. (g) Reprinted with permission from Son et al., Nanoscale 15, 2567 (2023).Copyright 2021 Authors, Creative Commons Attribution 3.0 Unported License.529 (h)
Reprinted with permission from Zhang et al., Sci. Adv. 8, 4240 (2022). Copyright 2022 Authors, Creative Commons Attribution Noncommercial License 4.0 (CC BY-NC).137 (i)
Reprinted with permission from Aouani et al., Nat. Nanotechnol. 9, 290 (2014).190 Copyright 2014 The American Association for the Advancement of Science. (j) Reprinted with
permission from Hanh Duong et al., Opt. Mater. Express 12, 3696 (2022). Copyright 2022 The Optical Society.557

was first realized in 2021 using arrays of truncated LiNbO3 nanopyra- thickness and crystalline orientation by two orders of magnitude.
mids [Fig. 19(c)]. These arrays exhibited Mie-like electric dipole reso- Remarkably, there was no discernible indication of biphotons emitted
nances at telecom wavelengths.526 Given the high reflectivity of the in the forward direction.556 The resonances characterizing the meta-
metasurfaces at resonance wavelengths and their low reflectivity else- surface were adjustable by altering the size and period of the pyramidal
where, an amplified emission of frequency-degenerate biphotons was nanoresonators, thereby enabling the tuning of the biphoton emission
observed in the backward direction. Notably, the rate of pair genera- wavelength. However, we note that that only frequency degenerate
tion surpassed that of an unpatterned LiNbO3 film of equivalent SPDC exhibited a noticeable rate enhancement.

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The enhancement achieved in SPDC due to Mie resonances is microcubes557 [Fig. 19(j)] and GaAs nanowires,558 to amplify the
generally moderate. For more substantial enhancements in biphoton biphoton rate while retaining a certain degree of engineering flexibil-
generation rates for specific directions, optical resonances with higher ity offered by nanophotonics. In a different vein from SPDC, some
Q-factors, such as photonic quasi-BIC384,527,528 and guided-mode reso- groups are investigating SFWM in doubly resonant gold plasmonic
nances,137 come into play. Symmetry-protected BICs can prevent, via nano-antennas and metasurfaces.158,511,546
design, the outcoupling of radiation in the direction normal to the
metasurface.546 However, a symmetry-breaking perturbation of a reso- D. Future directions
nator or the metasurface lattice can convert a symmetry-protected BIC Optical metasurfaces have significantly improved the emission of
into a quasi-BIC. Quasi-BIC resonances,525 with their elevated Q- single and entangled photons, offering unprecedented control over
factors, can lead to significant enhancements of biphoton generation polarization and directionality. For single-photon emission, optical
rates compared to those obtained from traditional Mie metasurfaces. metasurfaces have enabled efficient coupling of QEs to closely located
For example, this enhancement was expected in a meta-grating config- optical resonances, resulting in substantial enhancements in emission
uration comprising (110)-cut Al0.18Ga0.82As nanofins atop a dielectric rates. Two promising directions have thus emerged in this context.58
substrate [Fig. 19(d)],528 and within an array of AlGaAs nanocylinders First, exploring anisotropic quantum metasurfaces has the potential to
with pairs of holes [Fig. 19(e)].527 Experimentally, tunable biphoton revolutionize the design of hybrid plasmon-QE coupled metasurfaces.
generation mediated by quasi-BIC has been observed in a metasurface Composed of anisotropic nano-scatterers as elements, these metasurfa-
consisting of GaAs nanoresonators arranged in a square lattice ces promise greater versatility in controlling photon properties, includ-
[Fig. 19(f)]. The shape of each nanoresonator was designed to disrupt ing polarization. This advancement could facilitate the realization of
the rotational C2 and C4 symmetries of the lattice.384 This metasurface on-chip single-photon sources with high polarization purity. Second,
facilitated not only degenerate, but also non-degenerate SPDC, with the development of tunable quantum metasurfaces presents an exciting
the photons of a single pair emitted at different wavelengths. The avenue for actively manipulating emitted photon properties, encom-
wavelength separation between the two photons reached almost passing emission rate, direction, wavefront, and polarization. Inspired
200 nm without significant efficiency loss. By coherently exciting this by dynamic optical metasurfaces used for classical light, the incorpora-
metasurface at various wavelengths, photons at multiple distinct wave- tion of phase-changing materials into metasurfaces that shape single-
lengths can be entangled via pairwise coupling, offering the potential photon emission can provide tunability through temperature variation
for generating more intricate quantum states. These methods of quan- or voltage application, thereby unlocking transformative possibilities

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tum state engineering, made feasible by the relaxation of momentum for quantum information technologies.
conservation and the exploitation of high-Q resonances, thus hold tre- Efficiency remains a critical challenge in the generation of photon
mendous appeal. pairs using quantum optical metasurfaces (QOMs). State-of-the-art
Metasurfaces can also impart distinct directionalities to SPDC. QOMs, due to their extremely thin profile, exhibit very low photon
Despite the relaxation in phase matching constraints, even within pair-generation rates: tens of Hertz at moderate pump powers.384,529
ultrathin layers, the probability of both photons being emitted back- However, practical quantum optical applications demand pair-
ward remains exceedingly low. However, metasurface resonances engi- generation rates on the order of 100 kHz, a benchmark that is still sig-
neered to exhibit enhanced reflectivity enable such backward pair nificantly distant from achieving with current QOMs. Several research
emission.526 Conversely, resonances configured for enhanced trans- directions to enhance the pair-generation rate predominantly rely on
missivity result in the forward emission of biphotons.384 By strategi- elevating the Q-factors of the optical mode at play, improving mode
cally designing a metasurface to possess high reflectivity at the overlap between pump, signal, and idler wavelengths, and involving
resonance of a quasi-BIC and high transmissivity elsewhere, bi- materials with high second-order susceptibilities, such as (110)-ori-
directional emission of photon pairs was observed529 [Fig. 19(g)]. In ented GaAs or van der Waals crystals like niobium oxide dichloride
this work, the photon at the resonant wavelength was predominantly (NbOCl2).559 In this context, polaritonic metasurfaces featuring reso-
emitted backwards, while its entangled partner was emitted forwards. nant susceptibilities present a promising avenue as well.518,560,561
The integration of quantum- and nanophotonics thus presents a Another challenge is the generation of tunable, polarization-entangled
promising avenue for generating complex photon states encompassing photon pairs, including Bell states, with recent advances in thin
more than two entangled photons. Additionally, as exemplified in films544 and optical metasurfaces,562 offering promising design
Fig. 19(h), guided-mode resonances have facilitated the creation of approaches.
spatially entangled photon pairs with a degenerate narrowband emis- SPDC is also a source of squeezed states of light. However, the
sion spectrum spanning approximately 3 nm around 1570 nm.137 This low parametric gain (G / Evð2Þ L, with E being the electric field ampli-
achievement was realized using a metasurface comprised of a silica tude of the pump, and L the length of the nonlinear medium), makes
metagrating atop a LiNbO3 film. Notably, the biphoton generation rate it rather challenging to observe light squeezing in metasurfaces. It
was amplified by over 450 times in comparison to an unpatterned might be possible to reach a parametric gain G 1, which is needed
film. for squeezing, in optical nonlinear metasurfaces using pulsed pumping.
Finally, we note other avenues for generating photon pairs at the Incidentally, the use of pulsed excitation could help to distinguish
nanoscale. These alternatives include the incorporation of a metalens— between SPDC and photoluminescence, as the latter is orders of mag-
constructed from a 10 10 array of GaN nanopillars—onto the surface nitude stronger than the former.563
of a 0.5 mm b-barium borate (BBO) crystal,190 which enables the Finally, the generation of quantum states via third-order nonlin-
generation of pairs in multiple modes as shown in Fig. 19(i). ear processes, such as SFWM and third order SPDC (TOSPDC)564 has
Additional methods encompass the utilization of LiNbO3 yet to be observed in optical metasurfaces. Importantly, the values of

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third-order susceptibility vð3Þ differ in various materials by up to four metamaterials. We note that some lasers discussed in the article do not
orders of magnitude; therefore, the freedom to choose any material strictly meet this definition because their individual units cannot
due to relaxed momentum conservation is crucial for third-order achieve lasing independently. However, the concept of those lasers can
effects. The use of strongly nonlinear materials like Si or Ge may facili- indeed be applied to arrays of coupled nanolasers. Therefore, to main-
tate the observation of new nonlinear effects such as TOSPDC. tain a broad scope and inspire potential future research, we have
included discussions of some metasurface-like, cutting-edge laser stud-
ACKNOWLEDGMENTS
ies that do not strictly conform to our definition of metasurface lasers.
I.B. and S.D.G. acknowledge support from the U.S. Nanolaser research gained traction around 1990 when it was dis-
Department of Energy, Office of Basic Energy Sciences, Division of covered that the threshold and modulation rate of lasers are influenced
Materials Sciences and Engineering. This work was performed, in by their size.565–568 First, miniaturized lasers with a smaller gain mate-
part, at the Center for Integrated Nanotechnologies, an Office of rial volume and a larger spontaneous radiation coupling factor exhibit
Science User Facility operated for the U.S. Department of Energy lower thresholds. Simultaneously, miniaturized lasers can achieve
(DOE) Office of Science. This article has been authored by an faster rates of spontaneous and stimulated emission, resulting in faster
employee of National Technology & Engineering Solutions of modulation rates. Since then, achieving miniaturized lasers with
Sandia, LLC under Contract No. DE-NA0003525 with the U.S. smaller mode volumes, lower threshold power consumption, and faster
Department of Energy (DOE). The employee owns all right, title modulation rates has been a focal point of research in the relevant field.
and interest in and to the article and is solely responsible for its Innovations such as the microdisk laser, photonic crystal defect-state
contents. The United States Government retains and the publisher, lasers, and nanowire lasers have significantly reduced the characteristic
by accepting the article for publication, acknowledges that the dimensions of lasers to the order of a vacuum wavelength.569–571 In
United States Government retains a non-exclusive, paid-up, 2009, the experimental realization of plasmonic nanolasers achieved
irrevocable, world-wide license to publish or reproduce the characteristic scales one-tenth of a vacuum wavelength, approaching
published form of this article or allow others to do so, for United the characteristic scales of electronic devices.572–575
States Government purposes. The DOE will provide public access to In recent years, novel methods of controlling optical fields have
these results of federally sponsored research in accordance with the continually been introduced into the micro and nanolaser domain, cre-
DOE Public Access Plan [Link] ating the development of metasurface lasers. These encompass plas-
doepublic-access-plan. This paper describes objective technical monic lattice lasers,576–579 topological lasers,91,113,580–616 bound-state
results and analysis. Any subjective views or opinions that might be in the continuum (BIC) lasers,617–619,624,625 non-Hermitian parity-time

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expressed in the paper do not necessarily represent the views of the symmetric lasers,624–637 supersymmetry lasers,638–640 and moire
U.S. Department of Energy or the United States Government. lasers,641–644 injecting renewed vitality into the advancement of micro
and nanolasers. In this article, we first briefly discuss the significance of
XI. METASURFACE LASERS metasurface lasers in the context of laser development, specifically
addressing why these mode control methods are introduced from a laser
Ren-Min Ma perspective. Following that, we delve into the mode engineering of indi-
vidual nanolasers. Finally, we explore the characteristics of metasurface
renminma@[Link] lasers formed by the coupling of multiple nanolasers.

A. Introduction B. Key performance parameters

The definition of metasurface lasers can be arguably derived from The key performance parameters of a laser include threshold
the conceptual framework of metamaterials. Metasurface lasers exhibit power density, lasing linewidth, external quantum efficiency, modula-
a fundamental similarity to metamaterials by employing artificial func- tion speed, power consumption, emission directionality, emission
tional “atoms” to tailor the properties of the composite matter formed power, and side mode suppression ratio, among others. These parame-
by these constituent atoms. In the realm of metasurface lasers, individ- ters are intricately linked, often imposing constraints on one another.
ual nanolasers serve as the fundamental atoms. The eigenmode of a For example, the pursuit of reduced size to achieve lower threshold
nanolaser can be deliberately shaped to synthesize the inner laser cav- power and enhanced modulation speed may inadvertently lead to a
ity field and/or emission beam in a highly controlled manner. broadening of the lasing linewidth, increased divergence angles, and
Furthermore, coordinated ensembles of nanolasers can generate a diminished output power. However, the silver lining lies in the fact
macroscopic response surpassing the capabilities of conventional that various applications necessitate the fine-tuning of specific parame-
lasers. Within the near field, manipulation of the polarization and pro- ters, making the optimization process application-dependent.
file of each nanolaser eigenmode is possible, and additional control Consequently, the performance of lasers is contingent upon the unique
over the ensemble can be achieved through coupling, relative phase, requirements of a given application context.
symmetry, and topology. This approach has the potential to provide To illustrate, industries employing lasers for precise material
unprecedented control over the macroscopic laser field, offering processing, such as cutting, welding, and marking, demand higher
diverse applications in the far field. power. In contrast, applications like data communication or consumer
The definition of metasuface lasers proposed in this article aims electronics necessitate lower output power to achieve energy efficiency.
to capture the essential characteristics of metamaterials and metasurfa- Beyond these traditional laser characteristics, the incorporation of
ces, combined with the features of lasers. We hope this definition offers novel optical field control introduces a transformative dimension to
a stimulating perspective for studying lasers from the standpoint of metasurface lasers, endowing them with features not inherent in

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conventional counterparts. This includes the attainment of higher radi- factor exceeding 2:9 1011 (Ref. 689). A cavity with an extremely large
ation field dimensions, superior single-mode characteristics, relative Q/V enables exploration of light–matter interaction in extreme condi-
phase control, and reconfigurability. tions, facilitating tests of fundamental physics. Moreover, it can be used
in nanolasing, ultrasensing, nonlinear optics, optomechanics, and
C. Eigenmode engineering in a single microscale laser quantum-optical devices.
cavity
In the domain of microscale lasers centered on individual cavities, 3. Controlling radiation field
the impetus for eigenmode engineering manifests through three pri- The advantage of nanoscale lasers lies in the minimal number of
mary objectives.645 First, the focus is on advancing laser performance modes permitted within the cavity, facilitating the targeted design of
by reducing lasing thresholds and accelerating modulation speeds. eigenmodes for controlling the near-field and far-field properties.645
Second, there is a concerted effort to generate a strong local field. Each laser mode represents a specific eigenmode of the cavity. The esti-
Finally, the goal is to control field properties of a nanolaser in near and mated number of eigenmodes (N) allowed in a cavity is given by the
far field. expression N ¼ qVPHY D E , where q denotes the density of states of
the cavity, VPHY is the physical size of the cavity, and D E is the gain
1. Enhance laser performance spectrum bandwidth. As typically D E spans a few tens of terahertz for
conventional organic dyes and semiconductor materials, only a few
The lasing threshold power can be categorized into two compo-
eigenmodes generally coincide spectrally with the gain spectrum when
nents. The first involves achieving population inversion of the gain
the laser cavity size is subwavelength scale in all three dimensions. This
material, essentially rendering the gain medium transparent. The sec-
characteristic enables precise engineering of the eigenmode in a nano-
ond requires compensation for cavity loss, ensuring the condition of
laser in a controllable manner, leading to novel inner laser cavity fields
having one real photon in the cavity mode is met. The quest for
smaller lasers has been a persistent research goal, striving for a more and/or emission beam synthesis. Various eigenmode engineering
compact size and reduced power consumption. Whispering-gallery- mechanisms have been proposed to control the optical field distribu-
mode microlasers, photonic crystal defect nanolasers, nanowire lasers, tions inside and outside nanoscale laser cavities, including parity-time
plasmonic nanolasers, bound states in the continuum nanolasers, symmetry, exceptional point, supersymmetry, topological nanocavity,
magic angle nanolasers have been invented to miniaturize lasers and among others. Optical fields exhibit rich dimensions,690 providing a
vast development space for eigenmode engineering.

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consequently lower their threshold power. In both dielectric and plas-
monic cavities, cavity loss increases as the volume decreases.646,647
Therefore, the exploration of materials with higher optical gain and D. Eigenmode engineering in arrayed lasers
the meticulous design of nanocavities with lower cavity loss are pivotal We can classify arrayed lasers into two categories: those originat-
for the advancement of nanolasers.648 In the case of a small laser cavity ing from photonic crystals and those stemming from individual nano-
with a large free spectral range, the meticulous design of the lasing res- lasers. While there is no fundamental difference between the two, the
onance wavelength becomes crucial in lowering the total cavity loss. approaches and methods employed to construct arrayed lasers differ.
This is due to the wavelength dependence of gain material loss, empha- Both strive for characteristics such as large-area single-mode lasing,
sizing the importance of aligning the resonance wavelength of the cav- higher laser field dimensions, and reconfigurability (Fig. 20), empha-
ity for optimal performance. Additionally, it is important to carefully sizing similar performance goals despite the varied methodologies.
balance the radiation rate and the cavity loss rate to ensure that micro-
scale lasers have a high external quantum efficiency.607,649 1. Large area single mode
Semiconductor lasers, valued for their compactness, efficiency,
2. Enhancing local field
and controllability, play vital roles in information technology.
The interaction between light and matter is generally a weak pro- However, achieving semiconductor lasers with single-mode operation
cess owing to the disparity in wavelength between photons and elec- over a large area presents a significant challenge. The attainment of
trons. Over the decades, artificial microstructures have been employed single-mode operation in a spacious region is essential for semiconduc-
to enlarge and manipulate the density of states of photons, thereby tor lasers to exhibit high output power and superior beam quality, cru-
enhancing light–matter interaction.645,650–662 In this context, the ratio of cial attributes for various applications such as laser processing, remote
quality factor to mode volume (Q/V) emerges as a crucial figure of sensing, and long-range free-space communications.
merit, signifying the strength of light field confinement on both spatial Achieving a semiconductor laser with a large-area single mode
and spectral scales. Various localization mechanisms, including total using photonic crystals involves two primary physical aspects. First, to
internal reflection,655,663–670 photonic bandgap,671–680 plasmonic reso- enable surface emitting, it is necessary to utilize the lattice momentum
nance,681–686 and bound states in the continuum (BICs),151,177,624,687,688 formed by the photonic crystal to scatter a portion of the guided
have been developed over the years to craft optical cavities with modes within the photonic crystal into the light cone, preferably at the
high Q/V. However, in photonics, a persistent trade-off exists between Gamma point. Second, to achieve a large-area single mode, it is essen-
confining a light field in space and in frequency due to the limitations of tial to enhance the contrast between the lasing thresholds of the funda-
the applicable finite potential well. Recent innovations of twisted lattice mental mode and higher-order modes.
nanocavities can overcome this trade-off by enabling a mode volume Photonic-crystal surface-emitting lasers: Photonic-crystal sur-
approaching to diffraction limit, accompanied by an exceptional quality face-emitting lasers (PCSELs) currently stand as the most mature

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FIG. 20. Metasurface lasers. (a) and (b) Photograph (a) and schematic of the cross-sectional structure (b) of a 3-mm-diameter photonic-crystal surface-emitting laser
(PCSEL).110 (c) and (d) Schematic (c) and SEM image (d) of a surface emitting topological bulk laser based on band-inversion induced reflection.590 (e) and (f) Schematic (e)

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and SEM image (f) of a topological vortex laser based on spin-momentum-locked edge mode.591 (g) Schematic of a supersymmetric microlaser array.640 (h) SEM image of a
hyperdimensional spin–orbit microlaser.691 (i) and (j) SEM images (i) and schematic of reconfigurable moire nanolaser array.642 Reproduced with permission from Yoshida
et al., Nature 618, 727 (2023). Copyright 2023 Springer Nature. Reproduced with permission from Shao et al., Nat. Nanotechnol. 15, 67 (2020). Copyright 2020 Springer
Nature. Reproduced with permission from Yang et al., Phys. Rev. Lett. 125, 13903 (2020). Copyright 2020 American Physical Society. Reproduced with permission from Qiao
et al., Science 372, 403 (2021). Copyright 2021 AAAS. Reproduced with permission from Luan et al., Nature 624, 282 (2023). Copyright 2023 Springer Nature. Reproduced
with permission from Zhang et al. Nature 612, 246 (2022). Copyright 2022 Springer Nature and Copyright Remains with the respective publishers.

system for realizing semiconductor lasers with single-mode operation. around plasmon nanocavities leads to nanoscale exciton-plasmon cou-
PCSELs achieve single-mode oscillation across expansive areas pling and mixed photon modes.
through careful tailoring of the photonic crystal’s unit cell design. Topological surface-emitting lasers: In recent years, significant
Recent research outcomes showcase the capability of PCSELs to progress has been achieved in the field of topological lasers, with the
achieve 50 W continuous-wave operation in a single mode, even in integration of a novel degree of freedom linked to band topology in pho-
areas with diameters exceeding 3 mm.110 Notably, these lasers boast a tonic crystals. This integration holds the promise of providing topologi-
very narrow beam divergence angle of 0.05 and an impressive bright- cal protection characteristics and introducing innovative optical
ness of 1 GW cm–2 sr–1. feedback mechanisms for laser cavity design. Such advancements prove
Plasmonic surface lattice nanolasers: Plasmonic surface lattice particularly beneficial for driving the development of surface emitting
nanolasers leverage collective coupling among metal nanoparticles in a semiconductor lasers with large-area single-mode. Effective mechanisms
lattice to establish the resonance mode for lasing.76 This coupling in this context include topological bulk modes, topological insulator
involves the localized surface plasmon mode and lattice-defined dif- edge modes, topological vortex defect modes, and open-Dirac modes.
fraction mode, resulting in sharp Fano lines with reduced radiative Surface-emitting topological bulk lasers have been realized through
loss. The integration of dye molecules within a polymer matrix or band-inversion-induced reflection, emitting vertically with divergence
organic solvent with plasmonic nanoparticles in a surface lattice ena- angles less than 6%, despite their microscale cavity size.590
bles lasing, with the wavelength tunable by modifying the refractive The topological bulk laser achieves high-performance single-
index, nanoparticle size, interparticle spacing, or lattice geometry. mode lasing due to the exclusive operation of band-inversion-induced
Plasmonic surface lattice nanolasers can achieve a small divergence reflection around the C point, where the band inversion occurs. This
angle (<0.5 ) and provide a robust platform for mode control.578,692 topology-induced mode selection not only restricts the number of cav-
Modifying the shape or symmetry of plasmonic NP lattices allows for ity modes with efficient confinement but also enhances the quality fac-
precise control over lasing emission properties. Low-symmetry lattices tor of the mode closer to the band edge. Furthermore, an array of
exhibit polarization-dependent lasing, while multiscale plasmonic vertical-cavity surface-emitting lasers (VCSELs) has been strategically
superlattices support multiple plasmon resonances for controlled mul- arranged to form photonic crystals featuring topological insulator edge
timodal nanolasing. The spatial organization of photoactive materials modes for collective array lasing.599 Additionally, the utilization of the

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topological vortex defect mode has led to the creation of a surface- serve as a natural source, sharing the azimuthal phase factor of a vortex
emitting topological laser with a device diameter of 500 lm and a sub- beam propagating in free space and controlling the topological charge
1 divergence angle.606 In open-Dirac cavities, surface-emitting lasing of the emitted vortex beam.695
has been achieved, demonstrating that single-mode lasing can be However, constructing a robust chiral whispering gallery mode
maintained as the cavity size is scaled up.604 that circulates only in one direction has been a long-standing chal-
Supersymmetry lasers: Recently, leveraging concepts from super- lenge. Typically, at a resonant frequency, two degenerate chiral modes
symmetric quantum mechanics has led to the development of scalable travel in opposite directions, leading to potential coupling caused by
laser arrays with the distinctive features of single-mode operation. In a backscattering, bending, or defects. This coupling transforms circling
supersymmetric laser array, the linear spectrum of the superpartner is waves into standing waves, resulting in zero orbital angular momen-
meticulously constructed to mirror that of the primary array, with the tum in the emission. To overcome this challenge and directly generate
exception of the fundamental supermode. The operating principle of a vortex beam, the symmetry of whispering gallery mode lasers needs
the supersymmetric laser array is derived from the deliberate coupling to be broken.
of the main array with its dissipative superpartner, strategically reduc- In recent years, the introduction of new physics such as excep-
ing supermode competition by limiting the available lasing modes. tional points,631,632,696–698 unidirectional topological edge states,591,597
The mode matching between the supersymmetric partners guarantees and spin–orbit coupling691 has enriched the capability of laser cavity
the suppression of all except for the fundamental supermodes. This eigenmode engineering. This enables the direct use of chiral whisper-
fundamental supermode, confined solely in the main array without a ing gallery modes in a microscale laser to directly generate radiation
superpartner, exhibits the lowest threshold and is conducive to lasing fields carrying high-dimensional information.
under suitably applied pumping. The initial realization of a supersym-
metric laser array was based on a one dimensional waveguide struc- 3. Reconfigurable phased array nanolasers
ture.638,639 Subsequently, two-dimensional supersymmetry lasers were
developed, exemplified by a two dimensional five-by-five supersym- One of the ultimate objectives in nanolaser research is to develop
metric microlaser array.640 reconfigurable coherent nanolaser arrays. This advancement will
Moire lasers array: The utilization of a moire nanolaser array broaden the applications of nanolasers, encompassing areas such as
can result in extensive single-mode operation over a large area.642 The coherent computing and communication, laser displays, and LiDAR
synchronization of emission within the moire nanolaser array is con- (light detection and ranging). Recently, reconfigurable moire nanolaser
tingent upon the flatness of the band structure in momentum space. arrays with phase synchronization has been realized.642 This device is

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The use of a moire superlattice with a predetermined twisted angle based on moire-angle nanolasers, whose modes are highly localized
ensures the necessary periodicity for the formation of a flatband, within a single moire unit cell.641
thereby facilitating the scalability of the moire nanolaser array. The optical moire superlattice structure is formed by processing
However, practical limitations may arise due to nonuniformities two sets of twisted photonic crystal lattices in the same layer of a semi-
induced during the fabrication process. Enhancing the uniformity of conductor membrane. Non-local Bloch modes in the structure are
the fabricated devices, the fabrication of the moire nanolaser array coupled through moire reciprocal vectors, resulting in spatially local-
onto a SiO2 substrate eliminates any deformations that may occur ized eigenmodes in real space. In the band structure, these localized
when suspending the membrane. Through this process, more than 160 eigenmodes correspond to Moire flat bands. The wavefunction local-
nanolasers have been synchronized to achieve single-mode lasing with ized in a single moire unit is employed to construct single-cavity moire
a divergence angle of only about 3 .642 nanolasers.
When moire-angle nanolasers are arranged in an array, the local-
2. High dimensional radiation ized wave functions of individual moire-angle nanolasers form Moire
flat bands. These bands ensure the degeneracy of frequencies, enabling
The optical field is a transverse wave field with two polarization coherent emission of nanolaser arrays in arbitrary shapes. Building
degrees of freedom, which can also be transformed into two spin upon this principle, synchronized nanolaser arrays have been realized,
degrees of freedom. In addition to polarization, spatial modes provide demonstrating high spatial and spectral coherence across various dis-
a promising avenue for creating high-dimensional Hilbert spaces. In tinct patterns, including P, K, and U shapes, as well as the Chinese
1992, the orbital angular momentum degree of freedom of optical
characters “中” and “国” (“China” in Chinese). Furthermore, the
fields was discovered.693 Optical vortex beams, carrying orbital angular
introduction of spatially varying relative phases has enabled the reali-
momentum, are distinguished by a helical phase front and a phase sin-
zation of phased-array nanolasers, facilitating the manipulation of
gularity at the beam center. The number of phase front twists around
emission directions.
the axis of propagation within one wavelength determines the beam’s
topological charge. Vortex beams with different topological charges are
orthogonal, implying the potential for high-dimensional multiplexing. E. Future directions
This property has been leveraged in applications such as optical com- Navigating the current landscape of metasurface lasers and their
munication and quantum information processing. Various methods, evolving mode engineering capabilities reveals a field in continuous
including the use of spiral phase plates, metasurfaces, synthesized holo- evolution, characterized by emerging concepts and innovative
grams, plasmonic nanostructures, and photonic crystals,694 exist to approaches. Looking ahead, several promising directions stand out,
convert a normal laser beam into a vortex beam. A compact vortex guiding the trajectory of future research in this dynamic domain.
emitter can be constructed by engineering the eigenmode of a micro- In the realm of single cavity microscale lasers, the most crucial
scale laser. Chiral eigenmodes of a whispering gallery mode resonator future research direction remains miniaturization. Much like the

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miniaturization of transistors for electronic chips, miniaturizing XII. SOLUTION-DERIVED NANOFABRICATION FOR
lasers is pivotal for optoelectronic technology. Efforts should be NONLINEAR METASTRUCTURES
directed toward constructing lasers with smaller volumes, lower
power consumption, and faster speeds. This dual focus aims to €
Helena C. Weigand, Ulle-Linda Talts, Irene Occhiodori,
explore the limits of coherent light sources in various dimensions Viola V. Vogler-Neuling, and Rachel Grange
while promoting their applications in integrated photonics, super-
resolution imaging, high-resolution displays, and beyond. grange@[Link]
Simultaneously, constructing stronger local fields is a crucial
research direction, particularly for investigating light–material A. Introduction
interactions and developing coherent light sources with atomic- Miniaturization of optical components without compromis-
scale characteristics in extremely localized optical fields. Finally, ing functionality or scalability is a main challenge for deploying
further development and exploration of single nanolaser mode compact photonic solutions in current and future technologies,
control are advantageous for the advancement of nanolaser arrays.
such as telecommunication with fast data transmission, imaging
For photonic crystals or nanolaser arrays, achieving large-area
with small mobile cameras, or light sources with quantum features.
single-mode outputs to realize kilowatt-level or even higher output
Nonlinear materials used in telecommunication, lasers, and quan-
powers in semiconductor lasers remains a crucial research direction,
tum applications are typically bulk metal–oxide single crystals.699
poised to extend the current application scope of semiconductor lasers.
Those high-quality bulk crystals are neither integratable, due to
Integrating new physics concepts into the toolbox for laser cavity
limited compatibility with top-down nanofabrication methods
eigenmode engineering is another promising avenue. By leveraging
compared to typical semiconductors, nor scalable, due to the low
recent advancements in physics, researchers can enhance the capabili-
generated signals, especially in frequency conversion at small scale.
ties of metasurface lasers, potentially unlocking new possibilities for
Current material platforms rely on a top-down fabrication
high-dimensional information processing and communication.
approach with standard semiconductors (Si, InP, GaAs), which is
The realization of the reconfigurable moire nanolaser arrays high-
limited to the available wafers, crystalline orientation, and trans-
lights the potential to construct phased array nanolasers with signifi-
parency range. To access more sophisticated features such as para-
cantly enhanced information capacity and functionality. Through
metric or electro-optic effects, metal-oxides thin films, i.e., lithium
phase synchronization, nanolaser arrays can achieve large-area, high-
niobate on insulator have been commercially available for a few
power single-mode lasing. Precise adjustment of relative phases ena-

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years.700 However, they come at high wafer cost and huge con-
bles accurate control of the emission direction of the laser array.
Complete control of the intensity and phase of individual nanolasers straints to master the smart-cut technique and etching process flow
within an array will enable the customization of the outgoing wave- of a thin layer of metal-oxides to obtain the best photonic inte-
front of metasurface lasers, resulting in outputs such as holograms, grated chip performances.701
focused beams, or other desired emission patterns. Simultaneously, the The quest for a material or fabrication method to harvest their
coherence between nanolasers can be utilized for coherent computing functional response at the nanoscale that will favor energy require-
and communication. In the realm of fundamental physics research, the ments and simplify their production is still widely open. Recent advan-
extreme localization of the optical field in a twisted lattice nanocavity ces based on photonic assemblies of randomly oriented nanocrystals
provides an excellent platform for studying cavity quantum electrody- instead of bulk crystals have shown excellent tailored optical properties
namics, nonlinear optics, quantum optics, and other related in the linear regime.703 More rarely, also frequency doubling and
phenomena. electro-optic responses have been demonstrated, mainly in isolated
nanoparticles,516 individual microstructures,552 and rare-earth doped
nanoparticles for the quantum regime704—all not very well suited for
F. Summary
integration in large surface areas with fully controlled design.
In summary, the field of metasurface lasers has witnessed signifi- These limitations are key motivations for exploring bottom-up
cant progress and diversification in recent years, marked by the inte- polycrystalline nonlinear assemblies of metal-oxides for miniaturized
gration of innovative methods to control optical fields in micro and photonic components, which, in fabrication complexity, energy con-
nanolasers. Metasurface lasers, stemming from the conceptual frame- sumption, footprint, and functionalities, can compete with the perfor-
work of metamaterials, utilize individual nanolasers as artificial func- mance of bulk crystals or top-down thin films. Overcoming the
tional atoms to tailor the properties of the composite matter they form. intuitive, yet disproven, perception that nonlinear optical effects are
This approach enables unprecedented control over the macroscopic limited or even completely eradicated in random assemblies of nano-
laser field. The future of metasurface lasers presents exciting prospects crystals gives rise to puzzling questions and new functionalities that we
for groundbreaking discoveries and advancements that can further aim to address. Hence, bottom-up assembly of nonlinear materials
push the boundaries of laser technology, opening up new possibilities may potentially become the most agile technique for classical and
for applications in communication, computing, sensing, and beyond. quantum devices.
ACKNOWLEDGMENTS
This work was supported by the National Natural Science B. Nanoimprint and solution derived principles and
Foundation of China (Grant Nos. 12225402, 91950115, 11774014, advantages
and 62321004) and the New Cornerstone Science Foundation Nonlinear optical metal-oxides such as lithium niobate (LiNbO3 or
through the XPLORER PRIZE. LNO) or barium titanate (BaTiO3 or BTO) are chemically inert due to

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compatible with various substrates. Furthermore, the elastomer

molds are permeable to trapped air and solvent vapors, enabling
higher conformity to the design and lower remaining organic resi-
dues.712,713 The latter is essential for ensuring dense and uniformly
filled metal-oxide unit cells. This etchless method entails dispersing
or synthesizing the material of interest in a liquid and malleable
solvent. Nanoparticle solutions may be used, but this can result in
limited conformity to the design and increased porosity, which
reduces the quality of the effective material and causes unwanted
scattering effects. However, specific metal-oxide sol-gels optimized
for imprint lithography can overcome these limitations and
provide a flexible material platform based on chemical synthesis
protocols. Third-order nonlinear optical effects can be investigated
in metasurfaces fabricated using binary sol-gel recipes, which have
been relatively well-established for silica and titanium dioxide.712
Second-order nonlinear optical effects arise from the non-
centrosymmetric crystalline properties of ternary metal oxides.
This means the sol-gel precursors for nonlinear metal–oxide pho-
tonic devices must be tailored to incorporate two metal elements in
a defined stoichiometry. This makes the synthesis more complex
and sensitive to small environmental or composition variations.
Nevertheless, sol-gel derived non-centrosymmetric crystalline
films and assemblies have been shown to exhibit nonlinear optical
FIG. 21. Process flow of the direct soft nanoimprint lithography (SNIL). (a) The only properties for example in potassium titanyl phosphate,714 barium
step with top-down approach is to produce the master mold by EBL. (b) Stamps titanate,715,716 or lithium niobate.717,718
(daughter molds) are used to transfer the pattern from the Si master mold to the Solution deposition for crystalline materials requires the removal
PDMS daughter mold. (c) Preparation of the nonlinear material sol-gel liquid film for
of organic solvents and stabilizers by pyrolysis steps and final anneal-

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(d) imprinting and annealing to obtain the metasurface.
ing at high temperatures to enable the formation of dense crystallites
from the cross-linked xerogel matrix. Material characterization techni-
their oxide character, which prohibits chemical wet etching techniques ques, such as x-ray and Raman spectroscopy, can be used to verify the
for nanostructuring these materials.705 They possess strong nonlinear final composition after imprinting and annealing. The chemistry-
susceptibility (d33;max;LNO ¼ 34 pmV1 ; d15;max;BTO ¼ 17 pmV1 ) based approach enables adjusting the chemical composition to account
and electro-optic tensor components (r33;max;LNO ¼ 31:8 pmV1 ; for the evaporation of volatile precursors. Considerable research has
r42;max;BTO ¼ 730 pmV1 ) at around 1060 nm. been dedicated to enhancing ternary metal–oxide sol-gel formulas for
Nevertheless, nonlinear metasurfaces have been top-down creating thin film transistors or capacitors,719 and bridging this inter-
fabricated using, e.g., gallium-based focused-ion beam milling, to disciplinary research field with developing materials for nonlinear
realize nano-gratings for second-harmonic generation and electro- optics has significant potential, particularly when combined with SNIL
optically active metasurfaces.706–708 Alternatively, electron-beam nanofabrication. The advantages of the SNIL process over the top-
lithography (EBL) and physical dry etching were employed for down fabrication of quadratic nonlinear metasurfaces are the large
pillar-based metasurfaces from LNO thin films.709 Finally, nonlin- surface areas up to full wafer scale [Fig. 22(a) shows imprints over
ear thin films can serve as a substrate on which nanostructured approximately 5 mm], high-aspect-ratio more than 10 [Fig. 22(b)], the
metasurfaces from e.g., plasmonic materials have been fabri- potential to increase the dimensionality of the system to three-
cated.710,711 BTO top-down second-harmonic metasurfaces have dimensions, the ability to avoid material redeposition-caused artefacts
been achieved by pulsed-laser deposition (PLD) of polycrystalline such as slanted sidewalls [Fig. 22(b)], access to more diverse geometries
BTO thin films, EBL, and physical etching.551 These top-down and more economical processing.720 Metal-oxides such as BTO and
processes are limited in footprint, typically in the range of a few LNO also have a high refractive index in the visible to IR spectrum
hundreds of l m2 , in aspect-ratio and sidewall angles. However, and are transparent over the whole visible range down to the UV
they allow the processing of monocrystalline materials. [Fig. 22(c)], resulting in sufficient refractive index contrast for resonant
An alternative and upscalable process is soft-nanoimprint structures even with sol-gel processing. Applying SNIL for metasurfa-
lithography (SNIL) combined with solution-derived metal-oxides. ces, second-harmonic enhancing nanohole arrays,716 second-harmonic
Direct SNIL, also known as substrate conformal imprint lithogra- generating nano-gratings,721 and imprinted metalenses with a broad-
phy, is a bottom-up fabrication method that utilizes a polydime- band focus722 have been demonstrated so far.
thylsiloxane (PDMS) elastomer intermediate mold to replicate
nanostructures from a silicon master mold (Fig. 21). Applying this C. The challenges of solution-based processing of
highly scalable and cost-efficient technique to form nanostructures metasurfaces
directly from solution-derived metal oxides has shown to drasti- While the advantages of sol-gel-based fabrication can be primar-
cally reduce the embossing temperatures and pressure while being ily found in the flexibility due to the initial liquid solution, there are

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FIG. 22. SNIL metasurfaces and their properties (a) metasurface array with color responses over the whole visible spectrum (b) Overview of different achievable metaatom

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geometries with maximum aspect ratios included in brackets: (i) pillars (4), (ii) fins (16), (iii) triangles, (iv) nanoholes, (c) refractive index comparison for barium titanate for bulk,
sol-gel derived and a nanoparticle film. (d) Polarization-dependence of second-harmonic generation for a thin film (gray) and off resonance (pink) nanohole array (NhA) showing
an isotropic response. The nonlinear behavior becomes however polarization dependent at the structures optical resonance (green). (e) Two-photon microscopy image of the
second-harmonic response of an imprinted metalens with a large surface area (diameter 100 lm).

challenges regarding the material composition. Solution-based techni- space available for metasurface designs, as volume shrinkage needs
ques do not give monocrystalline material structures as opposed to to be taken into account from the initial master mold design and can
ion-slicing thin films used for, e.g., LNO thin films. The crystallization be as large as 80%.712 Annealing conditions need careful engineering,
process starts from numerous nuclei in the solution, yielding a poly- as the temperature, ramping rate, atmosphere, and pressure can be
crystalline yet very dense material structure.723 While polycrystallinity, used to optimize the density, domain size, and crystalline phase of
especially with random domain orientation, can be exploited for its the nonlinear material. For example, the electro-optic properties of
advantageous properties,724 it could also, if needed, be mitigated by BTO sol-gel were enhanced by a factor of 3 under oxygen anneal-
aligning the domains with an external (e.g., electric) field.725 However, ing.715 Keeping in mind the restrictions of high annealing tempera-
the overall effectiveness of nonlinear processes, be it SHG or electro- tures (up to 800 C), chemical compatibility, or transparency
optic modulation, will be decreased compared to a monocrystalline requirements, the choice of substrate can additionally enhance the
material.726 It is attributed not only to the polycrystallinity of the sol- formation of pure crystalline phases (e.g., by choosing lattice-
gel-based material, which might not result in fully pure crystals but matching MgO for BTO sol-gel727). Finally, the presence of solvents
also to the formation of voids during the annealing process [see or organic stabilizers in the sol-gels induces void formation and
Fig. 22(b), e.g., in the triangle]. In the context of signal modulation via poses a technical challenge for SNIL, as the imprint with the PDMS
an applied electric field, these voids decrease modulation efficiency, as mold needs to happen while the spin-coated sol-gel is still in a liquid
any voltage drop will occur over the air inclusions instead of the sol- phase. This adds significant time constraints to the process, limiting
gel material. In addition to that, scattering of light currently limits, e.g., complicated multilayer imprints with precise alignment.728
sol-gel-based waveguides, but slightly rough surface profiles do not However, considerable progress has been made to develop special-
pose a problem for imprinted metasurfaces as can be seen in some of
ized SNIL tools for imprinting volatile sol-gel solutions.713
the SEM images of Fig. 22(b). Furthermore, the crystallization results
in a decrease of the total nanostructure volume due to the restructur-
ing of the material into a crystal lattice and the evaporation of D. Roadmap towards high-performing solution-based
organic materials present in the solution. This implies, on the one metasurfaces
hand, the formation of cracks in large structures (such as thin films Overcoming the mentioned challenges will be key to the success
or waveguides), while on the other hand, it restricts the parameter of this material platform for future metasurface-based devices. There

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are several handles for optimization. One key parameter will be the E. Future directions
quality of the crystalline domains in terms of increased size and pre- 1. Exploration of other materials and processes
ferred crystalline structure. This will improve the nonlinear prop-
erties of the material and minimize void formation for reduced Soft-nanoimprint lithography relies on capillary forces, and the
scattering and smooth surfaces. Handles for these improvements infiltration works best if the solution is still liquid. Still, the density of
range from controlling the nucleation by chemical composition the final material will be less than in bulk crystals. Aging the sol-gels
engineering to optimizing the annealing conditions and sub- could be a solution to densify the materials and avoid shrinking, lead-
strates. In addition, one could use hybrid systems of sol-gel and ing to higher linear and nonlinear properties. However, the aged sol-
nanoparticles, which could serve as crystallization nuclei and gels cannot be structured with SNIL. Therefore, one should start inves-
prevent the nanostructure shrinkage. The nanoparticles could be tigating other templating methods: (i) hard nanoimprint lithography
derived from the same sol-gel in a separate process to ensure might be an option as the imprinting relies on the applied external
identical chemical composition. 729 However, applications might forces and not on the capillary forces; (ii) block copolymer self-
directly use the sol-gel shrinkage, for instance, to increase the assembled templates in which the sol-gels could be infiltrated, already
aspect ratio of the structures. The same holds for the roughness been demonstrated with titanium-dioxide sol-gels;734,735 and (iii) con-
of the surface of SNIL devices, as it also increases the surface trolled dewetting of optical glass thin films could be adapted for non-
area, which is a property commonly sought for and exploited in linear optical materials.736
sensing or electrochemical applications. The randomly distrib- Interdisciplinary collaboration between the fields of material
uted domain orientation is also a factor that one can try to miti- sciences, chemistry, and nanosciences will play a crucial role in the
gate (poling after or during the annealing) or exploit, e.g., with future not only to help the optimization of the soft-nanoimprint
respect to quasi-random phase matching.552 In addition, it offers process and the nonlinear properties of the sol-gel derived metal-
the freedom to engineer the nonlinear susceptibility components oxides but also in the development of new materials with very high
based solely on the geometrically chosen symmetries thereby nonlinear optical properties.737 Existing sol-gel recipes for other
imprinting an artificial tensor structure on an otherwise unpolar- nonlinear materials, e.g., KTP, could be further developed.714 By
ized SHG-emitting material. For example, an imprinted nanohole using more sophisticated alignment tools for soft nanoimprint
array was shown to exhibit SHG orientation at the resonance com- lithography, one could stack several metasurfaces on top of each
pared to off-resonant behavior [Fig. 22(d)].716 Specifically consid- other to compensate hereby the lower electro-optic and nonlinear

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ering the efforts of the metasurface community to overcome material intrinsic coefficients.
unfavorable tensor parameter orientations by beam steering,730
this would be an exciting approach to follow up on, as crystal- 2. Nonlinear applications with high scalability,
symmetry considerations would not restrict the freedom in design transparency ranges, robustness, and dimensionality
due to the effectively isotropic vð2Þ of the polycrystalline material.
Particular attention should be given here to the field of One clear advantage of solution-processed nanofabrication of
Pancharatnam–Berry phase-based nonlinear structures [e.g., met- nonlinear metasurfaces compared to standard top-down protocols
alenses emitting SHG as shown in Fig. 22(e)], as they are com- is the upscalability. Soft-nanoimprint lithography has been demon-
monly thought to follow specific symmetry-selection rules.53 To strated on the wafer scale and roll-to-roll fabrication.738 From an
what extent these can be influenced by unoriented but intrinsically economic viewpoint, the bare material cost of quadratic nonlinear
emitting vð2Þ -materials remains unclear. To ease the imprint pro- thin films is at least two orders of magnitude higher than that of
cess, engineering the chemical composition of sol–gels with the solution-derived materials. The only expensive part for the lat-
selected precursors or solvents that have lower vapor pressure ter is determined by what substrate wafer is required for the
would allow more time for precise alignment to enable large-scale intended device.
stacking of imprints. Further technological advancements can be Recently, metalenses have been realized on the length scales of
made in the imprint process itself. Different daughter mold materi- 10 cm in diameter with which the moon and nebulae could be
als with, e.g., hybrid PDMS stacks (hPDMS/sPDMS) or polyvinyl imaged.739,740 Nonlinear metalenses based on frequency conversion
alcohol (PVA) can be used to achieve high-aspect ratio struc- could allow access to other wavelength ranges, e.g., up to the mid-
tures.722,731 Employing degassing processes, curing in a vacuum or infrared and down to the ultraviolet wavelength ranges, thanks to their
under high pressures, or inverse application of sol-gel on the high transparency window. Metasurface sensors from these materials
PDMS could reduce residual layers and improve uniformity. could be used in harsh environments. They would be easy to clean,
Alternative imprint techniques like hard imprints from the master, increasing their reusability and decreasing waste by exploiting the
microcontact printing, capillary force-based or microfluidic-based intrinsic inertness of metal oxides. Furthermore, the inherent material
imprinting, or eventually roll-to-roll imprinting will pave the way robustness also results in a high optical damage threshold, making
for higher quality or larger-scale nonlinear photonic devices, simi- these photonic devices more sustainable and long-lasting. The second-
lar to developments in the field of photovoltaics.713,732,733 An asset harmonic generation mechanism, combined with photonic crystal
not discussed so far is also the possibility of extending this imprint design, could add to the linear responses in advanced security features.
technique to non-flat substrates like curved lens surfaces or fiber In addition to flat devices, three-dimensional metasurfaces could be
facets. Already the possibility of these applications demonstrates applied, e.g., if stacked to realize electrically tunable metalenses for fast
the resilience of this fabrication technology toward defects like switching that might be an alternative to membrane-type liquid lenses,
dust particles. which suffer from gravitational lag.741

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3. Unexplored properties and more fundamental nanostructures is relatively straightforward by using electron beam
aspects lithography (EBL). As a result, many high-quality metallic nanostruc-
tures have been proposed, fabricated, and studied. Despite numerous
We focused on the classical nonlinear and electro-optic properties
advantages allowing for near-field enhancement, metallic nanostruc-
of LNO and BTO, though both materials belong to the class of ferro-
tures suffer from Ohmic losses at optical frequencies, leading to light
electrics, which also exhibit other compelling effects such as piezoelec-
absorption. Hence, metallic nanostructures can be irreversibly dam-
tricity and pyroelectricity. Therefore, the potential of further exploring
aged under illumination by high-power lasers, which is not preferable
the functionalities of this type of compound is enormous, mostly unex-
in many applications, particularly nonlinear metasurfaces.53,747,748
plored at the nanoscale and in the polycrystalline form of those
Subsequently, a quest has taken place to employ other materials with
materials.
more intrinsic and extrinsic properties to offer more versatile degree of
Finally, spontaneous parametric downconversion, used in the
freedom to produce metasurfaces with exotic properties.510 As a result,
early sources of entangled photons for quantum cryptography from
materials’ intrinsic and extrinsic properties have been employed as a
periodically poled LNO,742 remains to be demonstrated in polycrystal-
versatile degree of freedom to produce metasurfaces with exotic prop-
line sol-gel. In doing so, the miniaturization of quantum sources may
erties. Several scenarios, such as solution-drive nanofabrication or
benefit from a new type of fabrication process that can further help the
nanofabrication on flexible metasurfaces are discussed in this road-
integration of current bulky quantum systems.
map. This section focuses on recently demonstrated approaches for
ACKNOWLEDGMENTS fabricating semiconductor metasurfaces on insulators—a task that has
been deemed challenging for decades.510
The authors acknowledge ScopeM and D-MATL X-Ray Service
Platform at ETH Zurich for providing instrumentation for
characterization, nanofabrication support from the operation team of
the Binning and Rohrer Nanotechnology Center (BRNC) and the B. Semiconductor metasurfaces and fabrication
operation team of FIRST–Center for Micro and Nanoscience at ETHZ. challenges
This work was supported by the Swiss National Science Foundation Semiconductor metasurfaces, driven by their high refractive index
SNSF (Consolidator Grant Nos. 2022 213713 and 179099), the and wide bandgap, have attracted significant attention in the photonics
European Union’s Horizon 2020 research and innovation program community recently. In addition to their loss-free nature, which distin-

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from the European Research Council under the Grant Agreement No. guishes them from metals, semiconductor metasurfaces benefit from
714837 (Chi2-nanooxides). H.C.W. acknowledges financial support exotic electronic properties and controllable crystalline structures that pro-
from the Physics Department at ETH Zurich. vide vast and new opportunities to engineer light–matter interaction.749
Therefore, semiconductors have been deemed as major building blocks
XIII. SEMICONDUCTOR METASURFACES: MATERIALS for the development of advanced optical devices such as meta-lenses,
AND NANOFABRICATION APPROACHES holograms, displays, sensors, and more.15 As a result, precise control of
the geometry of sub-unit nanoparticles via top-down nanofabrication
Mohsen Rahmani and Lei Xu approaches has gained remarkable importance. However, unlike metallic
nanostructures, regular lithographic and liftoff processes cannot be
[Link]@[Link] exploited for fabricating semiconductor metasurfaces, as discussed below.
The major categories of semiconductor metasurfaces include: (a)
A. Introduction Group IV semiconductors, such as silicon or germanium, which are
Metasurfaces consist of artificial atoms, also referred to as sub- widely explored using the complementary metal–oxide–semiconductor
units, with dimensions and separations much smaller than the light (CMOS) processes, (b) III–V compound semiconductors, like GaN,
wavelength. The light passing through the metasurfaces interacts with GaAs, or AlGaAs, renowned for their high intrinsic nonlinearity, or (c)
the material’s effective parameters, such as permeability (l) and per- recently emerging materials, such as perovskites, with strong light
mittivity (e). In other words, in addition to the lattice constant, i.e., sep- absorption, high charge-carrier mobilities and long lifetimes.750 The com-
aration, the refractive indices (n2 ¼ le) of the atoms and their mon challenge for fabricating metasurfaces out of these semiconductors
surrounding environment also play an essential role in stimulating and is the high-temperature requirements for the growth of a thin film.
controlling the light interactions with metasurfaces. Meanwhile, to Therefore, the regular liftoff process (i.e., patterning, film deposition, and
obtain strong light confinement in these atoms and enhance the optical liftoff) cannot be exploited, as photo/electro resist is vulnerable against
effects produced by the metasurfaces, fabricating metasurfaces on low- high temperatures. In addition, each category comes with its own set of
refractive-index insulators, such as glass and sapphire, has become an fabrication challenges, including but not limited to lattice mismatch
important factor in designing the geometry of metasurfaces.743 between film and substrate (particularly insulators), controlling the crys-
In the past decades, advanced nanofabrication techniques have talline orientation, or resistance against dry or wet etching, etc.,510 high-
enabled complicated assemblies of nanoscale structures that can be light a need for innovative approaches for fabricating semiconductor
employed for engineering the metasurfaces. Metals were among the metasurfaces. This section reviews the community’s effort to balance
first exploited materials for producing nanoscale particles and meta- these fabrication challenges with the inherent properties of different
surfaces,5 mainly employing the oscillation of free electrons on the semiconductor materials to advance both the fabrication techniques and
surface, so-called surface plasmons.744–746 Fabrication of metallic the applications of these versatile materials in metasurface design.

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C. Group IV semiconductor metasurfaces nanoantennas and metasurfaces, comprised of materials such as

Group IV semiconductor nanostructures and metasurfaces, espe- Gallium Arsenide (GaAs), Gallium Phosphide (GaP), Indium
cially those made of silicon and germanium, have come to the fore- Phosphide (InP), benefit from the non-centrosymmetric crystal struc-
front as viable alternatives to traditional metallic nanostructures, ture, large second-order susceptibilities,503 and fast carrier recombina-
largely motivated by their ability to mitigate the Ohmic losses preva- tion times.760 The strong second-order bulk susceptibility of III–V
lent at optical frequencies in metal materials.146,751–754 High-refractive materials would, therefore, intrinsically increase the nonlinear conver-
index materials offer a promising platform for different nanophotonics sion efficiency as compared to silicon or germanium. Furthermore,
applications in the visible and infrared regions, such as flat optics, sens- like IV semiconductors, III–V semiconductors also exhibit high refrac-
ing, computing, imaging, etc.15 They support both electric and mag- tive indices that allow the use of strong Mie resonances to amplify the
netic resonant optical modes, facilitating enhanced linear and nonlinear signals. Moreover, III–V semiconductors are pivotal in vari-
nonlinear optical effects.755 Notably, the ability to finely tune these ous advanced technological areas in optoelectronic applications due to
materials through sophisticated fabrication methods allows for the pre- their direct bandgap and high electron mobility. Therefore, the unique
cise manipulation of their optical properties, making them even more electronic and optical properties of III–V semiconductors enable supe-
promising for the aforementioned applications.15 rior performance for various applications ranging from high-efficiency
Given that germanium can be deposited with standard evapo- solar cells, light-emitting diodes, and photodetectors to quantum com-
ration techniques, Germanium nanostructures can be fabricated puting and photonic integrated circuits.
through the standard top-down techniques, involving EBL for pat- Unfortunately, the full fruition of III–V metasurfaces in photon-
terning hard masks, transferring the masks to the germanium film ics has been bottle-necked because of the absence of good-quality
via inductively coupled plasma (ICP)/reactive ion etching (RIE), dielectric-semiconductor interfaces. The main challenge is that III–V
and mask removal via dry or wet etching.146 On the other hand, sil- semiconductors, which are generally grown epitaxially, must be grown
icon films cannot be deposited through evaporation or sputtering. on a substrate with a minimal lattice mismatch to avoid defects.761
Therefore, the fabrication of silicon nanostructures often leverages Over the years, various techniques for fabricating III–V semiconductor
silicon-on-insulator (SoI) technology, which was initially devel- nanostructures and metasurfaces on insulators have been developed.
oped for electronic applications. However, SoI wafers, benefiting Recently, a solution was achieved by Cambiasso et al., who introduced
from a crystalline silicon film, have been recently employed in pho- a novel approach to circumvent the challenges associated with growing
tonics, as well. SoI enables planar waveguides that strongly confine III–V films on mismatched substrates. Instead of using conventional

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light, thanks to the high refractive index contrast between the sili- film growth, they directly fabricated GaP nanoantennas on a GaP
con core and a SiO2 substrate.756 wafer. This technique involves using EBL to create highly precise and
More recently, the use of amorphous silicon (a-Si), which can be intricate patterns on the GaP wafers. Following the EBL process, these
grown directly on any substrate by plasma-enhanced chemical vapor patterns are transferred into the wafer using ICP etching. Eventually,
deposition (PECVD), has opened up new possibilities in fabrication.757 GaP nanopillars with a height of 200 nm were created and optimized
a-Si films can then be converted to any complicated metasurfaces via for visible light applications, demonstrating enhanced SHG character-
EBL patterning followed by ICP/RIE etching.758 PECVD allows for the istics as described in Ref. 762.
growth of thin films of hydrogenated amorphous silicon under lower Pioneering a novel approach in III–V semiconductor fabrication,
temperatures compared to crystalline silicon, making it suitable for a Person et al. focused on creating GaAs nanoantennas on glass sub-
broader range of substrates, including fully transparent ones, e.g., SiO2 strates.763 Initially, they grew a thin film of GaAs on a GaAs substrate
or quartz. This method involves the decomposition of silane gas in a using molecular beam epitaxy (MBE). This was followed by an epitax-
plasma environment, where the ions and radicals facilitate the deposi- ial liftoff process, where the GaAs film was separated from its substrate
tion of silicon on the substrate. The ability to control the deposition and then transferred onto a fused silica substrate via a water-bounding
parameters, such as gas flow rates, power, and temperature, allows for procedure. Subsequently, by using RIE, the thickness of the film was
tuning the properties of the amorphous silicon layer, such as its optical reduced to the desired value, and then the nanoantennas were pat-
bandgap and conductivity. This control is crucial for tailoring the terned onto the film through EBL, followed by another RIE process.
materials to specific applications, such as absorbers, holograms, metal- This technique marks a significant step in fabricating GaAs nanostruc-
enses, and other optical components. Amorphous silicon’s flexibility in tures on transparent substrates.763 Although it was the first of its kind,
deposition and adaptability to different substrates have significantly the relatively low quality of resonators and the rough side walls
broadened its applicability in the nanophotonics field, making it an restricted its performance for nanophotonics applications, such as the
invaluable material in the fabrication of advanced semiconductor obtained field confinement for nonlinear enhancement. In the pursuit
metasurfaces.758 of efficient nonlinear optical materials, Gili et al. introduced an
AlGaAs-based monolithic platform. Their process starts with growing
D. Group III–V semiconductor metasurfaces a layered structure on a non-intentionally doped GaAs wafer through
As explained in Sec. IV (Nonlinear Optical Metasurfaces) above, MBE. This structure includes a layer of AlGaAs on the top an
nonlinear metasurfaces have great potential to revolutionize modern aluminum-rich layer for later oxidation. Following the growth, the
photonic devices, including optical signal processing, control over the sample then undergoes patterning using the EBL, and the resultant
frequency spectrum of laser light, ultrafast switching and generation of patterns are etched into the substrate using nonselective ICP-RIE.
ultrashort pulses.759 However, weak nonlinear optical responses of Subsequently, the aluminum-rich layer was oxidized to create a uni-
metasurfaces have guided the community’s attention to materials, form AlOx substrate. Such a substrate with a low refractive index plays
which naturally possess large nonlinearities. III–V semiconductor a crucial role in enabling effective optical confinement within the

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FIG. 23. (a-i) SEM image of an array of monolithic AlGaAs-on-AlOx nanoantennas. (a-ii) Schematic of a single monolithic AlGaAs-on-AlOx nanoantenna. Adapted from Ref.
504. (b-i) Steps illustration for fabricating GaAs metasurfaces, proposed by Adapted from Ref. 764. (b-ii) A side view and (b-iii) top view SEM images of the fabricated GaAs
metasurfaces. The inset gives the reflectivity spectrum of the GaAs metasurface. Liu et al., Nano Lett. 16, 5426 (2016). Copyright 2016 American Chemical Society. [(c-i)–(c-v)]
Fabrication procedure for the AlGaAs nanoresonators in a transparent media Rocio et al. Adapted from Camacho-Morales et al., Nano Lett. 16, 7191 (2016). Copyright 2016
American Chemical Society.197 (d-i) Fabrication process flow for slicing the nanowires. (d-i) SEM image of one nanowire sliced by FIB into standing disks (highlighted in blue).

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(d-ii) SEM image of the resulting single standing disk (blue) on an ITO substrate. Scale bars are 300 nm. [(d-i)–(d-iii)] Adapted with permission from Timofeeva et al., Nano Lett.
18, 3695 (2018). Copyright 2018 American Chemical Society.512

AlGaAs nanocylinders to facilitate strong nanoscale light–matter inter- standing III–V disks, by slicing nanowires with focused ion beam
actions, as shown in Fig. 23(a).504 (FIB) milling to create disk-based configurations on any substrate, as
Shortly afterward, Liu et al. demonstrated a similar approach for shown in Fig. 23(d).512 Another promising technique is to grow GaP
creating nonlinear metasurfaces composed of a square lattice of GaAs on GaAs substrate with an AlGaInP buffer layer, then bond it to a sap-
nanodisk resonators.764 These resonators were placed on a low refrac- phire substrate after depositing SiO2 layer on top of both surfaces. By
tive index AlGa oxide spacer layer, formed by selectively oxidizing removing the AlGaInP/GaAs layer with wet etching, one can obtain
high-Al content AlGaAs layers. It began with the growth of alternating GaP film on an insulator that can be used to produce high-quality
layers of AlGaAs and GaAs on a GaAs substrate via MBE. A negative nonlinear metasurfaces.152,765 Depositing GaN on sapphire by
hydrogen silsesquioxane (HSQ) mask was then applied for patterning. MOCVD is another exciting technique enabling many applications of
The shapes of the SiOx nanodisks were transferred onto the GaAs and both linear and nonlinear metasurfaces in the visible range, particularly
AlGaAs layers using ICP etching. Finally, via the selective wet oxida- meta-lenses.737 Overall, all these advances in fabricating III–V meta-
tion process, the AlGaAs layer has converted into a low refractive surfaces on a wide range of substrates open many doors to make them
index (AlxGa1-x) layer. In parallel with these studies, Camacho et al. compatible with CMOS technologies in the near future.
implemented a recipe for III–V in insulator fabrication, enabling the
production of metasurfaces on fully transparent substrates like glass or
sapphire. Their approach includes metal-organic chemical vapor depo- E. Multi-layered semiconductor metasurfaces
sition (MOCVD) growth of AlGaAs or GaAs on a thin sacrificial AlAs Stacking several metasurfaces on each other, to benefit from sev-
layer, pre-grown on a semi-insulating GaAs substrate. The process was eral functionalities simultaneously, is an important step forward for
followed by EBL patterning and RIE etching to imprint the designs realizing multi-functional end-user devices. This concept was first
onto the top and AlAs layer. Subsequently, the AlAs layer was studied in plasmonic bilayered chiral structure,766 and stacked meta-
removed by wet etching, and loosely bound nanostructures are embed- materials, so-called Stereometamaterials.767 The concept of multi-
ded in a benzocyclobutene (BCB) polymer layer that can be transferred layered semiconductor metasurfaces is a recently developing field, with
to a glass substrate. As a result, high-quality AlGaAs nanoresonators the vision of integrating multi-functions, such as linear, nonlinear, pas-
were obtained on a fully transparent matrix [see Fig. 23(c)].197 sive, and active metasurfaces, into a single, compact device.768,769 This
Furthermore, several alternative approaches were reported for fabricat- approach promises significant advancements in optical technology,
ing III–V metasurfaces on insulators. Timofeeva et al. proposed free- enabling more sophisticated and versatile functionalities.770

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FIG. 24. (a-i) A schematic of a three-layered silicon metasurface triplet lens. (a-ii)–(a-iv) Illustration of the fabrication of layered silicon metalens doublet. Adapted with permis-
sion from Zhou et al., Nano Lett. 18, 7529 (2018). Copyright 2018 American Chemical Society.771 (b) Schematic illustration of a chiral bilayer dielectric metasurface. Adapted
with permission from Tanaka et al., ACS Nano 14, 15926 (2020).773 Copyright 2020 American Chemical Society. (c) Sketch illustrating the evolution from the design of indepen-
dent 2D metasurfaces to a multi-layer stack exploiting a single-shot thin film self-rolling mechanism. Side-view (bottom left) and top-view (bottom right) SEM images of self-
rolled microtubes after the sacrificial layer removal, revealing the two nanohole array stacks in the microtube walls. Adapted with permission from Bermudez-Urena and Steiner,
ACS Photonics 6, 2198 (2019). Copyright 2019 American Chemical Society.774 (d) SEM image of the fabricated three-layer AlGaAs metasurface. Adapted from Ref. 775. (e-i)–
(e-v) Illustration of the steps for fabricating stacked AlGaAs/GaAs alternating multi-layer resonators. (e-ii) A top view image of the final pillar structures, scale bar 1 lm. (e-iii)–
(e-v) Tilted views of the finalized one, two and three AlGaAs nanodisk stacks. The scale bars are 100 nm in (e-ii)–(e-v). (e-i)–(e-v) Adapted from Ref. 778.

Recently, Zhou et al. demonstrated tightly spaced multi-layer bilayer semiconductor chiral metasurfaces.773 Figure 24(c) demon-
metasurfaces for multiwavelength focusing.771 They fabricated two a- strates another approach proposed by Bermudez-Urena and Steiner. It
Si meta-lens embedded in PDMS, separately. The two layers were involves a thin film self-rolling technique to fabricate multi-layered
bounded by heating and curing the PDMS. As a result, they demon- semiconductor metasurfaces.774 During the fabrication process, the
strated a multiwavelength metalens doublet (NA ¼ 0.42) with focusing semiconductor materials primarily used include Ge and SiO2, along
efficiencies of 38% and 52% at wavelengths of 1180 and 1680 nm, with gold, for certain steps. When the sacrificial underlayer (Ge) is
respectively [see Fig. 24(a)]. Later, the same group extended this fabri- selectively removed, these strained layers naturally roll up, either
cation technique to realize bilayer metasurfaces for multiwavelength upwards or downwards, creating a microtubular structure with multi-
holograms, multiwavelength waveplates, and polarization-insensitive layered surface walls, depending on the number of turns completed.
3D holograms.772 A similar technique, shown in Fig. 24(b), but using a This method reduces the number of steps required for creating multi-
spin-on-glass layer instead, has been proposed for the creation of layer metasurface devices.

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In 2021, Marino et al. employed a novel fabrication technique for G. Conclusions and future perspectives
a three-layer metasurface in the AlGaAs-on-insulator platform Today, semiconductor nanoscale devices are routinely used in the
designed to enhance the optical performance in applications like ultra- electronics industry. The possibility to engineer their bandgap and
fast optical switching and high harmonic generations.775 As depicted electrical conductivity has made them an ideal platform for making
in Fig. 24(d), the metasurface features three AlGaAs layers separated transistors and integrated circuits.795 Alongside this, the optoelectronic
by a low-index AlOx spacer, all resting on an AlOx optical substrate. properties of semiconductor nanomaterials, mainly based on quantum
The fabrication process involves MOCVD growth of the epitaxial mechanical effects of light on electronic materials, have also been
structure on a GaAs wafer, PECVD deposition of a SiO2 hard mask, employed to find, detect and control the light via photo-diodes, solar
EBL, Electron-Beam Physical Vapor Deposition (EBPVD) nickel cells, plasma displays, nano-lasers, etc.796 However, engineering and
deposition, liftoff, ICP-RIE etching, and selective oxidation of AlGaAs exploiting purely optical properties of semiconductor nanostructures,
layers, resulting in a deeply etched, high-efficiency metasurface. The including metasurfaces on insulators, is a relatively new field of
lower refractive index contrast between the resonator and the spacer research that has recently flourished via developing novel fabricating
layers (AlOx) reduces the energy confinement within the resonators. techniques.510 As briefly summarized in this section, despite challenges
To maximize the index contrast and field confinement, later in 2022, for growing semiconductor films, including high-temperature deposi-
Vennberg et al. proposed another approach to fabricate vertically tion and lattice mismatch, which forbid regular liftoff nanolithography,
stacked AlGaAs/GaAs nanodisk resonators with a fast and scalable many innovative techniques have been recently proposed for fabricat-
patterning method using charged sphere colloidal lithography, where ing high-quality semiconductor metasurfaces. It is worth noting that
they have under-etched the spacer layer (GaAs), as illustrated in this concept differs from fabricating quantum dots via the synthesis of
Fig. 24(e).776 sub-30-nm semiconductor nanoparticles. Quantum dots employ semi-
conductors’ optoelectronic properties, which is beyond the scope of
F. Metasurfaces made of hybrid and emerging this section.
materials Given the recent development in the fabrication techniques of
semiconductor metasurfaces, there is a promising perspective on the
Despite the recent progress in semiconductor metasurfaces, there capability to fabricate more complex and hybrid metasurfaces. As a
is still a quest to explore new materials for various applications to result, significant interest has grown in integrating metasurfaces in
address the major issues hampering the full-scale development of photonics chips and tunable metasurfaces, two areas requiring well-

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metasurface technology, such as high loss, cost-ineffective fabrication, controlled and precise nanoscale devices. Recently, the incorporation
and challenging integration.3,777–779 Some research works have dem- of metasurface principles into integrated photonics has grown rapidly.
onstrated that combining the advantages of the metal and semicon- This capability opens opportunities to control the off-chip emission of
ductor approaches can address such issues. Various types of hybrid customized free-space wavefronts and on-chip manipulation of
nanoantennas, consisting of metallic resonators embedded in semicon- light.797 Similarly, a great interest has appeared in tunable metasurfaces
ductor media or vice versa, have been proposed and realized in recent where external tools, such as mechanical force, heat, applied voltage,
years, such as hybrid metal-oxide nanostructures191 or nanopatterned etc., can be used to control the light emission, propagation direction,
plasmonic films filled with GaAs,780 metal/dielectric core-shell nano- polarization, phase, or wavelength.798–801 These developments are not
particles,781 plasmonic ring filled by concentric lithium niobate,782 sili- only enhancing the performance and efficiency of existing applications
con,148 or AlGaAs.783 The fabrication technique for hybrid for semiconductor metasurfaces but also paving the way for future
nanostructuring is generally a combination of the techniques discussed applications of nanostructures ranging from advanced imaging and
above, consisting of multiple EBL steps, requiring precise alignment of signal processing to sensing and energy harvesting, unlocking more
every subsequent mask to the previous steps. potential in nanotechnology and photonics fields.
2D materials, ranging from WS2, MoS2, MoSe2 to WSe2 with
semiconducting band gaps on the order of 1–2.5 eV, to hexagonal ACKNOWLEDGMENTS
boron nitride (h-BN) with a wideband gap of 6 eV, are recently pro- M.R. and L.X. acknowledge support from the UK Research and
posed materials for semiconductor metasurfaces, particularly in non- Innovation Future Leaders Fellowship (No. MR/T040513/1). M.R.
linear regime,784,785 Chemical vapor deposition (CVD) technique is appreciates the support of the Royal Society and the Wolfson
the most employed method that has enabled the synthesis of large area Foundation.
and uniform thickness 2D layer of metal and insulating surfaces for
the large-scale device fabrication including electronic and flexible opto- XIV. CONFORMAL AND FLEXIBLE METASURFACES:
electronic devices.786 II–VI compound semiconductors, such as ZnS or A BRIEF PERSPECTIVE
CdHgTe, with a large range of electronic energy bandgaps, have also
been considered for optoelectronic metasurfaces,787 and Cd–Te helices S. M. Kamali, E. Arbabi, and Andrei Faraon
have been proposed for chiral nonlinearity.788 More recently, perov-
skite materials with a large ability of tunability have been proposed for faraon@[Link]
reconfigurable semiconductor metasurfaces91,789–794 The optical prop-
erties of perovskite metasurfaces can be tuned by changing the compo- A. Introduction and brief history
sition of the perovskite material or the thickness of the perovskite film. Metasurfaces designed for, and fabricated on, flexible substrates
All these emerging materials are already subjects of heavy studies in enable very interesting concepts and have potential for applications in
the community of semiconductor metasurfaces. conformal optics where a thin metasurface can vastly alter the optical

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function of an optical element with a given shape,467,468,802,803 or a machines with special capabilities are needed to define the metasurface
stretchable metasurface can act as a compact tuning element in an pattern, and the utility of regular planar techniques that are widely
optical system.804–806 Nevertheless, despite the attention and advances developed and used for electronics will be very limited in fabrication of
made over the past decade, this technology has not been adopted conformal metasurfaces. The requirement of special equipment and
beyond academic and research efforts. In this Perspective, we give a methods for their fabrication severely limits the types and shapes of
short account of the history of conformal and flexible metasurfaces, structures that could be directly made as well as the shape and mate-
briefly discuss their design, fabrication, and potential applications, and rial of the target non-planar surfaces, and would thus hinder the
share our view of their opportunities and the challenges that must be development and scaling of conformal metasurfaces. To circumvent
overcome before those opportunities can be realized. these issues, the idea of transferring metasurfaces to flexible sub-
The applications of gratings fabricated on curved surfaces goes strates, that could later conform to a non-planar surface, was devel-
back more than a century where concave gratings have extensively oped.468 Using this method, flexible metasurfaces can be fabricated
been used in spectroscopes to reduce the optical aberrations and separately and later fitted to the target structure, altering its optical
improve spectral resolution.807–810 Since then, diffractive structures function to one that does not match its form, or adding totally new
patterned on non-planar surfaces have also been used to mitigate the functionalities.467 For instance, a specially designed metasurface can
chromatic aberrations of lenses811,812 or enhance the power of optical be used to make a diverging cylindrical lens work like a converging
system without compromising size and weight.813 Independently, con- spherical one,468 or metasurfaces can be added to regular eyepieces
formal RF and microwave phased array antennas814,815 and metasurfa- and turn them into visors for near eye displays.467
ces816–818 have been developed over the past many decades to fit Since many flexible substrate materials are also stretchable, trans-
certain functionalities in structures dictated by other factors such as ferring of metasurfaces to these substrates enables other lines of appli-
aerodynamics, stealth, or physical constraints of the host structure. cations utilizing this property.806,822,823 For instance, a main property
Over the past decade, the increased availability and reduced cost of of optical gratings is their period, which would change proportional to
advanced nano-fabrication and computational resources have allowed the local strain if a metasurface on a flexible material is stretched. This
for the design and fabrication of conformal metasurfaces at optical would in turn change the grating momentum and thus can be used to
length scales, see Figs. 25(a) and 25(b).821–823 As intrinsically quasi-2D tune the diffraction angle at a certain wavelength of light, or change
structures (i.e., having a third dimension much smaller than the first the color appearance at a given angle.824 The focal length of diffractive
two), metasurfaces are suited for conforming to non-planar structures and metasurface lenses can also be tuned through radial stretching
and can be directly fabricated on the target surface.802 Direct fabrication,

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[albeit with introduction of additional geometric abberations, see
however, is only possible if the target surface has small curvature (i.e., a Fig. 25(c)].822 The deformations of the substrate, such as stretching,
very large radius of curvature) and very small height variation overall (in can significantly alter the optical function of flexible metasurfaces, pro-
the tens of micrometers, maximum).802 Otherwise, pattern generation viding an opportunity to tune their functionality. Various tunable and

FIG. 25. Conformal and flexible metasurface concepts. (a) A metasurface conforming to an optical elements modifies the optical function of the element in a desired way.468 (b)
Concept of a flexible metasurface conformed to an eyeglass’s eyepiece to redirect display light from the micro-display to the eye. Similar to holographic optical elements, meta-
surfaces can implement a grating and wavefront control functions simultaneously in a single layer, allowing for the thin metasurface to both correct for the eyepiece shape and
redirect light.467 (c) Schematic illustration of a flexible tunable metasurface. Upon stretching, the focal length of the metasurface changes proportional to strain squared.822 (d)
Schematic of a stretch tunable filter, where the transmission and reflection spectra can be modified upon stretching the metasurface.825 All images are reprinted (adapted) with
permission from the respective Journal and copyright remains with the original publisher.

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stretchable metasurface lenses and gratings have been demonstrated flexible substrates, we would like to distinguish and separate them
using different metasurface platforms (see Fig. 25),806,824 in addition to for the purposes of this paper by the effective volume thickness (i.e.,
tunable filters and color tuning in metasurfaces.825–827 wavelength and subwavelength scale thickness for metasurfaces vs
It is worth noting here that fabrication of diffractive optical ele- multiple to several wavelengths for these more conventional devices),
ments (e.g., surface relief optics like blazed gratings, Fresnel lenses, and the critical dimensions of the structures involved (i.e., subwave-
diffusers, etc.) using non-rigid materials such as polymers and resins length for metasurfaces and single to multiple wavelength scales for
is relatively mature and multiple companies (Luminit, Viavi, etc.) the conventional ones). Each of these technologies have their own
have already commercialized these technologies for many years now. benefits and drawbacks and the specific choice of which one to use
While these technologies, and devices fabricated using them, are in depends on many technical and non-technical factors involved.
many aspects similar to metasurfaces fabricated on or transferred to Nevertheless, in the rest of this chapter we will focus on metasurfaces

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FIG. 26. Fabrication methods for flexible metasurfaces. (a) For non-planar surfaces with small bumps (i.e., a few tens of micrometers of height variation and slopes smaller
than a few degrees) the pattern can be directly generated on the non-planar surface using electron-beam lithography, and then transferred to the active metasurface layer using
etch or liftoff processes.802 (b) Metasurface can be patterned directly on the non-planar surface using nano-imprint lithography. The patterned layer can then be used as an
etch mask or liftoff agent to transfer the pattern to the metasurface layer material.821 (c) A pre-patterned layer can be used like a stencil shadow mask to transfer a pattern to a
flexible substrate using a directional deposition method.831 (d) The metasurface pattern can be generated using master and soft molds and a nano-imprint lithography pro-
cess.832 (e) The metasurface structure can be fabricated on a conventional rigid substrate, and then transferred to a flexible substrate using spin and cure and a sacrificial
layer.468 (f) Spin-coat and peel-off method can be used to transfer plasmonic metasurfaces fabricated on conventional rigid substrates to a flexible layer.803 All images are
reprinted (adapted) with permission from the respective Journal and copyright remains with the original publisher.

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and will not discuss these more conventional techniques and devices the case of conformal metasurfaces, each part of the metasurface
any further. should be designed around the actual local nominal incidence angle
In Sec. XIV B, we will briefly discuss the design methods, fabrica- that is generally different for separate areas.
tion techniques, and demonstrated applications of conformal and flexi- For tunable metasurfaces based on flexible substrates, it is usually
ble metasurfaces, and in the third section we will layout some the local strain of the substrate and metasurface that is used to tune the
perspectives, opportunities, and challenges facing the development and function. In these devices, the changes in the metasurface lattice caused
scaling of this field moving forward. by this strain (or the actual length scale used in the local full-wave sim-
ulations) should be taken into account. Additionally, a solid mechanics
B. Design, fabrication, and applications simulation might be required to predict the local strain of the metasur-
face, especially if the stretching force is not completely symmetric. It is
1. Optical design
also worth noting here that our focus has been consciously on optical
The optical design of conformal and flexible metasurfaces is for wavelengths, not microwave frequencies where generally the structural
the most part similar to that of planar ones on rigid substrates as in length scales of the non-planar surfaces are comparable to the wave-
most practically relevant cases the radii of curvature of the involved lengths involved, and therefore some sort of full-wave simulation or
surfaces are significantly (i.e., thousands to million times) larger more advanced approximation technique is required for the design.
than the wavelength of the light. As such, most of the techniques
used for designing planar metasurfaces can also be applied in the 2. Fabrication techniques
design of non-planar ones.468 In the simplest methods, the nano-
scatterers can mostly be treated independently from each other and Generally we can separate the fabrication methods used to make
their impact on the transmitted/reflected light can be estimated as conformal and flexible metasurfaces into three categories: (1) direct
such. Due to the large radius of curvature of the surfaces, locally we fabrication on the rigid non-planar substrate [Figs. 26(a) and 26(b)],
can assume that the nano-scatterers are arranged on a planar surface (2) fabrication done on a flexible substrate and transferred to the non-
and therefore the scattering properties estimated from simulations of planar surface if needed [Figs. 26(c) and 26(d)], and (3) fabrication
planar versions can be used. Even more complicated design and opti- done on a rigid flat substrate, transferred to a flexible medium and fit-
mization methods, that are usually based on optimizations at grating ted to the non-planar substrate [Figs. 26(e) and 26(f)]. Methods 2 and
period or Fresnel zone length scales instead of single scatterer ones, 3 can be utilized to fabricate tunable metasurfaces based on flexible
can still be applied to the conformal metasurfaces the same way.828 substrates too.

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While mostly the same, there are still considerations and In the direct fabrication method, usually the metasurface pattern
design practices that are specific to conformal and non-planar should be generated via electron beam lithography (with a depth of
metasurfaces. The most important difference is the role of the opti- focus greater than the surface height variation or an adjustable beam
cal function of the substrate on determining the desired scattering focus system), holographic pattern generation, or nano-imprint lithog-
properties of the metasurface. In the case of wavefront shaping raphy. The main challenge with this method is that the steps after the
metasurfaces, the phase imparted by the metasurface added on top pattern generation are limited to conformal processes (i.e., methods
of the wavefront transmitted/reflected by the substrate should pro- like atomic layer deposition and wet etching, as opposed to directional
duce the desired total wavefront. To be more precise and reduce methods like plasma enhanced chemical vapor deposition or deep
optical aberrations, even the role of flat substrates should be taken reactive ion etching). This limits the material, shape, and aspect ratio
into account in the design of optical metasurfaces (e.g., in the case of the nano-structures that can be fabricated by this method. For
of a lens where the incoming beam passes through the metasurface instance, this method has been used to fabricated thin plasmonic meta-
first and substrate second, and is then refracted by the boundary surfaces thorough liftoff, or low aspect-ratio low-index contrast
between the substrate and the environment). Nevertheless, the gratings.821
impact of substrate form is much larger in the case of conformal Metasurface patterns can also be generated on the flexible sub-
metasurfaces, necessitating the utilization of ray-optics or physical strate itself either via nano-imprint lithography,465,833 spin/cast and
optics to estimate the impact of the substrate in addition to the cure, or through optically or electronically sensitive resins. The flexible
full-wave simulations needed to model the metasurface locally. For substrate and whether it is compatible with high-temperature or high-
various types of non-planar surfaces like spherical and cylindrical vacuum processes could be a major limiting factor in this technique.
ones the combined functionality of the substrate and metasurface Therefore, devices fabricated with this method have mostly been lim-
(modeled as a thin phase surface) can already be simulated using ited to plasmonic metasurfaces made through liftoff831 or imprinted
commercial software packages like Zemax OpticStudio, allowing a substrates back-filled with a high-index resin.832 When nano-imprint
concurrent optimization of the two. or spin and cure patterning plus high-index filling method is used, this
Another factor to consider in the design of conformal metasurfa- technique is well-suited for high volume and low-cost roll to roll
ces is the impact of incidence and/or diffracted angle on the phase and manufacturing.
polarization of transmitted/reflected light. Generally the scattering Finally, metasurfaces can be fabricated on regular planar rigid
properties of the nano-scatterers are functions of incidence angle, and substrates (e.g., silicon or glass wafers), and then transfer printed to a
therefore it is important to take this into account for an improved flexible one like PDMS [Fig. 27(e)].822 The main advantage of this
design. For instance, in order to make a metasurface grating really method is its compatibility with most conventional planar nano-
polarization independent at non-zero incidence angles it might be nec- fabrication techniques including high temperature and high vacuum
essary to make the nano-scatterers themselves asymmetric.829,830 In deposition and etching. Thus, it is relatively versatile and can be used

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FIG. 27. Potential applications for flexible metasurfaces. (a) Image of a flexible metasurface conformed to a concave cylindrical lens, and the measured focal spot intensity of
the combined optical system.468 (b) A free-form metasurface optical element with wavefront shaping and grating deflection ability combined, fabricated on a non-planar sub-
strate.467 Metasurfaces designed and fabricated with the same mindset could be integrated on eyepieces of headmounted displays. (c) Simulated performance of a metasurface
spectral filter proposed as a mitigating solution for deuteranomaly. Original image (left), simulated image without correction (middle), and simulated image after correction (right)
are shown.803 (d) A stretchable metasurface with tunable reflection spectrum showing full spectral tuning from blue to red for both linear polarizations of light.804 (e) Focal length
tuning using a stretchable tunable metasurface singlet. The change in focal length is proportional to strain squared.822 (f) A tunable grating with enhanced first order diffraction
efficiency used to achieve color tuning. As the grating period changes when stretched, the appearing color varies with it.826 All images are reprinted (adapted) with permission
from the respective Journal and copyright remains with the original publisher.

to fabricate and transfer most types of metasurfaces. The transfer step Dielectric conformal metasurfaces have been used to alter the opti-
to the flexible substrate can be done through simple transfer printing cal function of conventional refractive optical elements [Fig. 27(a)].822
in cases where adhesion to the flexible substrate can be higher than the The phase profile of the metasurfaces were chosen to change the func-
rigid one, or using a sacrificial layer that can be dissolved away from tion of diverging and converging cylindrical lenses to converging spheri-
underneath the metasurface and release the metasurface inside the cal ones. In practice, this method can be useful when there is need for
flexible substrate.822 The main disadvantage with this method is the optical windows through transparent surfaces whose shapes are dictated
complication and number of process steps involved that could increase by factors other than optics. Similar to other metasurfaces and diffractive
the process cost and lower the total yield. optics wavefront shaping elements, chromatic aberrations limit the
bandwidth of the light that can be used. Another main challenge with
3. Applications this line of application is that it requires high accuracy alignment
between the metasurface and the target surface, which doesn’t necessar-
In a coarse division, we can categorize the applications of confor- ily have suitable alignment marks, or might require deformations in the
mal metasurfaces to modify/improve performance of a non-planar flexible substrate that cause non-uniform strain throughout.
object, or add a totally new functionality to an optical element. One As mentioned in the first section, adding gratings and diffrac-
example of the first category was wavefront shaping plasmonic reflec- tive optical elements to non-planar surfaces has had a long line of
tive metasurfaces used to compensate for phase distortions caused by applications, for instance in spectroscopes that use it to reduce aber-
height variations on a reflective surface [Fig. 25(a)].802 While called rations and improve resolution.808 More recently, the use of meta-
cloaking, the phase compensation only works over a narrow band and surfaces as the combining element on near eye display systems has
the direct fabrication method utilized limits the application to small been proposed where the metasurface would be integrated onto the
surfaces with bumps in the few micrometers, also requiring very pre- visor or eyepiece element in lieu of a holographic optical element
cise alignment between the non-planar surface and the metasurface. and work either as a pure grating or a grating with wavefront

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shaping [Fig. 27(b)].467 This is an interesting line of applications, yet Finally, conformal and tunable metasurfaces have a chromatic
cost, scalability, and worse see-through compared with volume holo- dispersion similar to other diffractive optical elements that could
graphic elements are challenges (among others) that should be over- severely limit their useful operation bandwidth, unless the dispersion is
come for it to become promising. useful for the application (like in spectrometers), or could be compen-
Apart from wavefront shaping, metasurfaces have shown other sated for (e.g., in diffractive-refractive combinations, or augmented
functionalities like spectral filtering.500 Similarly, conformal metasurfa- reality waveguides).
ces integrated on contact lenses have been used as spectral filters to A major opportunity for flexible substrates is in roll-to-roll fabri-
improve color separation for colorblind users [Figs. 27(c) and cation of metasurfaces. Whether the flexibility and conforming ability
27(d)].803 When the substrate is stretchable, the transmission/reflec- of the metasurface is critical for an application or not, nano-imprint or
tion spectra can be tuned with stretching as well, and therefore flexible cast-and-cure methods of fabricating metasurfaces can provide signifi-
metasurfaces can be used as tunable color filters. cant cost reduction over other methods that rely on lithography and
Stretching has also been used to tune grating pitch and deflection etch.
angle to steer beams822 or generate variable color structures [Figs. With the growing interest in wearable and head mounted displays
27(d) and 27(f)]826 or tune lenses and make lenses with tunable optical in recent years (and potentially over the coming decade), metasurfaces
power [Fig 27(e)].822 In both cases, the tunable range is significantly in general, and flexible metasurfaces in particular, face a great opportu-
larger than what is possible with other methods like liquid crystal inte- nity. With stringent requirements on weight, volume, and power con-
gration or electro-optic modulation, but the tuning speed is very lim- sumption, while demanding high performance optics for various parts
ited, the tuning mechanism is relatively large, and the long term of the system like cameras, eye tracking, and the display system all in a
reliability and number of cycles are very limited compared to those fashionable form factor, conformal metasurfaces pose many appealing
alternative methods. Due to these limitations, it might be more appro- properties that could make them suitable for sensor optics, holographic
priate to call these devices reconfigurable rather than tunable. elements on visors, or diffractive optics on waveguides.
In addition to wearable displays, various types of compact con-
C. Challenges, opportunities, and future perspectives sumer electronics (e.g., smart watches, wireless headphones, etc.),
Flexible and conformal metasurfaces have some similarities with
flexible electronics (mostly in fabrication processes and materials), and
therefore the vast body of knowledge developed around flexible elec-

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tronics can be (and has been) utilized here. Nevertheless, there are
both fundamental and technical differences between flexible metasur-
faces and flexible electronics (or even integrated photonics). First,
functionality and form are tightly correlated in optics, and as such the
shape of the structure and the conforming metasurface should remain
controlled and known during operation, unlike flexible electronics
where the capability to operate under various deformations is usually a
key characteristics. One exception where flexible metasurfaces might
be fine with deformations is the case of arrays of small elements (e.g., a
micro-lens array). In such cases, it is possible that the metasurface
remains functional under deformation as long as the deformation in
each element remains small. One potential application could be for a
micro-lens array integrated with a flexible OLED panel.403,834,835
On the technical side, the target substrate of a conformal meta-
surface should be well-known and well characterized, and the
conforming metasurface should be aligned with it to the regular opto-
mechanical alignment accuracy of the system. In addition, if the
conformal metasurface goes through a planar deformation or local
stretching during the alignment and fitting steps (e.g., due to a finite
Gaussian curvature of the target surface), these deformations need to
be well-controlled and understood, and their impacts need to be con-
sidered in the design and fabrication steps.
Tunable flexible metasurfaces can be very light and compact by
themselves (e.g., they can be as thin as a few tens of micrometers).
However, the mechanical system required to stretch the metasurface
can be relatively large and heavy as the stretch generally should be very
uniform and well-controlled. This necessitates close attention to the FIG. 28. Scattering of light traveling in the x direction at a (a) spatial and (b) tempo-
ral interface can be illustrated with dispersion diagrams, where the full and dashed
design and implementation of the mechanical tunable system for the
lines denote the dispersion cones for the two media. (c) An illustration of a device
benefits of low weight and volume to be realized. Reliability and cycle that combines advanced structuring of both spatial and temporal inhomogeneities to
count are other important factors that need improvement, requiring provide dynamic control over the momentum and frequency of scattered light,
the exploration and use of better flexible substrates. adapted from Ref. 48. Copyright remains with the original publisher.

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smart appliances, medical imaging systems, and many other smart and Time-varying optical metasurfaces emerge through temporal
electronic systems are becoming ubiquitous with an ever increasing modulations of the optical properties of a sub-wavelength medium,
push for integrating more sensors and machine vision cameras. If the forming an interface characterized by time-varying reflectivity and
challenges facing flexible metasurfaces are overcome or circumvented transmissivity. The scattering of light from the temporal inhomogenei-
for the relevant applications, these areas could become significant ties of such an interface inherently deviates from the temporally
growth opportunities for flexible metasurfaces, in particular if low-cost switched medium illustrated in Fig. 1(b), where propagation may lead
and scalable fabrication pipelines are developed. to complications from effects such as self-broadening.836 The control
Optical metasurfaces, in general, and flexible metasurfaces, in obtained with a temporally modulated interface mimics the approach
particular, have gone through a major cycle of attention and research employed by spatial metasurfaces, which leverage sub-wavelength
growth in the past decade. We believe over the coming years there are structuring of high-contrast inhomogeneities to efficiently manipulate
many opportunities for them to enable consumer level applications, the momentum of scattered light. Likewise, high efficiency time-
but they have to overcome the multiple barriers and challenges out- varying metasurfaces require a mechanism which acts on sub-period
lined above. timescales and provides a large modulation contrast between the time-
varying structure and its unmodulated surroundings.845 Furthermore,
XV. TIME MODULATED METASURFACES the framework of temporally structured interfaces lends itself to the
development of space-time structured devices that combine the
A. C. Harwood, S. Vezzoli, and R. Sapienza matured science of spatial metasurfaces with complex temporal modu-
lations. This envisioned device, a space-time metasurface [XXI(c)],
a.harwood22@[Link] would utilize engineered spatial and temporal inhomogeneities to pro-
vide simultaneous and dynamic control of the momentum and spec-
A. Introduction tral content of scattered light from a nanoscale component. This
Traditional, bulk optical components are ubiquitous in modern versatile device holds promise for a wide range of applications, span-
day life, providing a means to transform light into an essential techno- ning from temporal aiming and antireflection coatings to the explora-
logical tool through the use of engineered spatial inhomogeneities. tion of photonic time crystals and the development of magnet-free
This framework for light manipulation is underpinned by Noether’s nonreciprocal devices.50,846
theorem, which dictates that light scattered at a spatial interface To explore the extensive and varied research avenues concerning
between two media must conserve energy, and thus frequency, as the time-varying optical metasurfaces, the current state-of-the-art for tem-

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system is invariant in time [Fig. 28(a)]. Conversely, a system exhibiting porally engineered metasurfaces will first be reviewed in Sec. XV B.
homogeneous and instantaneous changes in its optical properties scat- This section will discuss the prevalent experimental systems that have
ters light in time through non-conservative processes. This temporal illustrated the great potential, alongside challenges that must be
scattering modifies the frequency of light while maintaining the con- resolved to be able to realize more complex temporal structures. In
servation of its momentum [Fig. 21(b)]. These novel processes of light extension to this paradigm, Secs. XV C and XV D will proceed to
scattering are known as time reflection and refraction, the temporal investigate the use of structuring in space and time simultaneously to
counterparts to the familiar, spatial reflection and refraction derived provide enhanced time-varying interactions and 4D control over scat-
from Fermat’s principle. The parallels between scattering in space and tered light, via spatially static and varying modulations. To conclude,
time can be readily visualized by using a phase diagram Figs. 21(a) and the current state of the field will be summarized, alongside the prevail-
21(b). As a consequence, the arrangement of temporal inhomogenei- ing obstacles that will determine the future of time-varying optical
ties in time-varying media serves as a mechanism through which a metasurfaces.
device may effectively manipulate the spectral content of light.836,837
Initial studies into time-varying phenomena were undertaken in B. Time-varying metasurfaces
the field of plasma physics,838 as well as systems of mechanical To identify a suitable material for a time-varying optical metasur-
waves839 and low frequency electromagnetic waves.840,841 These sys- face, one must first examine electronic state transitions that may give
tems facilitated high-efficiency time-varying experiments, as the rise to large changes in permittivity and occur over sub-picosecond
desired high-contrast modulations could be easily manipulated at fre- timescales. A familiar example of such a mechanism is the virtual-state
quencies equal to that of the propagating waves using convenient elec- transition of electrons induced by nonlinear polarizations, giving rise
tronic or mechanical driving mechanisms. On the other hand, systems to oscillating regions of permittivity. Although this modulation process
that demonstrate high-contrast, sub-period modulations in the optical meets the ideal requirement of being ultrafast, the change in permittiv-
regime rely upon Kerr-like processes, which are exclusively mediated ity induced by such processes is conventionally minimal. Alternatively,
by powerful femtosecond lasers. Consequently, the exploration of one may consider the modulation of a material’s refractive index via
time-varying photonics has been dependent upon the development of real-state transitions of electrons, for example the excitation, and sub-
ultrafast laser science and compatible material platforms for nonlinear sequent relaxation of electrons via photoexcitation. These real state
optics. Since its conception this decade, time-varying photonics has transitions are typically linked to substantial changes in permittivity;
been studied across a broad range of systems, such as 2D materials,842 however, they predominantly unfold over time periods exceeding pico-
ultracold atoms,843 and quantum wells.844 However, the discussion seconds.847 Consequently, traditional nonlinear materials do not pro-
herein will concentrate on systems that have demonstrated the vide an efficient platform for time-varying photonics. However, this
most profound capabilities and potential—time-varying optical paradigm is notably disrupted by transparent conductive oxides, a
metasurfaces. variety of epsilon-near-zero materials. Although constricted to the

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region about their near-infrared epsilon-near-zero wavelengths, the absence of any surface structure,863 advanced absorption systems
indium tin oxide and aluminum zinc oxide in particular, have been that surpass their static counterparts850 and the temporal analogue to
used to demonstrate vastly enhanced, non-perturbative nonlinear- Bragg gratings.864 In the case of transparent conductive oxides, the real-
ities,848 as well as interband and intraband transitions of electrons in ization of such temporal structures is resisted by the problem of heat
sub-picosecond timescales.184,185,849 It is this latter characteristic, aris- accumulation and dissipation due to high intensity optical pumping.
ing from their non-parabolic band structure, which distinguishes them Thus, the discussion as to whether or not transparent conductive
from most semiconductors and dielectrics, where real-state transitions oxides may offer a platform to explore photonic time crystals is an
occur over nanosecond periods.850 open one that hinges on the limits of the materials and the demand for
In wake of their discovery, sub-wavelength films of transparent power densities on the order of TWs/cm2.845 As a result, the realization
conductive oxides have facilitated the fundamental explorations of of a periodic modulation may demand a sacrifice in magnitude of the
time-varying photonics. By pumping these films with high intensity, momentum bandgap, or duration of the periodic temporal modulation.
ultrafast pulses of light, it is possible to inhibit ultrafast changes in per- More clarity regarding the future of photonic time crystals generated
mittivity via both the real and virtual electronic transitions. Through with transparent conductive oxides will come from comprehensively
the utilization of the fast, virtual transitions, these systems have been theoretical model of these materials, including electronic and lattice
used to demonstrate negative refraction851 and time reflection,852 as temperature and their effect on the optical properties.865 As a result,
predicted a decade earlier.853 Congruently, the ultrafast, real-state tran- the realization of a periodic modulation may demand a sacrifice in
sitions have enabled investigations into temporal interfaces, character- magnitude of the momentum bandgap, or duration of the periodic
ized by unity changes in refractive index with ultrafast rise and decay temporal modulation, possibly led by use of the ultrafast virtual transi-
dynamics, see Fig. 21(a).854 Temporal scattering from these temporal tions.866 Moreover, the observation of momentum bandgap character-
interfaces has been studied extensively via pump-probe experiments, istics, induced by vð3Þ nonlinear phenomena may also be marred by
demonstrating a novel method of frequency control via the ultrafast the presence of undesirable nonlinear processes, a concern that has
dynamics of the transition’s rise and decay time, leading to red and begun discourse into the use of vð2Þ processes845 and investigations into
blue shifted light respectively.855 Moreover, these phenomena not only new media.
provide innovative approaches for nanophotonic frequency control
but also serve as diagnostic tools for inferring the temporal dynamics C. Time-modulation in spatial metasurfaces
of the material’s ultrafast response.855 However, the spectral control
As detailed throughout topics Secs. III and X in this roadmap,

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obtained from these simple responses is limited. Thus, the natural evo-
lution of time-modulated metasurfaces involves exploring more com- metasurfaces are great resonance-hosting systems capable of increasing
plex temporal inhomogeneities. In the case of the aforementioned the efficiency of nonlinear interactions, via increased field localization,
system, this would materialize as designing the pump pulse’s temporal offering control over the directionality and propagation of emitted
profile. Through the pursuit of this avenue, it would be possible to light. The increased localization of electric field and thus energy has
investigate the eigenpulses of a time-varying system—temporal modu- allowed for time-varying systems that enhance effects engineered by
lations related to the Fresnel coefficients for the dispersive, time- spatial structures. For example, in semiconductor-based metasurfaces,
varying interface in question, which leaves scattered light spectrally temporal boundaries have been studied as tools for the enhancement
unchanged.856 Conversely, through careful design of the temporal pro- and control of nonlinear spectral effects induced by resonance-hosting
file of the modulation, one would also be able to design the spectral structures.867–872 Notably, the utilization of gold nanoantennas has
profile of the scattered light, offering applications across the fields of been central to numerous studies that observed reduced intensity
optical switching and computing.857 Moreover, promising theoretical requirements for significant frequency shifts based on temporal refrac-
investigations into systems that exhibit isotropic-to-anisotropic switch- tion by localizing energy in a transparent conductive oxide struc-
ing have motivated the concurrent pursuit of compatible media capa- ture.851,876 In these spatially structured devices, resonances are
ble of hosting unique temporal phenomena.858–860 leveraged to provide increased modulation amplitude at the expense of
Another direction of research regarding increased complexity of an increased interaction time. Hence, while these structures signifi-
temporal structuring, is the generation of periodic modulations. A first cantly enhance nonlinear efficiencies, temporal phenomena are con-
step toward this goal has been the investigation of double slit time dif- strained due to increased modulation timescales and the diminished
fraction a study which utilized two temporally adjacent modulation optical damage threshold.875 Yet despite the presence of these deleteri-
responses to obtain the characteristic diffraction response in the spectra ous characteristics, this paradigm offers a route to realizing low-power
of scattered light [Fig. 29(b)].861 A challenging extension to this frame- technological applications of these phenomena. In addition, the 1D
work of patterning numerous responses in time is the generation of a temporal modulation of a resonant structure that hosts an effective lat-
photonic time crystal. By mimicking the configuration of photonic tice of states, constructed via the structure’s supported modes, provides
space crystals in the time domain, periodic temporal modulations, gen- a method for accessing synthetic frequency dimensions. By using a
erated with a frequency comparable or greater than the probe frequency, time-varying modulation with a configurable amplitude, modulation
create bandgaps in momentum. The relative width of these bandgaps is frequency or phase, one can utilize the temporal domain as a method
dependent on the contrast of the temporal interfaces induced. Light to navigate the system’s synthetic dimensions.876 The realization of
propagating within these momentum bandgaps does so with an energy these synthetic dimensions promises to uncover a wealth of higher-
that exponentially grows in time, comprising a non-resonant amplifica- dimensional topological effects, as well as a potential route toward N
tion system.114,862 Additionally, periodic temporal modulations have dimensional control, alongside the benefits of conventional time-
been proposed as mechanisms for realizing surface-wave excitation in varying.836,876

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Alongside the amplification of nonlinear processes, static struc- photocarrier excitation in transparent conductive oxides, the modula-
tures offer systems from which the momentum of scattered light may tion can be controlled in space and time by manipulating the intensity
be configured. This framework, embodied by the pioneering metasur- and shape of the pump beam in both domains. This premise relies
face work of the early 2000s,877,878 in conjunction with temporal mod- heavily on the profound advancements made throughout digital micro-
ulations, enables frequency and momentum control over scattered mirror devices and spatial light modulators and has been effectively
light. By temporally modulating a gold gradient metasurface upon a applied to the fields of ultrafast beam steering,88 electron optics,881
transparent conductive oxide substrate, pioneering work by Karimi reconfigurable metasurfaces,882 and the generation of reconfigurable
et al.879 demonstrated simultaneous, dynamic control over the spectral integrated photonic circuits.883 Following in this vein, pursuit of such a
content of light that has been diffracted [Fig. 21(c)]. Moreover, the modulation strategy would reveal all-optical, reconfigurable metasurfa-
process of frequency translation via temporal refraction leads to beam ces capable of also harnessing temporal frequency generation.50,884 In
steering, via the conservation of the forward momentum, and thus 2023, Fan et al. demonstrated ultrafast wavefront control via the all-
dynamic control over the angle of the generated diffraction orders. It optical structuring of a thin film’s refractive index in both space and
can be envisioned that this framework offers a logical extension to the time [Fig. 21(d)].885 This work used the induced space-time modulation
impressive metalens work of the past decade,880 providing an all- to provide a spatially dependent response of temporal refraction, result-
optical method of fine-tuning the focal distance through beam steering ing in the focusing of probe light due to the subsequent beam steering.
or offering simultaneous spectral control. At present, these systems for In extension to this work, one can easily envisage simultaneous control
4D optical control offer potential applications across the field of over spatial diffraction from configurable diffraction-limited transient
dynamic metasurface designed for sensing and beam steering, how- structures alongside this time-varying control. This paradigm of simul-
ever, they also present a stepping stone toward unlocking the potential taneous structuring in space and time for ultrafast control of light lends
of simultaneous frequency and momentum control.846 itself straight-forwardly to 4D optics but also the advancement of opti-
cal holography,886 analogue optical computation,46 and neural net-
works.887 However, the generation of space-time modulations using
D. Space-time metasurfaces photocarrier excitation in transparent conductive oxides will encounter
In the previous section, spatially static, yet temporally varying, the constraint of the material’s high intensity requirements for high
optical metasurfaces were initially discussed as the most mature method contrast modulations ( 100 GW/cm2 for 100 fs pulses184) limiting
of structuring a device in space and time. Herein, space-time metasurfa- their complexity and size. This represents an avenue that may greatly
ces are differentiated by their use of a modulation mechanism that is benefit from the use of efficiency-increasing gold nanoantennas in

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configured in both space and time in order to exhibit control over the order to not only reduce power requirements but also as a method of
momentum and frequency of scattered light. In the context of localizing modulations to non-diffraction-limited regions. Thus, in

FIG. 29. (a) A spectrogram of negative and positive frequency translation via sub-cycle pumping of ITO.854 (b) Full experimental and theoretical interferograms for diffracted
light from a temporal double slit as a function of slit separation and frequency.861 (c) Spectrogram showing the ultrafast beam steering of light diffracted by a temporally modu-
lated static gradient metasurface.879 (d) Schematic displaying wavefront manipulation from a material structured in space and time.885 (e) A schematic illustrating the theoretical
demonstration of amplification and compression of light incident upon a luminal grating.888 (f) An illustration of non-reciprocal beam steering generated by a space-time modu-
lated metasurface based upon the illumination of a static, dielectric metasurface.889 Figures adapted from Refs. 854, 861, 879, 885, 888, and 889 and copyright remains with
the respective publishers.

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closing, achieving simultaneous spatial and temporal structuring of temporal and spatial modulations unveils a plethora of exciting
inhomogeneities is a significant milestone for space-time metasurfaces, research avenues in the field. Modulations in time alone provide a the-
but unlocking their full potential requires the development of new and oretical research destination of prophesied photonic time crystals,
improved time-varying systems. while complex space-time modulations unlock the potential of 4D
The exploration of traveling modulations of permittivity within optical components and synthetic motion. However, most advanced
dielectric media signifies this report’s concluding frontier in the inves- discussions and explorations have predominantly existed within the
tigation of optical time-varying metasurfaces, presenting experimental realm of theoretical and computational physics. In order for a majority
challenges beyond the previously discussed space-time metasurfaces. of these phenomena to be fully realized, the restrictions of the current
Systems which host traveling regions of modulated permittivity are systems must be overcome. It is possible that many applications may
generally referred to spatiotemporal metasurfaces. These traveling be realized, in a less efficient form, via a compromise with regard to
regions can be defined by a permittivity (and corresponding perme- the desired modulation strength or frequency. However, in order to
ability) that is described by deðx; tÞ ¼ deðgx XtÞ, where g and X are observe many advanced temporal or spatiotemporal phenomena, new
the spatial and temporal reciprocal lattice vectors. Spatiotemporal systems or mechanisms will be required. These considerations have
modulations have promised to result in a broad variety of phenomena begun to occupy an increasing presence in modern discussions of
and are thus defined by the modulation’s speed of travel m ¼ X=g. time-varying optical experiments, applying pressure on this direction
By consequence of this traveling modulation, physically realized of research. Nevertheless, the future of the field still promises to offer
through the conjunction of a modulation and the material response, great potential to light-based technologies and studies of novel physics.
probing light will observe synthetic motion of the modulation. This
phenomenon has been explored as a method to exert control over the XVI. DISORDERED OPTICAL METASURFACES: PHYSICS,
spectrum of scattered light via an artificial Doppler shift,890 capable of THEORY AND DESIGN
compensating for the Doppler shift of moving objects.891 Furthermore,
slab structures that host a traveling wave modulation offer unique Philippe Lalanne, Alexandre Dmitriev, Carsten
applications throughout beam splitting892 and recombination.893 Rockstuhl, Alexander Sprafke, and Kevin Vynck
Moreover, there has been broad research into the phenomena demon-
strated by such spatiotemporal synthetic motion, including Fresnel [Link]@[Link]

drag,894 Cerenkov radiation,895 and Hawking Radiation.896 The use of coherent wave phenomena to enhance device perfor-
Discussions into the demonstration of these phenomena have

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mance is a cornerstone of modern optics. In juxtaposition to (locally)
remarked the viability in low frequency regimes, as well as potentially periodic metasurfaces, their disordered counterparts exhibit an inter-
the terahertz regime in graphene, however, their demonstration in the play of destructive and constructive interferences occurring at the
optical regime is closely linked to the discussion of hosting period same spatial and spectral frequencies. This attribute provides disorder
modulations in time alone (Sec. XV B). with many degrees of freedom. Recognizing and comprehending their
In parallel, linear or rotational traveling modulations have been
utility across diverse applications is invaluable. Hereafter, we provide a
investigated throughout numerous wave domains as novel systems for
concise overview of the cutting-edge developments and offer insights
leveraging non-reciprocal responses. Notably, the inherently non-
into the forthcoming research in this dynamic field.
reciprocity of luminal synthetic motion represents a platform capable
of the amplification and compression of incident light [Fig. 21(e)].888
Moreover, such mechanisms have been heralded as a method for effi- A. Introduction
ciently breaking the constraints of a system’s reciprocal symmetry and Disorder has often been viewed as a constraining element in
thus offering a route toward compact, non-reciprocal devices without nanophotonics, which might explain the limited coverage of the sub-
need for magnetic bias, see Fig. 21.889,897 Consequently, a core motiva- ject of disordered metasurfaces in the existing literature.524,899
tion of research in this direction of spatiotemporal modulations is the Nevertheless, there exist plenty of reasons to delve into this area. Let us
pursuit of phenomena that do not rely upon high modulation frequen- highlight just a few. The presence of disorder is ubiquitous across man-
cies that are difficult to realize in physical systems.898 Moreover, could ifold complex structures. Leveraging disordered metasurfaces, as
spatiotemporal modulations substitute for modulations in time alone, opposed to their meticulously ordered counterparts, holds promise in
resulting in more feasible realizations of the temporal woods analogy realizing extensive, cost-effective devices. It also paves the way to a
or Bragg grating? Unlike periodic temporal modulations, the material wealth of specialized applications, such as anti-reflection coatings,900
limitations imposed upon the exploration of spatiotemporal modula- augmented absorption,901 surface-enhanced Raman scattering,902
tions have not been theoretically characterized—leaving the door open alongside contemporary applications to be discussed below.
to a rich experimental future. This article aims to survey the current state of research and offer
a forward-looking perspective on the topic. We highlight a few promis-
E. Conclusion ing future applications and anticipate forthcoming advancements in
design and fabrication.
Research into time-varying systems has reshaped the way we per-
ceive and control the propagation of waves. The last decade has
brought time-varying physics to the optical regime with seminal stud- B. State-of-the-art
ies being performed upon the framework of photocarrier excitation in The general problem of light scattering by disordered meta-
transparent conductive oxides. As discussed herein, the multitude of surfaces made of resonant nano-objects (a.k.a. meta-atoms) is very
pathways to enhance the complexity of current straightforward complicated due to multiscale effects, namely the multipolar

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FIG. 30. Illustration of the average (coherent) and fluctuating (incoherent) components of the scattered field [Eq. (4)] with fully vectorial simulations for a finite-size disordered
metasurface composed of identical Si nanocylinders in air. The incident (background) field Eb is a plane wave (k ¼ 440 nm) polarized along the y-direction. It is incident from
the top with an angle of 30 with respect to the surface normal. The rods are parallel to the y-axis and are placed using a random sequential addition algorithm with a non-
overlapping condition. The 2D simulations are made for assemblies of 15 infinitely-long nanocylinders (140 nm diameter, nSi@440nm ¼ 4:793 þ 0:109i), resulting in a side length
of 7.0 lm ( 16k) at a surface coverage of 30%. The y-component of the scattered field (component parallel to the cylinder y-axis), Es , is normalized to the amplitude of the
background field jEb j.

resonances of the individual particles, their interaction with the describes the diffracted light from a homogenized metasurface charac-
substrate, and their mutual interaction.903,904 In this section, we terized by effective parameters that vary non-uniformly in both the x
start by outlining some fundamental concepts on coherent vs inco- and z directions due to boundary effects.
herent scattering. We then familiarize the reader with computa- Given hdEs i ¼ 0, we can readily demonstrate that the averaged
tional tools and approximate models that predict the scattering intensity hjEs j2 i of the light scattered by the metasurface can be
properties of disordered metasurfaces, and finally examine recent decomposed into two components,
advances in fabrication techniques.
hjEs j2 i ¼ jhEs ij2 þ hjdEs j2 i; (5)
1. Diffuse (incoherent) vs. specular (coherent) light in which we identify the squared norm of the average field, which cor-
Within the context of wave scattering by rough surfaces—a responds to the specular intensity (first term), and the average of the
long-standing topic with many applications905–907—, the distinc- squared norm of the fluctuating field, i.e., the diffuse intensity or the
averaged speckle intensity (second term).

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tion between diffuse (incoherent) light and specular (coherent)
light emerges as a pivotal consideration. These two components The properties of statistically translationally invariant (i.e.,
have different physical origins, as we will see below, and have sig- infinite) disordered metasurfaces are fully determined by the
nificant implications for optical effects—for instance, their relative Bidirectional Scattering Distribution Function (BSDF), a radiomet-
weight play a decisive role in determining the glossiness or matte- ric quantity introduced in the 1960s, which describes how surfaces
ness of a surface. scatter light for all possible plane wave illuminations. Formally, the
This distinction can be understood from the statistical properties BSDF relates an incoming irradiance Ei (in W m–2) to a scattered
of the scattered light. In this framework, one considers separately the radiance Ls (in W m–2 sr–1),
average and fluctuating values of physical parameters, with the aver-
dLs ðk^ s ; ^e s ; xÞ
ages computed among a large statistical ensemble of independent real- BSDFðk^ s ; ^e s ; k^ i ; ^e i ; xÞ ¼ ; (6)
izations. The quantities of main interest in the present case are dEi ðk^ i ; ^e i ; xÞ
electromagnetic field characteristics, including the field itself, its inten- where x is the frequency, k^ i and k^ s are the (unit) wavevectors of the
sity or root mean square, along with auxiliary quantities such as the incident and scattered plane waves, and ^e i and ^e s are the polarization
Poynting vector and the energy density that a wave carries. (unit) vectors of those waves. Following the previous considerations,
Formally, the electric field Es scattered by a disordered system the BSDF can then be conveniently decomposed into two terms,
can be expressed as the sum of its ensemble average (the specular
BSDF ¼ BSDFspec þ BSDFdiff, the specular and diffuse components.
light), calculated among many disorder realizations, and a fluctuating
term (the diffuse light) that varies from configuration to configuration,
2. Full-wave analysis
Es ¼ hEs i þ dEs ; (4)
Predicting the BSDF of statistically translationally invariant meta-
with hdEs i ¼ 0. surfaces featuring resonant particles on layered substrates stands as an
Figure 30 illustrates this decomposition using fully vectorial simu- outstanding challenge.909,910 Two complementary strategies are
lations conducted on a finite metasurface composed of parallel infi- employed. The first approach involves solving Maxwell equations with
nitely long silicon nanocylinders in air. The metasurface is illuminated utmost precision, while the second approach (Sec. XVI B 3) relies on
at a 30 angle of incidence by a plane wave polarized parallel to the cyl- approximate models.
inder y-axis. In the rightmost panel, the fluctuating field dEs showcases In the former approach, the strategy is twofold: first, solving
a complex pattern known as speckle,908 which arises from the intricate Maxwell equations for larger and larger metasurfaces, and second,
interplay of near-field interactions among many monochromatic inferring the BSDF of infinitely large metasurfaces by extrapolation. In
waves scattered by multiple scatterers. In contrast, the central panel contrast to traditional general-purpose solvers such as the finite-
presents the average field hEs i that readily takes the form of a direc- difference time-domain method, disordered metasurfaces benefit sig-
tional reflected light beam indicated by black arrows. This average field nificantly from specialized numerical techniques. The latter harness

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the unique morphologies of these structures and enhance their effi- intensity (measured in W m–2). SðqÞ is the structure factor, which
ciency by precomputing light scattering by the individual scatterers incorporates the effect of far-field interference between pairs of par-
that compose the metasurface. ticles on the scattered intensity, and is defined as
In the widely used T-matrix method, the field outside the scat- * +
terer is expanded using spherical vectorial wave harmonics and a T- 1 X N
SðqÞ ¼ 1 þ exp ½iq ðrm rn Þ ; (8)
matrix is utilized to describe how each scatterer transforms incident N m6¼n
into scattered multipolar fields. The method has been extensively
explored over decades911 and is now available through multiple open- where q ¼ x=cnb ðk^ i k^ s Þ is the wavevector difference between the
source implementations.911,912 Alternative methods account for multi- incident and scattered waves and nb is the refractive index of the back-
ple scattering using vectorial Green functions and treat scatterers as ground medium.
ensembles of equivalent electric and magnetic surface currents,913,914 The structure factor can be readily evaluated through statistical
or employ numerical non-local dipoles915 obtained by numerically averaging. On the other hand, accurate determination of the form
solving an inverse scattering problem. A detailed comparative analysis factor involves iteratively solving Maxwell equations for multiple wave-
of these methods strengths and limitations is beyond this roadmap’s lengths, incidences, and polarizations, followed by applying a near-to-
scope and is deferred to a comprehensive future review.916 far-field transformation to obtain the radiation pattern. Alternatively, a
Two approaches exist for the extrapolation step. In the field quicker approach with deeper insights can be achieved by expanding
stitching approach, Maxwell equations are solved for numerous small the differential scattering cross section using the resonance modes of
square subdomains, each corresponding to an independent realization. the nanoparticles.923
These subdomains are then stitched together to artificially expand the Exploiting Eq. (7), one can derive straightforward expressions for
metasurface area, with field discontinuities smoothed at subdomain the BSDF of infinite metasurfaces with N ! 1. However, due to the
boundaries to mitigate artifacts.917 In the supercell approach, identical inherent limitations of the ISA, the model’s predictions exhibit notable
subdomains are “stitched” with pseudo-periodic boundary conditions. inaccuracies for high particle densities, grazing incident angles, or large
As the artificial period increases, both approaches generally yield stable angles. These inaccuracies prompt the need for further refinements
numerical outcomes for specular and diffuse light.918,919 Although and extensions. For readers seeking a more comprehensive under-
finite-size computations unavoidably introduce boundary effects,919 standing, let us note that advanced models for the diffuse contribution
the observed relative errors are often encouragingly below 10%. in the BSDF have been presented in Ref. 918. For the specular contri-
bution, an overview of various models can be found in a recent book

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However, the two approaches necessitate numerous computa-
chapter920 and the references therein. Noteworthy is the remarkable
tions to assess statistical convergence, and they offer limited physical
efficacy demonstrated by the quasi-crystalline approximation.921,925
insights. The challenge of effectively simulating infinite metasurfaces
remains, highlighting the need for approximate models.
4. Fabrication
3. Approximate models Several techniques exist for fabricating disordered metasurfaces.
Top-down patterning methods, which make use of electron-beam or
There are a few available models for predicting the BSDF of dis-
optical lithography, facilitate the precise positioning of the meta-atoms
ordered metasurfaces. Similar to research conducted on metamaterials,
with nanometer-level precision and a fine-tuned control over meta-
advanced studies have primarily focused on homogenization, i.e., on
atom size and shape. Furthermore, with the advent of nanoimprint
the specular contribution to the BSDF.883,884,922,923 To our knowledge,
lithography924 and soft lithography,925 they have opened up new ave-
there has been no research on diffuse light, despite its critical signifi-
nues for cost-effective fabrication.
cance in our context. An exception to this is the independent scattering Conversely, bottom-up approaches prioritize scalability and cost-
approximation (ISA), which assumes that each constituent particle efficiency over precision. Although they may not match top-down
scatters light independently, thus neglecting multiple scattering effects. techniques in shaping and arranging nano-objects, their utility remains
Although the ISA may appear simplistic to readers, it holds substantial unequaled.
value. This approximation plays a significant role in investigations on Among metasurfaces fabricated by scalable and cost-effective
the physics of waves in complex media. It also largely facilitates a techniques, semicontinuous colloidal films composed of metal nano-
transparent interpretation that is beneficial during the initial design islands stand out. These films naturally arise from deposition techni-
phases and is amenable to more accurate models relying on mean ques that interrupt metal film growth before percolation threshold is
fields.916 For a monolayer comprising N identical particles randomly reached.926 Originally investigated for enhanced Raman scattering,927
positioned at coordinates rp ¼ ½xp ; yp ; zp ¼ 0; p ¼ 1; …; N, the ISA these ultra-affordable films can be mass-produced by the glass industry
simply leads to on extensive scales, spanning tens of square meters. Because island
drs ^ dimensions and interspace distances are much smaller than visible
hIs iðk^ s ; ^e s ; k^ i ; ^e i ; xÞ ¼ I0 N ðk s ; ^e s ; k^ i ; ^e i ; xÞSðqÞ; (7) wavelengths, nanoisland metasurfaces act as coherent layers, absorbing
dX
rather than scattering incident light. Alternatives, such as utilizing
for the total radiant intensity hIs i (measured in W sr–1), encompassing block copolymer templates for self-assembly,928,929 also facilitate
both coherent and incoherent components, scattered by the particles. monolayer creation with such tiny particles.
In Eq. (7), drs =dX (measured in m2 sr–1) is the differential scattering Producing disordered configurations with larger particles
cross section of individual particles—a quantity directly related to the involves assembling pre-synthesized particles onto surfaces. Various
so-called form factor in condensed matter physics. I0 is the incident techniques fit within this category:

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For deeper insights, recent comprehensive reviews provide

substantial information regarding the subject. They additionally
cover deposition methods enabling the creation of densely packed
monolayers. These monolayers exhibit high sensitivity to electro-
magnetic near-field interactions. They offer complex and possibly
rich optical responses due to enhanced particle couplings and spa-
tial dispersion. Future research directions should, therefore,
include a more thorough investigation of these dense configura-
tions, extending modeling approaches far beyond the limits of ISA
and mean-field theories.99,933–936

C. Future directions and outlook

Disordered optical metasurfaces have unveiled a plethora of
applications, some of which can be traced back to historical con-
tributions, such as porous film-based anti-reflective coatings by
Fraunhofer in 1887,900 and observations of ultra-strong Raman
signals from semicontinuous nanoisland metal films in the 1970s.902
Over the past two decades, the field of disordered optical metasurfa-
ces has experienced remarkable activity, encompassing a diverse
array of applications. These include wide-angle broadband absorp-
tion,932,937,938 anti-counterfeiting measures,939 anti-reflection

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FIG. 31. A few selected examples of disordered metasurfaces fabricated with colloi-
dal chemistry. (a) Availability of almost monodisperse nanospheres in various
dielectric materials, e.g., PMMA, high-index Si nanospheres in the present figure.930
(b) Amorphous colloidal monolayers of polystyrene nanospheres with sizes of 170
and 270 nm with short-range order.931 (c) Monolayer of Au nanocubes with corre-
lated disorder on a 2.5 cm-diameter half sphere.932 All images are reprinted
(adapted) with permission from the respective Journal and copyright remains with
the original publisher.

• Colloidal lithography: This method hinges on nearly uniform in

size colloids in solutions of materials like polystyrene, PMMA, or
Si nanospheres930 [Figs. 31(a) and 31(b)]. After drop-casting and
drying, a monolayer forms,931 subsequently serving as a mask to
imprint patterns into underlying substrates. Since the sizing of
polymer beads and strategies for self-assembly—utilizing repul-
sive and attractive forces for instance—are well-mastered FIG. 32. (a) Harnessing the BRDF toward full manipulation of diffuse and specular
[Fig. 31(b)], the transferred patterns, often arrays of nanodiscs or light. In the sketchy example, the surface color varies abruptly, differently from the
continuous color variation of classical iridescence, when the light source and/or the
nanoholes in various materials, are fabricated on large scales with observer position move. (b) Hyperuniform metasurface for light trapping in solar cell
high fidelity and few aggregates. application. After Ref. 968. (c) Rendered images showing the visual appearances of
• Self-assembly: With this method, colloidal nanoparticles, ini- a car coated with disordered arrays of identical Ag nanospheres with a density of
tially stabilized in solution, arrange on surfaces via methods 4 lm–1. Top: no structural correlation. Bottom: short-range correlated disorder.
like blade coating, dropcasting, and dip coating.932 Diverse Adapted from Ref. 918. (d) Transparent display made of a bilayer metasurface
which offer completely different properties in reflection and transmission. The right-
particle shapes, sizes and materials are commercially available,
most images are camera pictures of a flower bouquet taken in reflection (top) or in
and controlled short-range arrangements can be achieved transmission (bottom). After Ref. 945. All images are reprinted (adapted) with per-
through nanoparticle and substrate surface functionalization mission from the respective Journal and copyright remains with the original
[Fig. 31(c)]. publisher.

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coating,900,917,940 wavefront manipulation,701,941,942 transparent dis-

plays,943,944 chiral films,945 fade-resistant structural coloring,938,946–950
visual effects,918,923 plasmonic electronic paper,951 solar radiation
management in architectural and consumer products glazing,952–955
radiative cooling,956 photocatalysis,957 light trapping in solar cells,931
and light extraction in LEDs.958–961
As nanofabrication capabilities continue to advance, these appli-
cations are progressively moving closer to industrial-scale production.
In the subsequent sections, we delve into emerging applications that
are poised to inspire numerous studies and emphasize two prospective FIG. 33. (a) Metasurfaces fabricated on curved substrates: air holes etched in
avenues for enhancing manufacturing flexibility and reducing pyramid-textured Si surfaces. Adapted from Ref. 975. (b) Production of vivid colors
manufacturing costs. despite a strong polydispersity in the size and shape of Al nanoislands used to res-
onantly absorb light. The resonance is due to nanogap plasmons supported by the
1. Prospective applications capped nanoislands obtained by dewetting on Al2O3/Al substrate (inset). The pho-
tography shows a black canvas painted with oil–based plasmonic paints obtained
Anticipating the forthcoming wave of research, we expect a con- by dispersing metasurface flakes in commercial paint oils. Adapted from Ref. 950.
certed effort to tackle the enduring question of how to master the All images are reprinted (adapted) with permission from the respective Journal and
copyright remains with the original publisher.
nanopatterning of surfaces for shaping the far-field radiation across
both spatial and spectral frequency domains. The ultimate ambition is
to attain comprehensive command over both specular and diffuse Future exploratory directions may capitalize on the monolithic
light. It encompasses manipulating independently these two compo- integration of multiple metasurface layers. A compelling feature of
nents, sculpting the directional patterns of diffuse light, monitoring these surfaces is their distinct behavior concerning diffuse light in
alterations in light color for varying viewing and illumination angles, transmission vs reflection. This contrast can be readily comprehended
and, in essence, molding the BSDF at will [Fig. 32(a)]. by examining the structure factor, SðqÞ in Eq. (8), in which q signifies
Two key physical parameters that play pivotal roles can be used the difference in wavevector between the scattered direction and inci-
for design [see Eq. (7)]. Through the form factor, an assortment of dent directions. It becomes evident that ðki k s Þ:ðrm rn Þ in the
shapes and high-index materials may be used to manipulate the reso- exponential term remains independent of the normal coordinate z

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nances of the meta-atoms at the nanoscale. These resonances may be around the specular transmitted direction (where k s kt k i ). In
further enriched through mode hybridization at the wavelength scale contrast, this term does vary with the normal coordinate around the
to achieve wavelength-selective control over the directionality of scat- specular reflected direction (where k s kr ki ). This intrinsic
tered light.471,962,963 Through the structure factor, we may engineer property has recently been ingeniously harnessed to create a transpar-
intricate mesoscale interferences. This engineering encompasses a vast ent display944 that selectively scatters reflected light while preserving
landscape of arrangements,524,964 ranging from full periodicity to transmitted light integrity [Fig. 32(d)].
entirely uncorrelated disorders. This gamut includes quasicrystals,
weakly defective crystals, hyperuniform configurations, and more. For 2. Metasurfaces on curved substrates
example, enforcing greater inter-particle distances engenders a short-
range amorphous-type correlation that mitigates the presence of dif- An overwhelming number of nanopatterning methods, including
fuse light around the specular direction,918,965 regardless of the angle of optical and electronic lithography, nanoimprint lithography,924 soft-
incidence. lithography,925 DNA-templating,969 and functional block copoly-
This effect is even more pronounced within stealthy hyperuni- mers,970 are available nowadays. They often function on 2D and atom-
form metasurfaces, which entirely suppress scattering within an angu- ically flat surfaces.
lar range centered on the specular direction.524 Ongoing endeavors in In general, adapting methods tailored for flat surfaces to curved
the domain of hyperuniform disordered scattering structures, particu- ones necessitates significant changes to mitigate curvature-induced
larly for solar cells, are only just emerging.965–968 A particularly variations in feature attributes like size, orientation, and spacing.
remarkable recent achievement is the 2.5-fold enhancement in absorp- While some fabrication methods can accommodate relatively simple
tion of a 1 lm-thick silicon slab, thanks to a hyperuniform metasurface curvatures, the adaptation challenge grows as curvature intensifies.
[Fig. 32(b)] meticulously designed to trap incident light into the slab This puts severe limitations onto the use of metasurfaces in a variety of
guided modes.968 every-day-use or advanced technologies, where materials with non-
Disordered optical metasurfaces also hold significant promise for planar, rough, soft, mechanically agile, or chemically sensitive surfaces
applications in applied and fine arts. Metasurfaces offer the potential are used.971–973
to manipulate the visual characteristics–such as color, glossiness, haze, Recently, several transfer protocols have been proposed to over-
transparency, and iridescence–of macroscopic objects of any conceiv- come the limitations.932,973–975 Figure 33(a) shows the example of a
able shape.918 A recent breakthrough in this domain introduced a mul- pyramid-textured Si surfaces which has been patterned with air holes
tiscale numerical tool capable of generating lifelike images of diverse to lower reflection at the Si-air interfaces and enhance the total absorp-
macroscopic objects covered with disordered metasurfaces [Fig. 32(c)]. tion. The hole pattern is obtained from a template manufactured with
This tool not only forecasts subtle effects resulting from the interplay colloidal lithography (other bottom-up or top-down approaches may
between diffuse and specular light but also unveils entirely new visual be used as well). In many instances, the key is the use of a 10 nm-thin
effects. carbon film deposited on a sacrificial layer for the template. Such a

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thin film combines extreme strength with a large degree of flexibility leading to a confined gap-plasmon resonance within the alumina film
that facilitates conformation of the transferred pattern to nearly any stands as a logical explanation, it is important to acknowledge the
macroscopic or microscopic 3D object. influence of other mechanisms as well. Among these, the generation of
subtractive color through the absorption of a “homogenized” film
3. Striving for ultra-low costs with augmented resilience emerges as a noteworthy consideration, deviating from the diffusion-
to fabrication imperfections based coloration observed with larger nanoparticles.

Optical metasurfaces, which harness resonant nanostruc- ACKNOWLEDGMENTS

tures at subwavelength scales, impose strong constraints on the
nanofabrication precision. These constraints are growing in sig- P.L. and K.V. acknowledge financial support from the French
nificance, as metasurfaces progress toward practical applications National Agency for Research (ANR) under the project “NANO-
that require large sample areas. In this evolving landscape, the APPEARANCE” (No. ANR-19-CE09-0014). A.D. acknowledges the
emergence of metasurfaces designed to exhibit resilience against Swedish Research Council for Sustainable Development (Formas)
imperfections becomes increasingly crucial. Recent studies have con- (Project No. 2021-01390). P.L. acknowledges financial support from
verged to provide compelling evidence that disordered arrays of nano- the European Research Council Advanced grant (Project UNSEEN
particles, when placed on a transparent dielectric spacer above a metallic No. 101097856). C.R. and A.S. acknowledge financial support from
substrate, exhibit an extraordinary resilience to variations in material, the Deutsche Forschungsgemeinschaft (DFG) (Nos. 413644979, RO
size, and nanoparticle shape. One fundamental mechanism that imparts 3640/11-1, and WE 4051/26-1).
resilience is through the process of mode hybridization.923 In scenarios
where plasmonic nanoparticles are situated on low-index substrates XVII. FROM PRINCIPLES TO PERFORMANCE: EPSILON-
without undergoing hybridization, the electromagnetic field becomes NEAR-ZERO METASURFACES FOR NONLINEAR
profoundly confined around the individual particle. Consequently, even OPTICAL DEVICES
slight variations in material composition or shape induce significant
shifts in resonance frequencies. For context, even a minor alteration of Jeremy Upham, M. Zahirul Alam, Israel De Leon, Robert
10 nm in the dimensions of a metal nanoparticle leads to a resonance W. Boyd, and Sebastian A. Schulz
wavelength shift of 10–20 nm. In contrast, within hybridized modes, the
field localization diminishes as it extends into the transparent layer. sas35@[Link]

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Consequently, hybridization inherently mitigates sensitivity to size and
Epsilon-near-zero (ENZ) materials, particularly thin films of
material polydispersity. This general attribute of hybrid modes has facili-
transparent conductive oxides, exhibit a variety of intriguing opti-
tated the discovery of a remarkable diffuse iridescence phenomenon, in
cal phenomena, two of which should be of particular interest to the
which a mere two distinct and vivid colors are discernible across all
metasurface community: (1) ENZ materials of sub-wavelength
angles of illumination and viewing, even when confronted with signifi-
thicknesses can exhibit large and very fast nonlinear optical
cant variations in nanoparticle size and shape across the metasurface.923
responses, including significant nonlinear phase shifts; (2) the
An alternative resilience mechanism emerges when nanopar-
nanoantenna of a metasurface can strongly couple to long-range
ticles are substantially smaller than the wavelength. This scenario is
surface plasmon polariton modes of these low index thin films,
exemplified by semicontinuous nanoisland films on a dielectric
making these nonlinear optical responses even stronger. In this
spacer atop a metal substrate, where empirical observations reveal
article, we examine how these enormous nonlinearities are cur-
that the pivotal factor shaping the specular reflectance spectrum is
rently understood and highlight examples of how this functionality
the spacer thickness,947 rather than the typical expectation of the
is already being exploited for applications in nonlinear optics, such
nanoparticle material choice. This material-independent response
as frequency conversion, self-phase modulation, time-refraction,
has been experimentally verified for various materials like Ag, Au,
and beyond. Looking forward, the current limitations on ENZ-
Pt, Pd, and numerically for Al, Cr, Cu, Ni, among others, under
metasurface performance appear to be predominantly engineering
normal incidence.947 Thus commonly accessible materials such as
challenges rather than physical limitations. We argue that through
Cu or Al could substantially mitigate costs related to
creative metasurface design and intuitive materials science optimi-
nanostructure-based coloration.
zation, ENZ-metasurfaces are poised to transform from compelling
This striking property can be attributed to the amalgamation of
proofs of principle to high-performance, all-optical devices.
localized plasmonic resonances at the nanoisland scale, hot spots
within the interstitial gaps, and delocalized modes, irrespective of the
metal used for the nanoislands. This synergy results in broad absorp- A. Introduction: The physics of ENZ
tion, further enhanced by the diversity in island size and shape. Exciting subsets of current metasurface research include the
Consequently, the film uniformly absorbs the incident light, except for development of dynamic, temporally varying devices and the enhance-
the Fabry–Perot resonance of the thin transparent spacer, for which ment of nonlinear optical responses to expand metasurface functional-
the field is nearly null within the semicontinuous film. ity. Fortunately, this has proven to be achievable simply by
Yet another illustration of resilience against manufacturing incorporating thin film layers of a class of materials with vanishing
defects is observed in a recent work on ultralight plasmonic structural- permittivity known as epsilon-near-zero (ENZ) materials. A material
color paints950 with a notably low-cost morphology shown in the inset is said to have ENZ properties if its dispersion curve features a spectral
of Fig. 33(b). Impressively, vibrant colors are attainable despite the region where 1 < ReðeÞ < 1, typically with the ENZ-crossing being
substantial variance in nanoisland sizes. While plasmon hybridization the wavelength where the real part of the permittivity crosses from

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1. Materials with ENZ properties

Depending on what part of the EM spectrum is being considered,
there are multiple ways to achieve this ENZ condition. At radio fre-
quencies well-established metamaterials such as arrays of split ring res-
onators can easily achieve this state,984,985 and similarly, ENZ behavior
has been shown in microwaves986 and through phononic resonances
in the THz spectral region.987,988 Within the deep UV, many metals
have ENZ crossings (e.g., silver near k ¼ 320 nm989) For the visible
and near- to mid-infrared spectral regions, two solutions exist. The
first is to engineer structures, either photonic crystal-like band struc-
tures982 or multi-layer materials, with an effective index990–993 such
that their effective permittivity is near zero. However, in the context of
metasurfaces, the prevailing solution has been to use transparent con-
ductive oxides (TCOs).994,995 These non-stoichiometric materials are
typically transparent dielectrics such as indium oxide, aluminum
FIG. 34. Dispersion of the real and imaginary components of the permittivity, as
oxide, or cadmium oxide that are degenerately doped so that the Fermi
well as the real part of the refractive index, for a typical ENZ material. kENZ indi- level moves to the conduction band. These TCOs hit a sweet spot for
cates the wavelength where the real part of the permittivity crosses zero. The ENZ performance in the near to mid-infrared range: they feature suffi-
shaded region indicates the ENZ spectral range where 1 < ReðeÞ < 1. Because cient free carriers to achieve a crossing of the real part of the permittiv-
the real part of the refractive index also depends on the imaginary part of the per- ity from positive to negative, but still fewer than noble metals, and
mittivity, the refractive index minimum is near, but not necessarily within the ENZ hence the crossing occurs at longer wavelengths. Furthermore, the
spectral range.
concentration and mobility of the carriers (the key factors determining
the plasma frequency) can be controlled during TCO deposition, e.g.,
positive to negative. This effect leads to a wide variety of unconven- by tuning the doping concentration.996–999 Together with the naturally
tional optical behaviors in both the linear and nonlinear regimes.977,978 slightly different plasma frequency depending on the dopant (e.g.,
For example, waveguides formed from ENZ materials can feature cou- indium, gallium, aluminum), this means that TCOs can place this epsi-

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pling through arbitrary shaped channels, phase-matching free nonlin- lon near zero condition anywhere within a wide range of the near- to
ear processes or manipulation of radiation from nearby or embedded mid-IR spectrum, covering important regions for optical communica-
emitters.977 In other platforms more relevant to metasurface technolo- tions and sensing.1000
gies, ENZ films have shown enhancement of nonlinear effects such as Certain TCOs, such as indium tin oxide (ITO) and aluminum
harmonic generation979 and the nonlinear refractive index.184,185 zinc oxide (AZO), have become reasonably mature fabrication materi-
To clarify, while the ENZ condition typically has the real als because they can be deposited as transparent yet conductive thin
part of the permittivity cross from positive to negative, the imag- films that enable touchscreen and solar cell technology.1001,1002 Driven
inary component need not change sign, nor does the permeabil- by these applications to be transparent to visible light (dielectric in the
ity. Therefore, the refractive index need not become negative as visible spectrum) but also as conductive as possible (lots of free car-
in the case of negative index metamaterials 980,981 or even reach riers), they are readily available materials for thin films with a plasma
zero as in near zero index materials.982,983 The ENZ condition frequency just past the visible spectrum in the near-infrared. As a
often occurs naturally in Drude materials simply by the impact result, these thin films typically exhibit ENZ behavior between 1 and 2
lm, with the additional benefit of a reasonably small absorptive
of the plasma frequency on the dispersion curve, delineating
loss.996 Because the real part of the permittivity crosses zero at a wave-
where a material crosses from metallic to dielectric behavior.
length where the imaginary component is also small, the refractive
One can also obtain ENZ conditions in a Lorentz-type material
index is less than 1 as well.
for a sufficiently large value of the oscillator strength. While a
near-zero real part of the permittivity can also be achieved for
values of the refractive index larger than one in such materials at 2. ENZ induced behavior in TCOs
absorption resonances, these are typically accompanied by high A consequence of the refractive index falling below 1 is that the
imaginary permittivity values. In these cases, such excessively wavelength of light within that material is stretched compared to that
high losses prohibit the observation of the desired ENZ effects. of free space. Equivalently, as the index approaches zero, spatial phase
Therefore, we generally consider ENZ materials to be Drude- variation within the ENZ medium also goes to zero. Because light in a
type materials where both the absolute real part of the refractive zero index medium can only radiate away normal to the bounding
index and the permittivity are less than unity over some range of interfaces, this leads to interesting linear optical effects,977 such as light
frequencies. The schematic of Fig. 34 shows the dispersion of propagating through arbitrary channels,1003 or wavefront shaping at
permittivity and refractive index for a typical ENZ material. The interfaces.1004
spectral range where the real part of the permittivity has a mag- However, from the point of the original motivation, i.e., the desire
nitude less than one is the ENZ range. The real part of the refrac- for large, dynamic modulation of metasurface behavior, the nonlinear
tive index can be below 1 in this same region, but this also enhancement in ENZ materials is of more interest. Many convention-
depends on the imaginary component of the permittivity. ally held equations for nonlinear optical phenomena, such as the Kerr

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FIG. 35. First experimental demonstrations of large, optically driven changes of refractive index of TCOs in their ENZ spectral regions. (a) Pump-probe measurement of Dn ¼ 0:45 for
AZO at 1390 nm. Reproduced with permission from Caspani et al., Phys. Rev. Lett. 116, 233901 (2016). Copyright 2023 American Physical Society.185 (b) Z-scan measurements of
ITO showed a Dn ¼ 0:72 at 1240 nm.184 All images are reprinted (adapted) with permission from the respective Journal and copyright remains with the original publisher.

effect, are written to be inversely proportional to the real part of the be reconsidered, specifically the assumptions of n 1 and n Dn
ð3Þ
linear refractive index, e.g., n2 ¼ 4e0 cn3v0 Rðn0 Þ (where n2 and n0 are the are no longer valid, making a compelling case for the use of ENZ mate-
rials in nonlinear optics.1008
nonlinear and linear refractive indices, vð3Þ is the third order suscepti- While other, non-perturbative nonlinear effects have been
bility and e0 is the vacuum permittivity), suggesting that such phenom- demonstrated before (e.g., the semiconductor-to-metallic light- or
ena would be enhanced or even diverge within an ENZ material.1005 heat-induced phase transition in vanadium dioxide1009) such
This led to the prediction1006 and demonstration1007 of ENZ materials strong effects are typically slow, as such thermo-optic or thermo-
boosting the nonlinear generation of harmonic frequencies. chroic responses occur on the ms timescale or longer. In contrast
In 2016, two studies on nonlinear optics in TCOs investigated the to this, the nonlinear effects in the TCO materials occur on an
effect of all-optical nonlinear interactions on light propagation and ultrafast timescale.184,185,1010 Often the onset seems to match the

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reflection within ITO184 and AZO films.185 Both studies demonstrate temporal width of an ultrafast pump pulse and relaxation times are
very strong enhancement of the nonlinear refractive index, see Fig. 35, on the scale of a few-hundreds femtosecond.184,185,1010 This holds
with values of Dn ¼ 0:72 and Dn ¼ 0:45, respectively, corresponding potential for THz switching speed operation of ENZ-based devices.
to up to 500% of the linear refractive index,184,185 reaching the regime The underlying nonlinear response of the TCOs is dominated by
where the nonlinear response exceeded the linear component of the the free carriers, resulting in a hot electron-dominated effect.
refractive index. We thus note that the conventionally held equations When optically pumped, the available carriers in the conduction
of the Kerr and other nonlinear effects that are based on perturbative band experience intraband transitions that significantly change
descriptions are no longer appropriate. ENZ materials feature such a their distribution and consequently the plasma frequency of the
strong nonlinear response that the equations of nonlinear optics must material. Because the transitions are principally intraband, the elec-
trons cool quickly, explaining the rapid onset and relaxation of the
index change. These transitions are so fast that light witnessing
changes of the refractive index will undergo an equivalent change
of frequency through adiabatic frequency conversion, otherwise
known as time refraction852,1011,1012 discussed further in Sec. XV.
Interestingly, the magnitude of the observed index change stems
from the fact that the response is free carrier dominated, even though
these are present in low concentrations. Because of the significantly
lower carrier concentrations in the conduction band (compared to
conventional metals), the excitation of even a modest amount of car-
riers is enough to significantly alter the overall carrier distribution, the
Fermi level, and consequently the effective carrier mass and plasma
frequency. The Drude model can thus explain the change of the TCO’s
dispersion curve almost entirely as a change of the electron effective
mass due to the changed effective electron temperature1013 (see
Fig. 36). The observed response is all the more dramatic in the ENZ
FIG. 36. Modeling changes to the real part of the permittivity of ITO as a function of region, where the initially low linear index can be effectively tripled by
the electron temperature. The green curve (1240 nm) has a real permittivity of 0 the magnitude of the nonlinear index change.
when Te is at room temperature, but increases with electron temperature. When
While these rapid and robust index changes show significant
heated up to 4000 K, the black curve (1300 nm) becomes ENZ crossing wavelength.
Reproduced with permission from Baxter et al., Adv. Photonics Res. 4(3), 2200280 potential for rapidly modulated optical components, the transitions
(2023). Copyright 2023 Wiley.1013 All images are reprinted (adapted) with permis- are not efficient. As a low-index material and a conductor, the index
sion from the respective Journal and copyright remains with the original publisher. contrast or impedance mismatch with optical modes in free space

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FIG. 37. Experimental demonstrations of plasmonic metasurfaces enhancing the nonlinear response of TCOs. a) Plasmonic dimers on ITO show a large, fast (sub-picosecond)

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modulation of optical density when exciting antenna resonances, suggesting a strong, fast Kerr-type nonlinearity.1018 (b) A sufficiently thin, bare layer of ENZ material will sup-
port a Berreman (LR-SPP) mode with high field enhancement, but cannot easily couple to light in free space.189 (c) Nanoantennas with resonances in the ENZ region of a thin
TCO layer exhibit mode splitting from strong coupling between the metasurface and the LR-SPP mode.1016 (d) When a metasurface enables optical pumping of this LR-SPP
mode, it not only shows an enhanced nonlinear response but can also extend this nonlinear enhancement well beyond the narrow spectral range where e is near zero.184 All
images are reprinted (adapted) with permission from the respective Journal and copyright remains with the original publisher.

makes coupling light into ENZ materials difficult. For this to be a truly coupled resonance spectrum. As a result, light of high intensity expe-
useful optical component, we must overcome this challenge. riences a dramatically different refractive index compared with that
experienced by low-intensity light154 [Fig. 37(d)]. Therefore, pairing
3. Incorporating metasurfaces with ENZ materials an array of plasmonic nanoantenna with an ENZ thin film will not
only improve energy transfer to the free carriers within the material
Fortunately, metallic nanoantennas can effectively couple but can further increase the nonlinear phase shift of the metasurface
light between propagating and localized modes. If a plasmonic by its shifted resonance. Significantly, the broadening of the split res-
nanoantenna is placed on the surface of an ENZ material, the inci- onance also extends the spectral range over which a large nonlinear
dent light can efficiently couple to the local surface plasmon reso- phase shift can be achieved to be well beyond the ENZ region of the
nance and then have the fields of this resonance penetrate the TCO bare TCO material.
and excite free carriers1014 [Fig. 37(a)]. Excitation of free carriers is This synergistic interaction enables a faster, larger, and potentially
further enhanced if the ENZ material can support a Berreman more flexible nonlinear optical response from a sub-wavelength ENZ
mode, which is a Long Range Surface Plasmon Polariton (LR-SPP) metasurface than can be achieved otherwise, significantly outperform-
mode traveling in the low index medium of a sufficiently thin ENZ ing thicker layers of TCOs or even highly nonlinear bulk materials.1017
material with field enhancement inversely proportional to its thick- Having established that a metasurface not only gains a large, dynamic
ness189 [Fig. 37(b)]. In fact, plasmonic metasurfaces of appropri- optical response from incorporating an ENZ material but in fact can
ately designed nanoantennas can even exhibit strong coupling with magnify the size of this response through strong coupling to the
the LR-SPP mode of a thin film of TCO,1015,1016 which greatly LR-SPP modes, we next consider how this functionality can be put to
improves energy transfer into the TCO through near-field interac- use by metasurface design.
tion [Fig. 37(c)]. Critically, this strong coupling between modes in
the ENZ material and the nanoantenna enhances the nonlinear
4. Metasurfaces exploiting the nonlinear ENZ response
response of the metasurfaces well beyond what the bare ENZ mate-
rial could achieve: Light couples through the antenna into the ENZ Having motivated the potential of ENZ-based metamaterials for
film, changing the latter’s refractive index. This change modifies the nonlinear optics, we next consider some recent, exciting examples of
dispersion of the TCO’s LR-SPP modes, which in turn modifies the devices where this strategy has been put into practice.

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FIG. 38. Compelling results in ENZ metasurfaces: (a) dyamically changing the direction and optical frequency of light diffracting from an ENZ-metasurface is different for diffrac-
tion orders.879 (b) SHG is enhanced by a factor of 104 and is polarization selective.1019 (c) Enhanced THz generation from an ENZ-metasurface that also dictates polarization
and wavefront.1020 (d) Four wave mixing enhanced by dynamic metasurface-ENZ strong coupling.851 (e) Enhanced adiabatic frequency conversion.875 (f) Strong coupling and
dynamic modulation of a dielectric metasurface on a thin TCO layer, for both the electric or magnetic dipole Mie resonances.1021 All images are reprinted (adapted) with permis-
sion from the respective Journal and copyright remains with the original publisher.

An example of time-refraction in an ENZ metasurface was realized emission. SHG enhancement has also been demonstrated in other
in a system consisting of a plasmonic blazed diffraction grating on an ENZ-metasurface geometries, such as through gap-plasmon enhance-
ITO thin film with a pump-probe excitation. In this instance, the pump ment, based on square-shaped antennas coupled to ENZ films.1022
pulses cause the diffracted probe to undergo a change of central wave- ENZ metasurface enhancement has also been demonstrated for
length while interacting with the metasurface and therefore have the dif- other frequency conversion processes. For example, split ring resona-
fraction angle dictated by the probe’s new wavelength. Interestingly, the tors (SRRs) on ITO metasurfaces have been shown to result in orders
light diffracting into the 1 diffraction order (the order suppressed by of magnitude enhancement in the THz generation efficiency, com-
the blazing) appears to interact with the metasurface longer than light dif- pared to the same SRRs on glass,1020,1023,1024 which allows the genera-
fracting to the þ1 order. Consequently, light in the 1 diffraction order tion of single-cycle THz pulses. This enhancement can be directly
experiences about twice as much wavelength shift and thus twice as linked to the hot-electron dynamics in the ENZ film, also altering the
much change to the diffraction angle as it’s counterpart879 [Fig. 38(a)]. spectral properties of the emitted THz pulse, with spectral broadening
Both the previously demonstrated large refractive index change, being observed.1023
as well as the time refraction are demonstrations of the Kerr-type A wide range of other nonlinear processes are enhanced in such
effect, i.e., an intensity-dependent refractive index change. However, ENZ-metasurfaces, with the geometry of both the ENZ film (e.g., thin
ENZ-metasurfaces can enhance a wide range of other nonlinear effects. films featuring the LP-SPP mode vs thicker films not featuring this
For example, Deng et al. used a hexagonal array of Y-shaped nanoan- guided mode) as well as the antenna shape and dimensions together
tennas to enhance the second harmonic conversion from an ITO thin with the excitation scheme controlling the achieved nonlinear effect.
film.1019 In this work the antenna array once again overcomes the issue For example, an array of rectangular antennas on an ENZ film was
of coupling light into the ENZ film, resulting in an experimental obser- examined in a pump-probe configuration, however, with the pump at
vation of a 10 000-fold enhancement of the SHG efficiency. double the probe frequency.851 This results in a number of nonlinear
Furthermore, this work demonstrates the multi-functionality of ENZ optical processes, including four-wave-mixing and negative refraction.
metasurfaces, as the symmetry properties of the antennas are used to Furthermore, ENZ-metasurfaces retain the design freedom of linear
control the polarization of the second harmonic light. For example, the metasurfaces. For example, through rectangular antennas we can design
metasurfaces can be configured such that excitation with a right-hand the strong coupling—and hence nonlinear enhancement—to be present
circularly polarized pump results in left circularly polarized SHG for only one polarization,154,851 or through the use of antennas with a 90

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rotation symmetry, e.g., þ shaped antennas, we can obtain polarization through sub-wavelength layers and this is exacerbated by coupling
independent nonlinear enhancement.875,1025 In a polarization-dependent with plasmonic resonances. Material science research into TCOs
setting, we can use the dynamic nature of the device to obtain controlla- intends to strike a balance between strong nonlinear response and
ble polarization rotation.1026 Here for a given incident polarization featur- absorption1027 and be able to produce materials tuned for specific
ing components both parallel and perpendicular to the antenna—e.g., of applications. However, there must always be some absorption remain-
axis linear polarization or circular/elliptical polarization—the two polar- ing for TCOs, making them ineffective for most low-light sensing or
izations will experience a different delay due to their varying interaction quantum optics applications where loss management is critical.
with the metasurfaces. However, this interaction will change for the par-
allel polarization as the antenna is excited nonlinearly (and its resonance c. Saturation and damage threshold. The majority of the above
shifts), while the cross-polarization retains the same interaction as in the examples of ENZ-metasurfaces are based on gold nanoantennas. It is
linear case. We thus have the ability to control the delay of one polariza- well known1028 that many metallic nanostructures and gold particles
tion component relative to the other. in particular, are very sensitive to absorption-induced heating and
While ENZ-metasurfaces based on plasmonic nanoantennas are melting, with the melting point significantly lower than for the bulk
used in the majority of nonlinear optical investigation efforts at this metal. However, more thermally robust materials such as TiN have
time, it is important to also consider how other nano-resonances could higher absorption losses. This therefore presents an interesting
be integrated with ENZs as well. Dielectric metasurfaces and their cor- research area, where materials and antenna design can be optimized to
responding Mie resonances do not provide the same field enhance- allow higher optical powers and operating temperatures. This low
ment in the TCO by the simple fact that their mode volumes lie damage threshold, together with the increased design freedom of the
principally within the dielectric material of the resonator rather than at ENZ metasurfaces means that nonlinear saturation effects have not yet
the edges. Nevertheless, experiments have shown strong coupling been studied extensively in these systems.
between an LR-SPP mode and either electric or magnetic dipole reso-
nances,1021 as well as confirming that these resonances can be optically d. Alternative modulation mechanisms. In this paper we have
tuned in a pump-probe set-up with sub-picosecond recovery time. Just focused on the ultra-fast, all-optical response of ENZ metasurfaces.
as with plasmonic metasurfaces, strong coupling between the Mie reso- However, the underlying tuning mechanism is much more general. We
nances and the ENZ mode of a TCO thin-film appears to enable large, recall that the mechanism is based on a shift of the ENZ dispersion,
rapidly tunable modulations of the optical modes and should thus induced by a change in the free carrier properties. Such changes can be
induced in an alternative fashion, for example through electro-optic

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facilitate a broad range of dynamic, nonlinear optical responses.
It is evident from these examples that ENZ-metasurfaces enable modulation1029,1030 or thermo-optic tuning,1031 creating the potential for
strong and fast nonlinear optical responses while still maintaining the dynamically reconfigurable metasurfaces. Here we note that the sign of
tremendous design freedom available to metasurfaces. There is a sig- the nonlinear response can differ compared to the hot-electron nonli-
nificant opportunity for devices that rapidly manipulate the phase, nearities discussed earlier, as some of these tuning mechanisms, can
direction, polarization, and even mode of propagating light, all within include interband transitions, or extraction or addition of carriers, hence
flat, sub-wavelength structures. allowing either a blue or redshift of the plasma frequency.

5. Future of applications e. Pushing back technical limits. Given the unprecedented large
changes of refractive index observed in ENZ-metamaterials, a natural
Going forward, there are still several outstanding research questions question is how much further such devices be engineered before reach-
that need to be addressed for the nonlinear response of ENZ materials in ing a new limit? Some examples still needing exploration include, can
general and optimizing the potential of ENZ-metasurfaces in particular. an ENZ-metamaterial be engineered to produce a rapidly modulating
nonlinear phase shift of D/ ¼ p2? In the electro-optic modulation
a. Speed of modulation. For the experiments presented here, the scheme, this full phase shift has been achieved, however, at the cost of
nonlinear optical response of the ENZ-metasurfaces is clearly faster a highly reduced efficiency1030 and limited to the tuning speed of the
than the short (sub picosecond) pump pulses can resolve. Knowing it control electronics. Reaching the D/ ¼ p2 limit all-optically would
can be faster than 100 fs supports the working understanding that make it possible to create a sub-wavelength, THz-speed switch.
rapid heating and intraband transitions of the free carriers are driving In adiabatic frequency conversion work, it’s been shown that
the index changes in the TCO. However, a more direct investigation large changes of the carrier frequency can be achieved in TCOs1011
into the onset time of this response, how it saturates, the thermaliza- and that plasmonic metasurfaces can manipulate this response more
tion time as well as how each of these is affected by coupling to plas- efficientl.875,879 However, in time refraction the fractional wavelength
monic nanoantennas could provide insight into devices that modulate shift is proportional to the refractive index change witnessed by the
at rates beyond GHz. The speed and magnitude of the nonlinear phase photons, which so far has been far less than the full index shift of the
shifts are likely large enough to enable non-adiabatic transitions, which TCO (Dn 1:0). If ENZ-metasurfaces could be designed to increase
could have significant implications for applications in which mode this interaction time, it should in principle be possible to shift the car-
degeneracy or spectrum engineering are important. rier frequency of light by an octave.

b. Absorptive losses. While the imaginary component of TCOs B. Perspective on future work
refractive indices are typically smaller than for properly conductive We can imagine that ENZ metasurfaces could be designed for a
materials,996 there is still a significant amount of absorptive loss seen much wider set of nonlinear interactions. For example, some of the

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most widely used interactions in commercial devices featuring nonlin- Deep learning (DL) is a specific type of artificial intelligence
ear optics are the sum and difference frequency generation in optical and has recently garnered tremendous attention within science and
parametric amplifiers and oscillators. Similarly, the field of attosecond engineering, including for the design and study of photonic meta-
science relies on efficient high-harmonic generation. As ENZ metasurfaces surfaces. However, there is a tendency to overvalue the current
have shown enhancement of second harmonic light it would be a natural capabilities of DL, often attributing powerful reasoning skills to it.
next step to investigate and extend this to higher nonlinear orders. Here we aim to clarify the current strength of DL methods for pho-
Furthermore, the broad response of ENZ metasurfaces could also be of tonic metasurface research and development. We highlight two
interest to other processes such as supercontinuum generation and cas- major successful use-cases. First, DL has been highly effective at
caded nonlinearities. However, these applications typically require nonlin- automatically constructing models that accurately predict the
ear interactions over an extended propagation length. How this could be properties of complex metasurfaces based upon their experimental
replicated in a metasurface geometry requires further research. parameters (e.g., geometric structure, or illumination).
As the combination of metasurface resonances with TCO thin Additionally, DL models has been used to build accurate models
films shows such potential, a natural next question is what functional- allowing users to predict the experimental parameters needed to
ity can arise from patterning the metasurface directly into the TCO yield some desired behavior, significantly accelerating metasurface
thin film itself? Initial investigations suggest sufficiently good coupling design. Despite these successes it is important to recognize that DL
and field enhancement to produce significant nonlinear optical effects primarily serves as a collection of advanced regression methods,
and non-reciprocal radiation patterns,1032 so further experimentation which represent a relatively rudimentary form of intelligence com-
could be fruitful. pared to, for example, human scientists. The fundamentally limited
The majority of the nonlinear optical work on ENZ metasurfaces reasoning capabilities of DL manifest as key practical limitations
has been performed in the near-infrared (1100–2000 nm) spectral that undermine its current value and impact, such as DL’s need for
region. Naturally, these same effects hold promise for other pump large quantities of training data, and their limited generalization to
wavelength regions, such as visible light, but also mid-infrared through new scenarios that were not represented in training data. We dis-
to THz spectral regions. Implementing these effects across different cuss several promising acute and long-term strategies for address-
wavelength regimes will likely require different ENZ materials or at ing these limitations, which may ultimately lead to DL models that
least wide tuning of the ENZ wavelength. fulfill more of their current promise.
Perhaps most intriguing, the field of photonic metasurfaces is

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rapidly becoming more sophisticated, as is readily demonstrated by A. Introduction
this roadmap. As new materials, resonance structures and metasurface Photonic metasurfaces have demonstrated great utility as a mate-
principles are being introduced, there are opportunities to investigate rials platform for the demonstration of numerous exotic electromag-
each of their interactions with ENZ thin films. For instance, incorpo- netic (EM) phenomena in both applied1033 and fundamental1034–1036
rating bound states in the continuum, disordered metasurfaces or settings. A common objective of photonic metasurfaces is to tailor
active emitters with ENZ thin films could demonstrate the enhance- the EM field to achieve a desired configuration which may consti-
ment or quenching of various light–matter interactions. tute various forms, including free-space scattered states, surface
wave conditions,1037 or localized field concentrations.682 Moreover,
C. Conclusion metasurfaces enable this control over diverse dimensions of
In this perspective, we have summarized the physics governing space,1038 time,1039 and frequency.1040 Although design constraints
nonlinear optical interactions in ENZ metasurfaces, consisting of including material choice, physical restrictions, and operational
antenna arrays coupled to thin films of ENZ materials. The strong cou- environmental limitations are unavoidable, there is otherwise great
pling results in huge nonlinear enhancements, exceeding the perturba- design flexibility in the type of photonic metasurface utilized. This
tive regime, on sub-picosecond timescales. We then highlighted some rich history of EM design, evolving through distinct theoretical,
recent key contributions to this rapidly growing field, well aware that computational, and now artificial intelligence (AI)-driven eras,
an even broader body of work exists. Considering the potential future informs our understanding of the interplay between design free-
dom and practical limitations in photonic metasurfaces, opening
directions for this field and identifying opportunities across physics,
new avenues for exploration and optimization.
engineering, and materials science, there is clearly a strong potential
In stark contrast to the vast EM design tools available today, at
for novel nonlinear optical applications. In effect, almost any applica-
the end of the 19th century scientists relied on manual calculations to
tion based on the mentioned nonlinear processes could benefit from
perform EM analysis1041 using the newly established Maxwell equa-
the enhancement in ENZ metasurfaces. Finally, as there remains an
tions of 1864 (Ref. 1042) and the refined set in 1873.1043 The initial
even wider set of nonlinear optical interactions to which ENZ metasur-
focus was on finding closed form solutions to Maxwell’s equations
faces have not yet been applied, we leave them as an exercise to the
and by 1910 there were a dozen or so including those of
reader to make their own mark on this exciting and growing field.
Sommerfeld,1044,1045 Lord Rayleigh,1046 Mie,1047 Hondros,1048
XVIII. DEEP LEARNING FOR PHOTONIC Nicholson,1049 Debye,1050 and Hondros and Debye.1051 During the
METASURFACES first half of the 20th century more complex EM problems were solved
by generalization of these explicit solutions. EM problems involving
Willie J. Padilla and Jordan M. Malof Sommerfeld integrals were more challenging to solve and benefited
from the development of asymptotic methods including stationary

[Link]@[Link] phase and the method of steepest descent. Perturbation and

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available including full-wave approaches based on either integral equa-

tions (both time and frequency domain) or on differential equations
(both time and frequency domain), or alternatively high frequency
methods based on either EM fields (geometrical optics) or currents
(physical optics). With modern commercial software, programs can be
created much faster, and a single program can be used to collect data
over a wide variety of physical settings.
The last decade has witnessed the emergence of deep learning
FIG. 39. Illustration depicting a conventional scientific workflow wherein a human (DL), which has received significant attention in the literature. In the
scientist acts as a reasoning engine, denoted (b); in this capacity, a scientist synthe- modern academic milieu, it is reasonable to ask whether this attention
sizes empirical data, denoted (a), and existing scientific knowledge, in the form of
models/theory, denoted (c), to develop novel scientific models, or perform design of is justified. To address this question, it is helpful to understand the fun-
physical systems, denoted (d). In many modern branches of science, empirical data damental role of DL in the EM scientific workflow: for example, how
are often collected through both physical experiment and electromagnetic (EM) sim- does DL relate to CEMS, human scientists, and the theoretical models
ulations. The promise of deep learning is to automate the process of reasoning that they develop? DL is a specific type of artificial intelligence (AI) tech-
is currently fulfilled by humans; however the reasoning capabilities of deep learning nique, and the long-term objective of AI is to enable machines to
are currently far more limited. Note that, in general, the relationships between these
components can be more complex than indicated here. achieve human-like intelligence.1056 In this regard DL occupies the
same role in the scientific process as human scientists, which is to rea-
son about empirical observation and existing knowledge (e.g., theory
approximation methods were also developed to solve more complex and models) to develop new knowledge, or to perform EM material or
problems, and these are generally termed high frequency methods, to device design. This broad scientific workflow is illustrated in Fig. 39.
which geometrical and physical optics belongs.1052 The prospect of automating the role of humans—or even enhancing
A key component of scientific inquiry is empirical observation, or it—using machines is enticing, and understandably garners tremen-
data, which is crucial to guide theoretical investigations, and ultimately dous attention.
to validate them. Prior to the advent of computational EM solvers While DL represents an important step toward automated reason-
(CEMS), the primary means to collect data were the construction of ing, at present, DL methods are quite limited in their reasoning capabil-
physical experiments, which was relatively slow and costly, severely ities. In their current form, the term “Deep Learning” most often refers

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limiting progress. The computational era began in the 1940s with the to a collection of machine learning (ML) methods—namely, deep neu-
development of the computer, but it was not until the 1960s, when var- ral networks (DNNs)—which are broadly designed construct models
ious numerical methods emerged to solve Maxwell’s equations, that that approximate the relationships present in observed data, e.g.,
the field really gained momentum. The CEMS developed were those of CEMS.1057,1058 This capability is illustrated and described in Fig. 40. DL
the finite-difference time-domain (FDTD) method,1053 the method of does, therefore, automate an important reasoning task that has histori-
moments (MOM),1054 and the finite element method (FEM).1055 In cally been accomplished by human scientists—building models of the
contrast to physical experiment, these approaches essentially allowed physical world from data. However, DNNs do not efficiently integrate
scientists to conduct experiments by writing and executing software, knowledge of the physical world, or perform deductive reasoning.
which is generally much faster and cheaper. Nonetheless, DL does present a significant advance over prior machine
The evolution of CEMS has continued in earnest, and in the past learning approaches in nanophotonic metasurfaces and has enabled
few decades, we have witnessed the emergence of many accurate and the analysis of far more complex materials than previously possi-
efficient options. Today, we have commercial computational EM tools ble,1059–1062 justifying some of the attention they have received.
Figure 40 depicts the current state of EM design approaches,
including (a) theory, (b) computational EMs (simulation), and (c) deep
learning. A theoretical approach strives to represent observations math-
ematically, aiming for closed-form solutions or, less favorably, accurate
approximations. In EMs, Maxwell’s equations are derived from the
experimental observations of Faraday, Ampere, Ørsted, Gauss, and
others, and verify the soundness of this method. We depict this theoret-
ical approach in Fig. 40(a) where the open green symbols are points of
observations which have given rise to the exact theory, y ¼ f ðxÞ, repre-
sented by the solid red curve. We next consider an EM design problem
FIG. 40. Illustration depicting the relationship between DL, theoretical findings, and
where the theory is not known, i.e., no exact solution exists. This may
experimental results (e.g., CEMS). Given some EM system we often have experi- arise due to the complexity of the problem or the incorporation of
mental parameters x, and observed experimental results y. (a) The true relationship some newly discovered material. Although no exact solution to our
underlying these data (red curve), denoted y ¼ f ðxÞ, can sometimes be uncovered problem exists, CEMS, which are based on Maxwell’s equations, are
via observation (open green symbols) and theoretical deduction. (b) Physical experi- able to model the problem accurately and we are able to determine f(x)
ments and CEMS (open black squares) can be used to sample this function, provid- at some discrete values, shown as the black squares in Fig. 40(b).
ing pairs of data (x, y) for specific settings of x. (c) Deep learning methods can
utilize empirical data (open black squares) to automatically construct models, However, since CEMS are limited by computer memory and calcula-
denoted ^f and shown as the dashed blue curve, that accurately approximate the tion time, the problem is usually restricted to some range, denoted by
true underlying relationships (solid red curve) over the domain of available data. xm in Fig. 40(b). The deep learning approach to EM design permits the

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denoted h and they influence the relationship between the input to the
DNN and its output, so that ^f h can be made to accurately approximate
a wide variety of complex functions depending upon the settings of h.
To approximate a forward function, DNNs assume the availability of
N empirical observations of the form D ¼ ðxi ; yi ÞNi¼1 , which is typically
procured by CEMS in EM applications, and where N may vary sub-
stantially across applications. The DNN is then “trained” to approxi-
FIG. 41. Illustration of forward modeling (bottom) and inverse modeling (top) illus- mate the relationship between x and y by iteratively adjusting the
trated using a metasurface comprised of repeating 2 2 supercells of cylindrical parameters h in a way that tends to shrink the error between predic-
resonators. Each resonator in the supercell has an adjustable geometric structure, tions made by the DNN, denoted ^y ¼ ^f ðxÞ and the true setting of y
denoted x in the main text. In forward modeling we build some mathematical model associated with the input setting provided to the DNN, x. In other
or algorithm, denoted ^f , for computing the behavior of the system, denoted y, given words, ^f ðxi Þ yi for most of the xi 2 D. Given a large enough DNN
some setting of x. One widely used method for forward modeling is computational
simulation, however, in some cases we can dramatically accelerate forward model- (i.e., enough adjustable parameters), it has been shown that a DNN
ing using a neural network. Using this acceleration, one can perform design by rap- can approximate any underlying function to an arbitrary degree of
idly evaluating ^y ¼ ^f ðxÞ for different candidate settings of x, and then comparing ^y accuracy.1066,1067 In practice however, the accuracy of the model
to a desired system behavior, denoted y . In inverse modeling we build a model, obtained may vary depending upon many factors (e.g., the available
termed ^g , that can predict a setting of x that would yield a desired set of properties, training data, N, or the complexity of the true underlying function that
denoted y . Deep Inverse Models are a class of DNNs that have been shown capa- we wish to approximate).
ble of directly making accurate inverse predictions ^x for complex metasurfaces.
Once the model ^f is constructed, it can be used to make accurate
predictions for settings of x that were not present in D. This process is
determination of a surrogate model from data (often CEMS data), essentially regression analysis, for which there are many techniques.
denoted ^f ðxÞ which approximates the true function f(x). In Fig. 40(c) However, in contrast to previous approaches, DL has been demon-
the open black symbols represent the same x points used in (b) for sim- strated to often produce much more accurate approximations for chal-
ulation, but now they are used in the deep learning workflow to deter- lenging high-dimensional systems that exhibit complex (e.g., highly
mine the surrogate function ^f , represented by the dashed blue curve. non-linear) relationships between x and y. Furthermore, and crucially,
The surrogate function ^f ðxÞ is significantly faster to evaluate than per- DL models have been shown in some cases to make predictions for
novel settings of x at a speed that is several orders of magnitude faster

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forming CEMS. Past results have demonstrated that one evaluation of
^f ðxÞ compared to one numerical simulation is nearly 106 times faster. than CEMS, e.g., by a factor of nearly 106. Therefore, using ^f ðxÞ, it is
Next we discuss in greater detail where DL has been successful in possible to rapidly explore the behavior of the system under study,
which can aid scientists with theoretical investigations.
EM materials, and the roadmap for realizing the greater potential for
In addition to scientific investigation, forward modeling can also
DL to automate human reasoning.
be used to accelerate design. In contrast to modeling, the process of
design involves the manipulation of experimental parameters to
1. State of the art achieve a certain system behavior. In other words, we wish to find
Where is deep learning currently most successful? Although some setting of x that will result in a particular desired setting of y. A
DL has been applied for a variety of purposes in EM materials, its pri- common design strategy involves using a forward model to evaluate
mary success has been as an instrument to dramatically accelerate for- different candidate settings of x until one is found that produces the
ward and inverse modeling. The goal of forward modeling is to desired behavior. For advanced materials CEMS is often the only avail-
uncover some, yet unknown, mathematical relationship of the form able means of evaluating the properties of arbitrary settings of x.
y ¼ f ðxÞ, that relates the parameters of an experiment, denoted x, to CEMS is often computationally expensive however, creating a major
the corresponding measurements obtained from that experiment, bottleneck to design. In such cases DL can be utilized to build a fast
denoted y. In the context of metasurfaces, x might quantify parameters
such as a metasurface geometry (e.g., radii and height of cylinders), its TABLE I. A list of three major components for construction of a deep neural network:
bulk construction material, or the illumination of the material; simi- Data, Architecture, and Loss. The NN architectures shown are some of the most
larly, the observations encoded in y might include electric/magnetic commonly employed in photonic metasurfaces and include: residual neural network
field measurements, or absorption,1063 reflection,1064 transmission1065 (RNN), convolutional neural network (CNN), multi-layer perceptron (MLP), graph neu-
ral network (GNN). Here the Transformer is a broad class of neural networks with
spectra, measured at a specific frequencies. On the other hand, the goal similar applicability as MLPs, and Generative Models are NNs that can be trained to
of inverse modeling is to construct some model of the form x ¼ ^g ðyÞ, create novel instances of data that resemble those from some collection of data.
wherein we can provide some desired experimental observation, and
then have the model efficiently produce the experimental parameters Data Architecture Loss function
that would give rise to those observations. These two basic objectives
are illustrated in Fig. 41. We next explain how forward and inverse Experiments RNNs Error metric, e.g. MSE
modeling have been utilized EM metasurfaces, to important effect. Simulations CNNs Differential equation
Forward modeling. DL accelerates forward modeling by auto- FCNs Algebraic equation
mating the process of uncovering f from observational data. In practice GNNs Complexity penalties
DL is usually implemented with some type of DNN which is essentially Transformers
a parameterized function, denoted ^f h . The parameters of the DNN are

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TABLE II. Examples of specialized DNN approaches to perform inverse modeling, often for the purpose of design.

Model Type Applications to AEM problems

Tandem (TD) Deterministic Liu et al.,522 Ma et al.,1068 Gao et al.,1069 and Hou et al.1070
So et al.,1071 Long et al.,1072 He et al.,1073 and Xu et al.1074
Ashalley et al.,1075 Mall et al.,1076 and Pilozzi et al.1077
Phan et al.,1078 Singh et al.,1079 and Malkiel et al.1080
Mixture Manifold Networks (MMN) Deterministic Spell et al.1081
Genetic Algorithm (GA) Optimization Zhang et al., Johnson and Rahmat-Samii,1082 and Deng et al.1061
312

Forestiere et al.1083 and Li et al.1084

Neural Adjoint (NA) Optimization Deng et al.1085 and Peurifoy et al.1086
Asano et al.678 and Miyatake et al.1087
Variational Auto-encoder (VAE) Probabilistic Ma et al.,1088,1089 Qiu et al.,1090 and Kudyshev et al.1091,1092
Shi et al.,1093 Liu et al.,1094 and Kiarashinejad et al.1095
Mixture Density Network (MDN) Probabilistic Unni et al.1096,1097
Invertible Neural Networks (INN) Probabilistic Ren et al.1098
Generative Adversarial Networks (GAN) Probabilistic Wen et al.1099

approximation to f, permitting a more efficient and effective design. successfully to rapidly identify designs that achieve customized settings
Consequently, DL represents a powerful tool to accelerate this type of of y , and do so for highly complex EM material systems.1098,1105
forward design procedure.1100 There are various DIMs which have been applied to photonic
State-of-the-art DL most often takes the form of DNNs, which metasurfaces and in Table II we list some of these models, their type,
have a large number of free design choices, sometimes called and references to associated studies. DIMs fall into three basic

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hyperparameters, that must be chosen to suit the particular system categories—namely Deterministic, Optimization, and Probabilistic.
under study. Some of the most important choices are the data uti- Broadly, each class of model represents a trade-off between computa-
lized for training, the model architecture (i.e., what functional form tional cost (e.g., speed) and design accuracy. Optimization approaches
does ^f or ^g take), and the loss function(i.e., what criteria is used to initialize a large population of randomly chosen candidate solutions
identify the “best” model during training). Fortunately, there are a and then sequentially improve all of them in parallel—a computation-
number of highly effective choices for these hyperparameters ally intensive process, but one that often achieves the highest design
depending upon properties of the problem, of which some are accuracies. Like Optimization methods, Probabilistic DIMs typically
listed in Table I. The number of neural network hyperparameters is initialize a large set of candidate solutions, but rather than incremen-
vast and we do not attempt to include an exhaustive list here. For tally optimizing them, they try to make the quality of these initial esti-
the reader interested in learning more we refer to reviews on these mates higher by learning a probability distribution of where good
topics.1101–1104 solutions are likely to exist, given some target y . These approaches are
Inverse modeling. Despite the acceleration provided by DL, the relatively fast because they avoid sequential processing, but they typi-
forward design procedure can quickly become intractable for advanced cally yield less-accurate solutions because their solutions are still ran-
photonic metasurfaces with many free design parameters (e.g., x is domly drawn. Deterministic methods attempt to learn a direct
high-dimensional), or the number of candidate settings for each design mapping from y to the appropriate design that will yield y .
parameter is large. Another powerful capability of DNNs is so-called Consequently these approaches require just one evaluation of a DNN
inverse modeling, whereby a DNN utilizes data to build a model of the (e.g., for Tandem), or just a few evaluations in parallel (e.g., MMN),
form x ¼ ^g ðyÞ with the property that f ð^g ðyÞÞ ¼ y; in other words, the making them computationally fast. There are also hybrid methods that
DNN approximates the inverse of f. In principle then, a scientist can combine different types of DIMs, or combine DIMs with traditional
specify a precise set of desired EM properties, denoted y , and the optimization approaches (see review in Deng et al.1061) Further infor-
DNN will produce the design that will yield those desired properties— mation about DIMs for photonic metasurfaces can be found in recent
a transformative capability depicted in the top path of Fig. 41. This reviews of the topic.177,1098,1106
approach essentially uses DL for regression, similar to modeling and
forward design, except with the roles of x and y reversed. However, 2. Future directions and outlook
this reversal of roles introduces some significant technical difficulties
for regression, such as the so-called non-uniqueness problem, where Although DL has become a powerful tool to accelerate EM
several different settings of x can produce the same desired setting of modeling and design, the long-term potential of DL is far greater. The
y . Non-uniqueness causes conventional DL methods to fail, however, future promise of DL, and AI more broadly, is to enhance and auto-
substantial recent work has focused upon specialized DL models— mate the role of human reasoning within the scientific process, as
termed deep inverse models (DIMs)—that can overcome these chal- shown in Fig. 39. Currently however the reasoning capabilities of the
lenges. Recent studies have demonstrated that DIMs can be trained most successful DL approaches—namely DNNs—are relatively limited

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compared to humans. Although there are several limitations of DNNs example, so-called physics-informed neural networks (PINNs)
compared to humans, we highlight two specific limitations that are encourage any DL model to be consistent with Maxwell’s
especially influential: (i) world modeling, and (ii) deductive reasoning. equations.1109
World modeling refers here to the ability of an intelligent agent • Transfer and incremental learning: These approaches attempt to
(e.g., a DNN) to represent and utilize knowledge of objects in the build upon knowledge gained from one problem—perhaps a
world, and their known relationships (e.g., physical laws), when rea- problem with substantial quantities of data—and leverage it to
soning. For example, if we wish to build a model relating the position aid the construction of a model for a new problem. Transfer
of a vehicle on a road, y, as a function of time, x, it is helpful to know learning is widely used in the broader DL community, and it has
that the vehicle is powered by a combustion engine, thereby limiting also recently been shown to dramatically reduce the quantity of
its maximum speed and rates of acceleration. This knowledge immedi- data needed to solve novel metasurface problems as well.1110,1111
ately and dramatically reduces the number of potential explanatory • Active learning: These approaches attempt to identify data points
models, yet building a DNN that can represent and utilize such infor- that are most “informative,” in the sense that the model can
mation when training (i.e., building a model) still requires substantial improve its accuracy faster, and thereby use less total training
time of a human expert, and often still doesn’t fully leverage this infor- data.1112
mation. Consequently DNNs often lack world models altogether, or • Modeling ill-posed problems: This research area is unique to
they are simplistic and limited in scope. inverse modeling, where non-uniqueness is a major obstacle to
Deductive reasoning refers here to the ability of an intelligent building inverse models. This is an active and important area of
agent to use existing knowledge to draw valid conclusions about the research for ultimately building effective deep inverse models.1098
world via logic. In the context of physics, deductive reasoning might
Long-term research directions. Long-term DL research should
include, for example, the use of mathematics to deduce closed-form
aim to endow DL methods with more sophisticated reasoning capabili-
solutions to Maxwell’s equations under specific conditions. Another
ties, such as general World Modeling and Deduction. Achieving these
example may be that field measurements from a EM material must
goals represents a tremendous challenge; however, some progress is
obey Maxwell’s equations, and therefore any exact model of the system
being made within the AI research community. Here we list three
[e.g., of the form y ¼ f ðxÞ] must also obey Maxwell’s equations.
promising areas of current research that may endow DL with these
Although DNNs sometimes incorporate the results of human deduc-
two more sophisticated reasoning capabilities.
tive reasoning (e.g., so-called physics-informed neural networks, or
Lorentzian Neural Networks) they do not explicitly perform deductive • Large language models (LLMs):1113,1114 LLMs have recently dem-

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reasoning. Like world modeling, deductive reasoning can be used to onstrated the capability of representing human language, and
dramatically reduce the number of valid models of observed data, and using it to perform some basic reasoning. If successful, LLMs rep-
also ensure certain levels of generality. resent one way to provide DNNs with knowledge about physical
Near-term research directions. The most acute consequence of systems, and potentially perform deductive reasoning.
DNN’s limited reasoning capabilities is that it limits their generaliza- • Neuro-symbolic models:1115–1117 These approaches attempt to
tion capabilities; that is, their ability to make inferences (e.g., predic- combine the existing capabilities of DNNs (e.g., data-driven mod-
tions) for scenarios (e.g., inputs) that were not present in their training els) with powerful existing symbolic reasoning engines, thereby
data. Consequently, DNNs typically require substantial quantities of providing DNNs with the capability to apply deductive
training data to build accurate models, which is problematic because reasoning.
these data are typically generated by expensive and/or time-consuming • Causal models1118,1119 These approaches attempt to use deductive
CEMS, and it must be generated independently for each unique prob- reasoning to help DNNs to distinguish between spurious correla-
lem (i.e., physical system) under consideration. Furthermore, the tions and causal relationships present in data.
quantity of data required to achieve a particular level of modeling
accuracy grows rapidly with respect to the complexity of the problem Although we highlight these areas of DL research, it is notewor-
under consideration (e.g., the dimensionality of x and y, and the non- thy that there are many important active areas of DL research (e.g.,
linearity of f).1107 At the same time, CEMS is also often more computa- interpretability)
tionally intensive for such problems, limiting the quantity of data that Outlook. Since its emergence roughly a decade ago, DL has had a
can be obtained. Therefore, data inefficiency represents a major limita- significant impact on many fields, including EM metasurfaces. Among
tion of DL, undermining its value even in applications where it has their successes, DNNs have been especially useful for utilizing empiri-
been highly successful. Importantly it also makes DL completely cal data (in particular from CEMS) to build computationally efficient
impracticable for many important open problems in EM, such as those approximate models that can dramatically accelerate the modeling and
involving multi-physics or multi-scale problems.1108 A variety of design of complex photonic metasurfaces. The capabilities of DNNs
research is under way to improve the data efficiency of DNNs. These are quite robust for these tasks, and they have quickly become perva-
approaches are relatively superficial, in the sense that they do not sig- sive within the EM research community. Consequently, we expect DL,
nificantly improve fundamental reasoning capabilities of DNNs, but serving in this capacity, to become an important tool for modeling and
they are also often more tractable, and have demonstrated some design of EM materials, alongside other tools such as theory and
CEMS. Despite their impact however, DL represents a relatively rudi-
effectiveness:
mentary form of reasoning about empirical data. The long-term poten-
• Physics-guided learning: These approaches try to utilize known tial of DL, insofar as it is an AI technique, is tremendous. The long-
physical laws or principles to guide the interpretation of empiri- term objective of AI is endow machines with human-level intelligence.
cal data, ultimately reducing the amount of data needed. For Currently, DL fundamentally lacks important reasoning capabilities of

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humans, for example, explicit world modeling and deductive reason- Optical singularities are points at which a physical quantity, such
ing. If DL or other AI techniques can be endowed with these more as the phase, polarization, polarization ellipticity, etc., is not defined,
sophisticated forms of reasoning, it may result in much greater advan- but around which this same physical quantity can take almost any
ces than has yet been provided by DL. Furthermore, DL possesses value. This latter property is very beneficial for designing photonic
some advantages over humans; specifically, DL possesses substantially devices with desired optical response. Moreover, singularities are ubiq-
greater computation speed and memory capacity. Consequently, upon uitous in nanophotonics as they generically occur when varying at least
possession of human-like reasoning capabilities, it may also dramati- two optical or geometrical parameters of the system. Here, we present
cally accelerate the rate at which such reasoning is done, considerably approaches to design nanophotonic building blocks with desired opti-
accelerating science. Although it is unclear how quickly DL and AI will cal responses via singularity position engineering. In particular, we
progress, important inroads have been made toward tackling some of show that the control of the positions of zeros and poles of optical
the aforementioned reasoning limitations it possesses (e.g., with LLMs, response functions (e.g., reflection, transmission coefficient or scatter-
and neuro-symbolic models). Given the tremendous potential impact ing, and Jones matrices), the so-called singularities, can be used to
of advances in AI, and the commensurate investment in its develop- design optical metasurfaces with desired amplitude and phase behav-
ment, we anticipate that it will be an increasingly important area of iors. Additionally, breaking the in-plane symmetries of the metasurface
research within EM metasurfaces. is shown to achieve a phase singularity for only one circular polariza-
tion state, while its orthogonal counterpart remains unmodulated,
ACKNOWLEDGMENTS thereby opening new avenues for the information multiplexing with
nanophotonic designs. Sharing similarities and inspiration from estab-
W.J.P. and J.M.M. acknowledge support from the Department lished works in signal processing and control theory, it is expected that
of Energy under U.S. Department of Energy (DOE) (No. the control of the position of complex-valued singularities in the “pole-
DESC0014372). zero complex-plane,” for example relying on symmetries, would pro-
vide new design methodologies in photonics.
XIX. COMPLEX-VALUED SINGULARITIES FOR
METASURFACE DESIGNS
A. Introduction
mi Colom, Qinghua Song,
Aloke Jana, Zijin Yang, Re Optical singularities refer to points or regions, either in the physi-
and Patrice Genevet cal or parameter space, where certain optical or electromagnetic prop-

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erties become undefined within the vicinity of steep gradients, as
[Link]@[Link] illustrated in Fig. 42. In ray optics, singularities manifest as points or

FIG. 42. Optical singularities and their topological features. (a) Depiction of a catacaustic formed by a circle with the source positioned on the circle. (b) Vortex beam associated
with the phase singularity of the complex scalar wave, (c) polarization singularity of the vector beam, (d) optical skyrmion lattice, (e) exceptional points: depiction of the topologi-
cal features of non-Hermitian systems linked with the degeneracy of the eigenvalue spectrum. Inset illustrates the real and imaginary parts of the eigenvalue spectrum in the
parametric space. (f) Scattering singularities featuring a zero-pole pair of the complex reflection/transmission coefficients. Inset displays the phase profile of reflection/transmis-
sion coefficients, along with a simple illustration of the reflection/transmission zero condition of the scattering processes. Figure (a) reproduced with permission from
“Catacaustics, Resultants and Kissing Conics — Greg Egan,” [Link] (2012). Copyright Author(s);1153 (c) repro-
duced with permission from Copyright Hindawi Publishing Corporation;1129 (d) reproduced with permission from Tsesses et al., Science 361, 993 (2018). Copyright 2018
AAAS;1130 (e) reproduced with permission from Miri and Alu, Science 363, eaar7709 (2019). Copyright 2019 AAAS;39 (e) reproduced with permission from Ozdemir et al., Nat.
Mater. 18, 783 (2019). Copyright 2019 Nature Publishing Group;1136 and (f) reproduced with permission from Colom et al., Laser and Photonics Rev. 17(6), 2200976 (2023).
Copyright 2023 Wiley-VCH.1154 Copyright remains with the respective publishers.

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lines of extreme light intensity (caustics) known as optical catastro- reflection or transmission coefficients in the complex-frequency plane.
phes. Meanwhile, phase singularities can be found in complex scalar Phase singularities of these coefficients such as zeros and poles play a
wave fields as a form of vortices, wavefront dislocation, or nodal fundamental role. In addition to the position of single zeros, two or
lines.1120–1124 This ensemble of phenomena belongs to the realm of more of these quantities can merge in the complex plane, potentially
Singular optics. One very familiar example of a singular optics phe- exhibiting EP behavior. This characteristic also holds true for the con-
nomenon is the existence of Laguerre Gaussian beams having zero ventional Jones matrix, which describes changes in the polarization
intensity lines along the optical axis and a helical phase front associated state between input and output channels. Therefore, the non-hermicity
with an intrinsic orbital angular momentum.1125–1127 Incorporating of the scattering/Jones matrices provides a ubiquitous tool to control
the vector nature of EM waves gives rise to additional polarization sin- and manipulate the properties of EM waves. By tuning the geometry
gularities.1128 These polarization singularities can manifest as singulari- and changing the composition of the individual unit cells, anomalous
ties in one or more parameters of the polarization ellipse, such as the light propagation or scattering effect, including unidirectional propa-
azimuthal angle and ellipticity angle, resulting in features like C points gation, polarization and diffraction control, maximum helical dichro-
and L lines.1129 Skyrmions are the stable topological defects of the ism, ultrasensitive sensing and biosensors, imaging, and surface waves,
three-dimensional vector field that exhibit promising applications in can be studied.5,880,1140–1151 Interestingly, even the most basic zeros of
the domain of magnetic storage and spintronics. Similar possibilities, the system response functions, such as the complex reflection/trans-
i.e., optical information, transfer, and storage arise in the realm of the mission function, also exhibit phaseÞ singularities associated with non-
photonic system by utilizing the topological properties of three- trivial topological charge of C ¼ 2p 1
c $ð/Þdx, where / is the response
dimensional EM waves.1130 Over the decades, singularities in optical phase function and the integration is carried out along a path c enclos-
systems have been studied extensively in different scenarios starting ing the singular zero response point in two-dimensional parameter
from the seminal work “Dislocation in wave trains” by Berry and Ney space. It turns out that the latter reflection and transmission zeros play
to “Observation of the optical mobius strips.”1123,1131–1135 In addition, a leading, and often neglected, role in the design of photonic systems,
recent advancements of spectral singularities associated with non- including MSs.1152
Hermitian systems have led down to fertile ground, revolutionizing This roadmap article focuses on these recent developments,
various fundamental and technological aspects.39,1136–1139 It’s well drawing some of the perspectives and implications offered by the
known that a closed and conservative system governed by Hermitian complex-valued zeros and EPs singularities of transfer functions for
Hamiltonian exhibits real eigenvalues with orthogonal eigenvectors the design of innovative photonic systems. This manuscript is orga-
nized into three sections. In Sec. XIX C, we begin by introducing the

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due to its unitary evolution nature. Instead, open and non-
conservative systems, described by non-Hermitian Hamiltonians, basic notion of zeros in electromagnetic quantities and elucidate the
exhibit complex eigenvalues and non-orthogonal eigenvectors. Non- impact of the position of singularities in the complex frequency plane,
Hermitian systems possess many features with no counterpart in such as zeros and poles, emphasizing the influence of symmetries on
Hermitian systems. For example, exceptional points, a new type of altering system responses. We discuss two examples of MSs designs
degeneracies, may occur in non-Hermitian systems. They correspond relying on the complex-valued singularity approach in reflection and
to the degeneracy of two or more eigenvalues along with the coales- transmission. In Sec. XIX D, we address a new wavefront engineering
cence of their associated eigenvectors. These EPs are linked with sharp mechanism—topology-protected 2p phase accumulation for a specific
transitions in the eigenvalue spectrum, capable of dramatically altering polarization channel by encircling EPs in the parameter space.
the response of the system. Exceptional points are very important in Furthermore, the construction of EP pairs is harnessed to achieve uni-
parity-time symmetric systems as they are associated with spontaneous directional full-color vectorial holography employing a wavelength-
symmetry breaking. They thus separate regions of the parameter space multiplexing scheme. Finally, in Sec. XIX E, we delve into the potential
where the Hamiltonian spectrum is real from regions where the eigen- future prospects of complex-valued singularities particularly higher-
frequencies occur in complex conjugated pairs.112 Interestingly, parity- order ones. We address a novel phase excursion mechanism associated
time (PT) symmetric systems can display entirely real eigenvalue spec- with the zero mode conversion in parametric space and the designing
tra despite being governed by non-Hermitian Hamiltonian. While EPs of ingenious toolboxes that would exploit the control theory methodol-
are initially discovered in the context of quantum mechanical ogy for nanophotonics design.
Hamiltonians, realizing EPs experimentally in quantum systems poses
significant challenges. However, optical and photonic systems have B. Designing metasurfaces according to the position of
emerged as promising platforms for exploring non-Hermitian physics. complex-plane zero singularities
This is primarily due to the controllable introduction of optical gain MSs may be considered as linear systems which transform inputs
and loss—non-conservative elements in these systems. Given their into outputs. These transformations are mediated by transfer functions
design versatility, metasurfaces (MSs) represent a convenient approach or matrices which generally depend on the frequencies and directions
to study and validate non-Hermitian concepts in photonics. MSs are of the input signals. Depending on the situation and the type of MS to
two-dimensional artificial structures consisting of subwavelength unit be designed, the transfer function can be the reflection or transmission
cells which exhibit peculiar electromagnetic responses, not achievable coefficient or even the S or the Jones J matrix. Designing a MS
in natural materials. Most importantly, the response of MSs building often amounts to looking for the right set of geometrical and optical
blocks, i.e., nanostructures, are characterized by the scattering matrices, parameters allowing one to obtain the desired amplitude and phase of
which are inherently non-Hermitian. The non-Hermitian nature of the transfer function for a given frequency or an interval of frequen-
metasurfaces greatly influences their scattering properties. This cies. One can therefore take inspiration from other fields concerned
requires to look at the properties of coefficients of the scattering, with the design of linear systems such as electronics or control

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FIG. 43. (a). Behaviors of the amplitude and phase of a function possessing a zero and a pole in the complex frequency plane (top) and on the real axis (bottom). (b).
Symmetries of transmissionless (top) and reflectionless states (bottom). (c). Silicon nanocone MS possessing a reflection zero and pole complex conjugated and whose ampli-
tude remains large and constant while the phase varies from 0 to 2p. (d). (Top) trajectories of a couple of transmission zeros of a Sb2 S3 nanocube MS as the height of the
nanocubes h is varied. At two degeneracies of the two zeros, there is a transition between a situation where zeros are real and one where they are complex conjugated. (bot-
tom) At h ¼ 160 nm, one zero is in the upper part of the complex plane and almost complex-conjugated of a pole leading to a high amplitude and a variation of the phase
between 0 and 2p for the transmission coefficient. Figure (b) reproduced with permission from Colom et al., Laser and Photonics Rev. 17(6), 2200976 (2023). Copyright 2023
Wiley-VCH;1154 (c) reproduced with permission from Mikheeva et al., Optica 10, 1287 (2023).Copyright 2023 OSA;40 (d) reproduced with permission from Colom et al., Laser
and Photonics Rev. 17(6), 2200976 (2023). Copyright 2023 Wiley-VCH.1154 Copyright remains with the respective publishers.

engineering to describe and design MSs.1155 In these fields, it is com- increase in the phase is defined as counterclockwise. The well-defined
mon to look at the analytic continuation of response functions sense of rotation of the phase comes from the fact that we consider
FðxÞ of the systems in the complex-frequency plane. As discussed analytic functions.1126,1156 These phase singularities bring fundamental
above, the necessity of analyzing the response at complex frequen- deeper topological aspects to the study and design of MSs. In this sec-
cies is rooted in the non-Hermitian nature of scattering processes tion, we will discuss approaches to shape the optical response based on
used for the design of metasurfaces, particularly the resonant ones the control of the relative positions of these phase singularities in the
that suffer from scattering losses, and also sometime, of additional complex-frequency plane. We will also discuss the relationship
absorption losses. between zeros of transmission, reflection, and S matrix coefficients
Of particular importance are the zeros and poles of the response and the symmetries of MSs. Finally, we will provide two examples of
functions which generally occur in the complex-frequency plane. As MS designs that rely on this approach, one in reflection and another in
displayed in Fig. 43(a), simple zeros and poles are a given type of topo- transmission.
logical defects at which the phase is singular and around which the The analytic continuation in the complex-frequency plane of
phase behaves like a vortex with a 2p winding counterclockwise response functions FðxÞ can be expanded according to the
around zeros and clockwise around poles (more generally it winds 2np Weierstrass expansion1157,1158 depending on both zeros xz;n and poles
times for nth order phase singularities). Their topological charge C, as xp;n of the response functions,
defined earlier, is, respectively, þ1 and 1 when choosing a contour c Y x xz;n
encircling the singularity in the complex frequency plane. In this study, FðxÞ ¼ A expðiBxÞ : (9)
the phase winding direction adheres to the right-hand rule, where 2p n
x xp;n

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It is well known that xp;n generally occur in the lower part of the two reflection zeros for light impinging from the same side at the
complex plane [for a expðixtÞ time convention] in passive photonic frequencies xRZ and xRZ . Just like transmission zeros, reflection
systems because of causality. However, a special occurs for the bound zeros are consequently either real or occur in complex-conjugated
state in the continuum (BIC), poles can occur at real frequencies. To pairs. On the other hand, when P symmetry is broken, symmetry
preserve energy conservation, this can only occur when they merge constrained are lifted and xRZ can be complex-valued. In fact, by
with a zero.141 breaking the MS P symmetry, one can control the coupling coef-
Zeros may on the contrary occur at any position in the whole ficients of its modes to the top cTop and the bottom cBottom . From
complex plane. Depending on the positions of zeros, the variations of the temporal coupled mode theory, one finds that a zero and pole
the response functions display different behaviors as a function of the of the reflection coefficient of a lossless MS illuminated from the
input frequency. To illustrate this, let us first consider the case of a sin- top with a resonance frequency whose real part is x0 take the fol-
gle zero-pole pair in the expansion (9) with A ¼ 1 and B ¼ 0, lowing expressions:40
i:e:FðxÞ ¼ xxxxp . It has been shown in Ref. 1156, that when the zero
RZ

is in the lower part of the complex plane, there is generally a dip in the xRZ ¼ x0 þ icTop icBottom ;
(10)
amplitude of the response function and the phase varies only on a xP ¼ x0 icTop icBottom :
small phase interval (usually smaller than p). When the zero is on the It is thus clear that P symmetry breaking allows control of the
real axis, the response function cancels out for a certain frequency and imaginary part of reflection zeros and their relative positions to the
as a result, there is a p phase jump. Eventually, as illustrated in poles.
Fig. 43(a), when there is a zero in the upper part of the complex plane, Let us illustrate the usefulness of this insight for designing MSs
the phase spans the full ½0; 2p interval as the frequency is varied pass- with a desired optical response. To create optical components such as
ing across the line separating the zero-pole pair. This property is better meta-deflectors or metalenses, it is necessary to use MSs whose
evidenced when the phase is unwrapped. Moreover, if the zero response function amplitude is large to ensure a good efficiency of the
becomes complex-conjugate of the pole, one obtains a similar response component. It is also important that the phase of the response func-
as a Gires–Tournois etalon,40,1159 i.e., a constant and unitary amplitude tions spans the full ½0; 2p to be able to generate arbitrary phase gra-
alongside with a 2p phase variation. This shows that one can use the dients. As explained before, this condition on the phase requires to
position of zeros and poles of response functions as a design methodol- design structures to possess a zero in the upper part of the complex
ogy to address MS with the desired response in both amplitude and plane while the condition on the amplitude requires that this zero is

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phase. complex conjugated of the pole. Let us show how to fulfill these condi-
To this end, it is necessary to have a good understanding of the tions for a MS working in reflection and another working in
rules constraining the positions of zeros in the complex-frequency transmission.
plane. These constraints are related to the symmetries of the MS. It is For the reflection case, it appears from the expression of reflection
for example well known that time-reversal symmetry imposes that zeros and poles (10) that it is necessary to cancel out the coupling of
zeros of the S matrix coefficients are complex-conjugated of poles for the mode to the bottom channel to obtain complex conjugated zeros
lossless passive systems. Let us consider the symmetries governing the and poles. This condition is quite intuitive as the energy transmitted
positions of transmission and reflection zeros. These symmetries are can be considered as loss altering the reflection-based MS efficiency.
illustrated in Fig. 43(b) for normal incidence for transmission zeros To achieve this condition, we considered in Ref. 40 a MS consisting of
(top) and reflection zeros (bottom). Delving into the scenario of a pas- an array of silicon 600 nm high nanopillar with a period of 800 nm
sive, lossless MS with a transmission zero at the frequency xTZ , the embedded in a medium with a homogeneous refractive index equal to
time-reversal transformation leaves the MS invariant while causing a 1.5. The symmetry was broken by reducing the diameter at the top
reversal of momenta in the incident and reflected waves. DTop of the pillar compared to the diameter DBottom at the bottom
Consequently, the time-reversed counterpart of a transmissionless which is equal to 500 nm leading to a truncated cone geometry as
state is also a transmissionless state. As time-reversal implies complex shown in the top left of Fig. 43(c). For a ratio DTop =DBottom
conjugation of frequency, one can conclude that a lossless MS possess- ¼ 0:84; cBottom is almost zero for the resonance we consider and the
ing a transmission zero xTZ also possesses a transmission zero at the zero and pole are consequently almost complex conjugated as can be
frequency xTZ . As a consequence, illuminating this device at normal seen in the right panels of Fig. 43(c). As a result, the amplitude of the
incidence should display transmission zeros at real frequencies or pairs reflection coefficient is almost unitary and the phase spans the full 2p
of complex-conjugated transmission zeros. This is reminiscent of interval as shown in the bottom left figure of Fig. 43(c).
eigenvalues of PT symmetric Hamiltonian in the unbroken and bro- The design of MS in transmission for normal incidence fulfilling
ken phases.1160 the condition of zero-pole pairs which are complex conjugated is more
Regarding reflection zeros, their positions depend not only on challenging since the position of zeros does not depend on the spatial
the time-reversal symmetry but also on the mirror symmetry with symmetries of the structure (as long as there is no polarization conver-
respect to the median plane of the MS which will be called Parity sion). Yet, a solution exists for MSs working in the regime where zeros
(P)symmetry in the following discussion. Let us consider a loss- are complex-conjugated. This is in fact the underlying mechanism
less MS possessing a reflection zero xRZ . Time-reversal transfor- describing the physics of dielectric Huygens MSs.362,1154 To illustrate
mation amounts to reversing the momenta of the incident and this, we consider a MS consisting of an array of nanocubes of Sb2 S3 .
transmitted waves, and as a result, this MS also possesses a reflec- The top figures in Fig. 43(d) show the trajectories of the real and imag-
tion zero for the light impinging from the other side at the fre- inary parts of a couple of transmission zeros as the height of the nano-
quency xRZ . If the MS also preserves P symmetry, it possesses disks is varied. It appears that there are two distinct heights ( 140 and

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180 nm) at which transmission zeros are degenerated, this represents avoided crossing in non-Hermitian systems involves pairs of complex
a specific type of exceptional points, previously dubbed scattering singularities. This behavior contrasts drastically with the more conven-
EPs.1154,1161 In the height interval between these two degeneracies, the tional avoided crossing of resonances in Hermitian systems.
two zeros are complex conjugated while they are real outside this inter-
val. As a result, one zero gets almost complex conjugated of a pole.
C. Asymmetric full 2p phase engineering based on
The amplitude thus remains large while the phase varies from 0 to 2p
as seen in the bottom plots in Fig. 43(d). Interestingly and unexpect- exceptional points in metasurfaces
edly, the nature of the 2p-phase modulation as a function of the real EPs may manifest in more complex-valued linear operators that
frequency is due to the crossing of the branch-cut connecting only one represent input-output conversion relationships, with the scattering
zero-pole pair, and it is not due to the sum of two resonances, as previ- matrix and Jones matrix being the most typical among them. Taking
ously stated. The full phase modulation occurring here results from a the second-order Jones matrix as an example, particularly under the
spontaneous symmetry-breaking behavior, as previously discussed in circular polarization basis, EPs correspond to conditions for which
the framework of topological photonics.1162,1163 As shown herein, only one of the off diagonal terms cancel out while the other remains

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FIG. 44. Exceptional points manifested in Jones matrix systems for asymmetric phase engineering. (a) Schematic diagram and results of achieving topologically protected 2p
phase by encircling exceptional points. (b) Construction of a pair of exceptional points with orthogonal polarization state using mirror-symmetry strategy. (c) Illustration of asym-
metric full-color vectorial holography using exceptional point pairs. (a) Reproduced with permission from Song et al., Science 373, 1133 (2021). Copyright 2021 AAAS;37
(b) reproduced with permission from Yang et al., Nat. Commun. 15, 232 (2024). Copyright 2024 Nature Publishing Group;1165 and (c) reproduced with permission from Yang
et al., Nano Lett., 24, 844–851 (2024). Copyright 2024 ACS.1166 Copyright remains with the respective publishers.

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not null, i.e., Tþ ¼ 0 and Tþ different from 0. This happens when equal but opposite in phase for both circular polarization states, is gener-
the two eigen-polarizations of the Jones matrix coalesce and both cor- ally picked up by rotating polarization-converting optics. Operating spe-
respond to the right or left handed circular polarization, where þ and cifically at an EP is shown to suppress one of the polarization-
represent left circular polarization (LCP) to right circular polariza- conversion channels, thus ensuring that PB-phase is encoded on only
tion (RCP), respectively. This signifies the suppression of the conver- one of the polarization-conversion channels asymmetrically. To expand
sion channel from LCP to RCP, resulting in a zero or singularity point this specific asymmetric response of the EP photonic systems, research-
in the Tþ channel. There is consequently a reflection or transmission ers obtained the enantiomer Sm of the L-shaped meta-structure (S)
zero for one conversion channel but not the other which will be useful through a general mirror-symmetry strategy.1165 As shown in Fig. 44(b),
for information multiplexing. The construction and observation of upon Ex incidence, the current distribution of the vertical arm in the
such EPs have been presented in previous papers.1131,1164 Building meta-structure Sm switches the flow direction relative to its counterpart
upon these works, some of the authors of the present paper have in S, resulting in the degeneracy point of the eigenstates flipping from
implemented a new type of functional device by harnessing the robust RCP to LCP, corresponding to the north and south poles of the
topological phase, namely, the exceptional topological (ET) phase, by Poincare sphere, respectively. Therefore, in the parameter space defined
encircling the EPs. Using a meta-structure as shown in Fig. 44(a), by by the two arms of the meta-structure ðL1 ; L3 Þ, a pair of singularity
manipulating the dimensions of the structure in two orthogonal direc- points induced by EPs are obtained, manifesting as zero conversion
tions, we can attain desired x- and y-polarized resonances, facilitating coefficients for the two channels of MLR and MRL m
at ðL1 ; L3 Þ
the construction of an EP of the Jones matrix associated with the can- ¼ ð52 nm; 119 nmÞ. Interestingly, these two singularities give rise to
celation of Tþ channel. Importantly, upon achieving a closed loop phase vortices characterized by opposite topological charges in the
encircling the EPs in the parameter space, a phase accumulation of parameter space. By judicious arrangements of structures S and Sm on
u ¼ 2p will occur, which is attributed to the phase vortex existing the same MS, the resultant output polarization can be expressed as37
around the singularity in the complex plane. Considering any point R
on the complex plane, there is hSjSi ¼ Aþ eiuþ jþi þ A eiu ji; (14)

PðRÞ ¼ ReðRÞ þ i ImðRÞ; (11) where A represents amplitude and u represents the corresponding
phase. According to Eq. (14), coupling a pair of EPs breaks the limita-
where PðRÞ represents the position function and ReðRÞ and ImðRÞ tion of the circular output polarization state. By adjusting the amplitude
represent the real and imaginary parts of R, respectively. Therefore, ratio and phase difference of the two rows of meta-structures, a full-

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the phase of PðRÞ can be described as polarization state covering the Poincare sphere can be constructed while
ImðRÞ maintaining the unidirectional asymmetric imaging properties of the EP
u½PðRÞ ¼ arctan : (12) system. In brief, this work extends the application of EP to any arbitrary
ReðRÞ
polarization state, surpassing the inherent limitations of the asymmetric
When R moves continuously in parameter space from P1 to P2, the response brought by EP to the system, and enhancing the potential for
resulting accumulated phase can be given by the integral form: topological wavefront shaping applications. Furthermore, based on the
ð P2 construction of the aforementioned EP pairs, they have achieved a
/¼ u½PðRÞ du: (13) unique unidirectional full-color vectorial hologram by introducing a
P1 wavelength-multiplexing strategy,1166 as shown in Fig. 44(c). Since the
According to Fig. 44(a) and Eq. (13), it is evident that a phase accu- EPs can maintain the asymmetry of conversion in a wide wavelength
mulation of 2p solely occurs when the loop encircles the zero point (or range, the designed full-color vectorial hologram can still achieve opti-
singularity) while failing to achieve full-phase modulation when the sin- mized energy distribution. This asymmetric full-color holographic strat-
gular point moves away from the loop. The above analysis underscores egy based on EP pairs is expected to be widely used in more complex
the distinctive nature of channel Tþ , differing from its cross- application systems such as information security and virtual reality.
polarization channel Tþ , as the latter’s nearly constant amplitude dis-
tribution lacks the topological protection of the singular points. D. Concluding remarks and future perspective
Leveraging this unique property, we successfully achieved the decou- In conclusion, we have presented methods to design MSs to
pling of two circularly polarized lights. Specifically, upon incidence of achieve various functionalities by engineering the positions of zeros of
the RCP beam, a holographic image of the letter “C” appears at the R, T, S, and J via parameter tuning. Wavefront engineering relies on
designed 30 angle, while under LCP incidence, no corresponding image strategically placing complex-valued singularities in the parameter
appears. Furthermore, by combining the Pancharatnam–Berry (PB) space while exploiting exceptional points (EPs) of the Jones matrix
phase and ET phase, more sophisticated information multiplexing can enabling asymmetric full 2p phase modulation and full-color vectorial
be realized. This new phase modulation mechanism, together with reso- holography. However, it is crucial to clarify a common misconception
nant scattering, guided mode propagation phase, and orientation-related about the EPs of the Jones matrix as discussed in Sec. XIX D. Although
phase retardation, enriches the optical control methods, while its ease of they exhibit singular behavior in the parametric space, they are not the
implementation and compatibility with other phase-control mecha- actual singular points of the linear system itself. Recent studies high-
nisms also open the avenue for the application of topological phenom- light that the degeneracy of 2 zeros of the S-matrix is associated with
ena in the optical wavefront modulation. However, due to the inherent EPs, particularly those linked to coherent perfect absorption (CPA),
asymmetric behavior caused by the handedness of EP, current EP sys- with phase-sensitive single-mode absorption.1167 The attainment of
tems are confined to operation within a specific circular polarization resonant, absorbing, and CPA EPs in linear systems provides a versa-
state and lack the versatility to engineer arbitrary states. A PB phase, tile platform for controlling scattering responses. Additionally, the

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potential for full 2p phase modulation with nearly 100% transmittance process. Here, simulations might help disclose the deviations and
has been demonstrated using a glide-symmetric bilayer MS.1168 suggest what to improve in a further fabrication round.
Recognizing the sensitivity of higher-order singularities to the pertur- The numerical analysis of optical metasurfaces is particularly suc-
bations, consideration of these in photonic systems can enhance sensi- cessful because multiple numerical tools that solve the governing equa-
tivity and robustness to their locations in the complex frequency plane. tions, i.e., the Maxwell equations, have been developed and equipped
Notably, the geometric phase associated with spatial mode transforma- with suitable constitutive relations. These tools are mainly derived
tion would allow innovative implementation of the zeros in the mode from the general field of numerical mathematics and rely on discretiz-
conversion process. Akin to the exceptional ET phase in polarization ing the Maxwell equations by finite differences or finite elements in the
channels, a novel phase-addressing mechanism can be realized by time or frequency domain.1170,1171 Also, for strictly periodic metasurfa-
encircling the singular points of the conversion polarization coeffi- ces, various grating algorithms to describe diffractive optical elements
cients in the parametric space. Drawing inspiration from the principles and photonic crystals1172 were developed. However, while indisputably
of control theory, wherein the placement of poles and zeros is crucial helpful, the direct numerical solution of Maxwell equations often com-
for shaping a system’s behavior, including its stability, frequency plicates obtaining insights into the governing physics of metasurfaces.
response, and transient dynamic. This principle is similarly critical in Especially for metasurfaces, assembled from what is frequently called
nanophotonic device design, where the location of poles and zeros in the meta-atoms and analyzed in terms of the multipolar response
the complex frequency plane profoundly influences properties such as induced in such meta-atoms, a discussion that is closer to scattering
transmission, reflection, and phase modulation, making it feasible to theory is suggested to be often superior.
define the real-axis response and tailor nano-geometry based on the This Perspective article aims to give an overview of the recent
strategic placement of these topological singularities. Adopting control developments of such a framework for the multipolar description
theory methodologies in photonics could thus pave the way to a new of metasurfaces. The framework tremendously relies on the notion
paradigm for designing nanophotonics devices. of scattering theory.1173 Initially, it puts the description of the
optical response of the individual meta-atom into focus. It derives
XX. MULTIPOLAR DESIGN METHODS FOR
METASURFACES from that a set of insights into the optical functionality of entire
metasurfaces. We emphasize that the optical response of the indi-
Carsten Rockstuhl, Karim Achouri, Andrey B. Evlyukhin, vidual meta-atom is typically expressed by a T-matrix or general-
Ulrich Lemmer, and Ivan Fernandez-Corbaton ized polarizabilities.1174 While both expressions can be made

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interchangeable, they are different. For example, the T-matrix
[Link]@[Link] relies on a problem formulation in spherical coordinates, while the
polarizabilities use Cartesian coordinates. Here, we start from the
multipolar description using the T-matrix and establish the link to
An efficient, fast, and reliable framework for the theoretical
polarizabilities at a later stage.
description and the numerical analysis of the optical properties of
metasurfaces is vital to their exploration from a fundamental science
perspective and for their integration into applications. Here, we review B. State of the art
one such framework that resides on the broader framework of a semi- 1. Theoretical framework of a multipolar description
analytical scattering theory. In that description, the incident and scat-
tered fields are expanded into a multipolar series, and their relation is The multipolar description of a metasurface has to start with the
expressed by a matrix-vector product where the matrix is called the multipolar description of its meta-atom. In the framework of scattering
transition or T-matrix. Besides summarizing the state-of-the-art of the theory in the frequency domain, we initially seek elementary solutions
method, we elaborate on current research questions and oversee future to Maxwell equations that arise from their separability in spherical
developments. coordinates.1175 These vector spherical harmonics expand the incident
and the scattered field from the meta-atom as
A. Introduction 1 X
X j
ð1Þ ð1Þ
Computational means are nowadays indispensable for Einc ðr; xÞ ¼ qejm ðxÞNjm ðr; xÞ þ qm
jm ðxÞMjm ðr; xÞ;
exploring the optical properties of metasurfaces.94,1169 On the one j¼1 m¼j
(15)
hand, we can design them in silico according to predefined needs, X1 X j
ð3Þ ð3Þ
E ðr; xÞ ¼
sca
bejm ðxÞNjm ðr; xÞ þ jm ðxÞMjm ðr; xÞ;
bm
achieving an optical response on-demand before any fabrication. j¼1 m¼j
In addition to being essential for the design, computational means
ðnÞ ðnÞ
are useful for obtaining insights into aspects notoriously challeng- where Njm ðr; xÞ and Mjm ðr; xÞ are the vector spherical harmonics.
ing to measure. An example of the latter would be the vectorial These modes have well-defined frequency x, angular momentum
details of the near-field distribution, an important quantity for squared j, and angular momentum along a specific axis m. Physically,
nonlinear metasurfaces or those used for light management in the fields with j ¼ 1 are dipolar fields, with j ¼ 2 quadrupolar fields,
solar cells. On the other hand, we can simulate the optical etc. We distinguish modes with electric parity N and magnetic parity
response of fabricated devices to explain measured quantities. M. Finally, we distinguish between those vector spherical harmonics
Particularly for complicated metasurfaces, e.g., stacked ones, the expanding the incident and the scattered field using the index n ¼ 1
measured response often does not correspond to what had been and n ¼ 3, respectively. Instead of parity, a helicity base can also be
predicted before because of imperfections in the fabrication chosen, especially if chiral light–matter interactions are at stake. The

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relation between the concatenated amplitudes expanding the incident In the following, we discuss metasurfaces made from a periodic
field q and scattered field b from a meta-atom in a linear response is arrangement of identical meta-atoms.1178 Disordered metasurfaces or
written as spatially inhomogeneous metasurfaces can also be considered. However,
they are covered in other perspective articles in this APL Roadmap.
bðxÞ ¼ TðxÞqðxÞ; (16) While considering an arbitrary chosen meta-atom to be the central one,
where the T-matrix TðxÞ had been introduced, which entirely charac- we can write the field illuminating the particle as a superposition of the
terizes the optical response of the meta-atom.1176 For a sphere, the T- external illumination and the scattered field from all the other particles.
matrix can be built analytically as a diagonal matrix containing the By dropping the frequency argument, this can be written as
Mie-coefficients. For an arbitrary shaped object, the T-matrix can be
X
obtained numerically by multiple means.1177 They all rely on exciting b¼T qþ 0 ð3Þ ð
C RÞbR ; (17)
the meta-atom with different illuminations, computing and expanding R
the scattered fields into vector spherical harmonics, and reconstructing where Cð3Þ ðRÞ are the lattice coupling matrices that convert the scat-
the T-matrix that links all the different incident and scattered field tered field from meta-atom i into an incident field on the central meta-
amplitudes determined numerically. atom. The prime in the sum indicates that the central particle is

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FIG. 45. Illustration of some phenomena and applications explored in the context of metasurfaces and which can be discussed extremely convenient using the multipolar
description. Starting at midnight and going clockwise, the phenomena are lattice resonances (figure adapted from Ref. 1179). Then we have diffusers as discussed in this road-
map also in the context of disordered metasurfaces (figure adapted from Ref. 1180). Next, we have holograms. Then, we have bound-states-in-the-continuum (BIC) that require
a multipolar analysis in their design (figure adapted from Ref. 1181). As the following phenomena, we have mentioned here pseudochirality and then angular scattering. Finally,
we also mention as a possible domain of exploration molecular metasurfaces. At last, we have as an example the wide field of Kerker effects (figure adapted from Ref. 1182).
All figures reproduced (adapted) with permission from the respective Journals and copyright remains with the original publishers.

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excluded. Considering plane wave illumination characterized by a Examples are reflectance and transmittance spectra or their phases,
transverse wave vector that expresses the phase variation of the inci- polarization-dependent quantities, or near- and far-fields, to mention
dent field across the metasurface and exploiting the Bloch theorem, we only a few selected ones. This is at that heart of many optical phenom-
can write the scattered field amplitude from each meta-atom forming ena that can be explored. We mention some of these phenomena and
the metasurface as applications thereof in Fig. 45 and elaborate on some of them further
below.
bR ¼ eikjj R b: (18) Also, scattering matrices can be defined that express reflection
and transmission upon illuminating the metasurface from both direc-
tions. These scattering matrices constitute the primary object of
Substituting this expression into Eq. (17) and solving it for the scat-
obtaining the response from stacked metasurfaces. Layer-doubling
tered field amplitude vector, we obtain
techniques are very efficient for getting the response from stacked
X 1 metasurfaces.1183
0 ð3Þ ð
b¼ IT C RÞeikjj R Tq: (19)
R

2. Numerical implementation
This equation is intuitive and says that the external illumination indu-
ces multipole moments that expand the scattered field. The response is The aforementioned theoretical framework is highly susceptible to
mediated by the T-matrix of the meta-atom renormalized by the inter- numerical implementation. The algebraic formulation reduces the com-
action with all the other meta-atoms forming the lattice. Their ampli- putational complexity to solving matrix-vector products. With the analyt-
tudes can be expressed by summing up the scattered field from all the ical availability of T-matrices for spheres, it is no surprise that the first
particles forming the lattice and projecting it onto the plane wave con- numerical implementations of the above-sketched framework were done
stituting the discrete diffraction orders. These amplitudes of the dif- nearly 30 years ago.1184 At that time, the algorithms were mainly used to
fraction orders are the primary quantity of the solution to the problem, explore photonic crystals made from spheres and gratings from high-
and many further properties of interest can be extracted from them. index dielectric or metallic spheres, which we call metasurfaces today.

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FIG. 46. A computational example to highlight the strength of the multipolar description of metasurfaces. (a) Geometry of the considered example: The layer sequence corre-
sponds to ITO (orange), amorphous silicon p-doped (green) and intrinsic (red), and crystalline silicon (purple). A metasurface made from titanium dioxide disks with a height of
100 nm and a radius of 150 pnm
ffiffiffi lies on top of that layer stack. The lattice and the period would be subject to variations. (b) Example of a hexagonal lattice with a square root of
the unit cell area equal to A ¼ 520 nm, we show the simulated reflectance at normal incidence and the reference reflectance from a sample without the metasurface. The fig-
ure also shows an AM1.5D spectrum. (c) Reflectance of the sample as a function of the wavelength and the lattice size for two different types of lattices, i.e., once for a hexago-
nal lattice and once for a rectangular lattice with an aspect ratio of 1.3. (d) When weighting the reflectance with the AM1.5D spectrum and integrating between 300 and
1100 nm, we obtain a measure for the current loss due to reflectance. That quantity is shown for different lattices and different lattice sizes. An optimum can be identified from
that FIG. Thanks to the effective multipolar description, the computation is extremely fast. The T-matrix of the disk needs to be calculated only once for each frequency. And the
reflectance analysis from the lattice are eventually matrix-vector-products of a small size, which can be done very efficiently. FIG adapted from Ref. 1178. All figures reproduced
(adapted) with permission from the respective Journals and copyright remains with the original publishers.

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With the renewed interest in expressing the response of meta- the size of the unit cell that can be effectively analyzed. So, if a simula-
atoms as building blocks of metamaterials on a multipolar basis, vari- tion of the response from a reasonably sized, uniformly heighted unit
ous groups developed numerical tools to study the optical response cell of a metasurface is required, a method like RCWA is a viable
from metasurfaces. The key aspect of all implementations is the evalu- option. For all other configurations, the T-matrix-based scattering
ation of the lattice couplings in Eq. (19). Here, Ewald summation tech- approach is more appropriate, provided that the additional computa-
niques are exploited that split the badly converging sums into a part tional effort to determine the T-matrix of the scatterer is worth it.
evaluated in real space and a part evaluated in reciprocal space.1185
Current development revolves around the computations of lattice 3. Analytical investigations
sums along different dimensions and considering multiple meta-atoms
per unit cell.1186 That latter would be needed when studying bound While the multipolar description constitutes a powerful tool to
states in the continuum or topological metasurfaces. The proper con- explore the functionality of metasurfaces numerically, it unfolds its
sideration of particles closely space above substrates or the consider- forte when considered from an analytical perspective.1191 Two aspects
ation of particles that penetrate their respective circumscribing spheres are important.
is also explored.1187 Finally, it remains to be mentioned that various First, explicit analytical expressions for many quantities of interest
codes have been made publicly available.1188–1190 A representative can be derived under some restricted settings. When isotropic scatter-
analysis of the optical response of a metasurface for an application as a ers are considered, i.e., spheres, the T-matrices reduce to a diagonal
light management structure is discussed in Fig. 46. All the simulations one, and only a few coefficients are non-zero. Moreover, while theoret-
shown in that figure were computed within 4.6 h on an ordinary desk- ically, the T-matrix is infinite in size and numerically truncated to a
top PC. That includes the computation of the T-matrix of the consid- sufficiently large size to ensure convergence behavior, it is analytically
ered disk. Performing the same simulations using a finite-element feasible to consider only a few lowest-order multipolar orders.
code would have taken 2.6 years. The analysis highlights the strength Furthermore, high-symmetry lattices, e.g., square and subwavelength
of the multipolar description of the metasurface.1178 lattices, can be assumed to lower the complexity of the setting. Then,
However, it needs to be clearly said that the approach is less pre- eventually, the system gets reduced in complexity, and explicit analyti-
ferred in specific situations. For example, when only the specific cal equations can be expressed for most quantities of interest. For
response to a specific excitation of a fixed metasurface is needed, the example, the reflection and transmission amplitude at normal or obli-
additional overhead of computing the T-matrix first that allows us to que incidence can be easily expressed. This dramatically simplifies the
analysis and allows for parametric investigations of effects such as

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express the response to any given illumination is not justified. This
should be the largest weakness of the method. Moreover, other meth- bound states in the continuum, lattice resonances, polarization filters,
ods, including both full-wave Maxwell solvers and semi-analytical or diffraction gratings. We wish to make clear that the formulated
techniques, are equally applicable to model metasurfaces. Common assumptions are only made for convenience to reach manageable
full-wave solvers utilize finite element or finite difference methods in expressions. It ultimately is up to the convenience and efforts of the
either time or frequency domain. Alternatively, semi-analytical person who uses the method to decide up to which degree of complex-
approaches such as the rigorous coupled wave analysis (RCWA) can ity they would like to work analytically. One can easily derive analytical
be effectively used. Initially developed for dielectric gratings, the expressions for any observable quantity by lifting the assumption on
RCWA has been adapted for photonic crystals, metamaterials, and isotropic scatterer and a square and subwavelength lattice, and one can
metasurfaces with a strictly periodic arrangement of identical unit cells. also consider arbitrary higher multipolar orders, it is just that the
In the RCWA method, one first solves for Bloch-periodic expressions get longer and are not that handy anymore. In cases with
eigenmodes of Maxwell’s equations within a metasurface assumed to too many unknowns, the problem can always be treated numerically.
be invariant in the principal propagation direction. These eigenmodes It is just that closed-form analytical expressions are no longer reason-
are represented in a plane wave basis, with interface conditions subse- able. We leave it up to the researcher to decide up to which order they
quently applied to determine the amplitudes of modes excited within wish to consider on analytical grounds.
the metasurface and the adjacent spaces. This method is particularly Second, the entries of the T-matrix themselves do not attain arbi-
suited for metasurfaces with discrete heights, treating the metasurface trary values. For example, for spheres, they can be parametrically
as a single layer. However, for metasurfaces with continuously varying expressed using a single angle hj bound between p=2 and p=2 for
surface profiles, the profile must be segmented into different layers. lossless particles. For absorbing particles, a second angle h0j bound
While RCWA rapidly predicts the optical response of a metasurface, it between 0 and p=2 parametrizes the dissipation.1192 The possible value
of a Mie coefficient reads then
does not provide extensive physical insights. Here, the multipolar scat-
tering framework is preferable, as it highlights the influence of individ- 1
bj ¼ : (20)
ual unit cells on the optical response. 1 i tan hj þ tan h0j
Moreover, although RCWA is efficient for metasurfaces with dis-
crete heights, the analysis becomes more complex and time- This constitutes a significant simplification, as a desired response
consuming for continuously varying profiles or metasurfaces com- can be adjusted by identifying the Mie angles of all involved entries of
posed of free-form particles. Each layer requires solving a dedicated the T-matrix. Combined with the analytical expressions, the necessary
eigenvalue problem, and if the unit cell varies within a supercell, the properties of the meta-atom in terms of Mie angles can be identified
expansion must include many plane waves, slowing the computation that provide a metasurface with a response on demand can be identi-
significantly. The complexity of these computations typically scales fied. Identifying suitable particles with the specified properties is a sec-
cubically with the number of plane waves, imposing practical limits on ondary problem that inverse-design techniques can solve.

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C. Future directions and outlook ikd my ikd Qxz ikd Myz
t ¼1þ px þ þ ;
1. A description using polarizabilities E0 2SL e0 ed cd 6 2cd
(24)
ikd my ikd Qxz ikd Myz
So far, the description has focused on an analysis using T- r¼ px þ þ ;
E0 2SL e0 ed cd 6 2cd
matrices that express the scattering response using basis functions
in a spherical coordinate system. Sometimes, that is inconvenient, where E0 is the incident electric field at the center of meta-atoms, SL
and a discussion in multipole moments linked to specific directions is the surface area of the metasurface elementary cell, and cd is the
in a Cartesian coordinate system may be more intuitive. Then, one light speed in the surrounding medium. For the above equations, we
speaks of multipolar polarizabilities that are induced instead of the assume that the metasurface plane coincides with the xy-plane of the
amplitudes of the vector spherical harmonics.1193 Instead of speak- Cartesian coordinate system, and the incident wave of the frequency
ing of a T-matrix, we speak of the Cartesian multipole moments x is ðE0 ; 0; 0Þeiðkd zxtÞ . The considered Cartesian multipole
and polarizabilities. When care is taken to eliminate the trace and moments of the meta-atoms (p and m are the electric and magnetic
the redundant components of the Cartesian tensors, the change dipole moments, and Q and M are the electric and magnetic quadru-
between Cartesian and spherical multipoles is merely a change of pole moments, respectively) enter through the components that pro-
basis. It has no implication on the physics as long as no additional vide radiation in a direction perpendicular to the metasurface.
approximations are made. Therefore, there is a useful opportunity to combine multipole
Expressions exist to convert between these amplitudes of the moments with the same parity symmetry (with respect to inver-
spherical harmonics and the Cartesian multipole moments. For sion)1195 into one group and introduce the corresponding effective
example, the two lowest-order electric coefficients can be converted multipole M ðpÞ and its effective polarizability aðpÞ , for the even (odd)
as1174 multipole moments p ! e (p ! o).1179 So that for the case (24) one
f1 can write
e1
d p¼ MDipole be1 ;
ik3d ikd ðoÞ
f2
(21) t ¼1þ ða þ aðeÞ Þ; (25)
kd e1 2SL
d Q ¼ 3 MQuadrupole b2 ;
e
ikd ikd ðoÞ
r¼ ða aðeÞ Þ; (26)
where the matrices that connect the electric multipole moments in a 2SL

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spherical basis (be1 and bew ) to a Cartesian basis (p and Q) are where aðoÞ ¼ M ðoÞ =ðE0 e0 ed Þ ¼ ðpx ikd Myz =2cd þ Þ=ðE0 e0 ed Þ
2 3
1 0 1 and a ¼ M ðeÞ =ðE0 e0 ed Þ ¼ ðmy =cd ikd Qxz =6 þ Þ=ðE0 e0 ed Þ.
ðeÞ
1 6 7 From the representation (25) and (26) one can see that the lattice ana-
MDipole ¼ pffiffiffi 4 i 0 i 5;
2 pffiffiffi pole effect, when the light wave transmits through the metasurface
2
0 2 0
3 without changes in amplitude and phase, is realized if aðoÞ ¼ 0 and
i 0 0 0 i aðeÞ ¼ 0 independently, that is due to destructive superposition
6 7 (22) between contributions of the multipole moments of the same inverse
6 0 i 0 i 0 7
1 6 p ffiffi
ffi 7 parity symmetry. In contrast, the lattice Kerker effect (only the sup-
MQuadrupole ¼ pffiffiffi 6 0 0 2 0 07 7:
266 7 pression of reflection) is realized for aðoÞ ¼ aðeÞ due to the destructive
4 0 1 0 1 0 5 superposition between the multipole moments with different inverse
1 0 0 0 1 parity symmetry. The case of a bianisotropic response (when multipole
coupling exists between the multipole moments of different inverse
Similar matrices also exist for higher-order terms.1191 In these expres- parity) can also be involved in this approach.1196,1197
sions, kd is the wavenumber in ffithe background medium with a permit-
pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi Note that we have been talking about the effective polarizability
tivity ed, and fj ¼ ð2j þ 1Þ!p. Using that framework, T-matrices can of meta-atoms inside a metasurface so far. However, significant advan-
be converted into polarizabilities with the same simplicity. For exam- tages can be obtained if the polarizability of single meta-atoms and the
ple, the electric dipolar part of the T-matrix Tee can be converted into so-called lattice sums are considered.70,1198,1199 Recently, a strategy has
the electric dipolar polarizability matrix aee as been proposed to tune a symmetry-protected bound state in the con-
tinuum in the desired spectral range by directly determining the period
Zd k3d c
Tee ¼ MDipole aee M1
Dipole ; (23) of a metasurface consisting of building blocks with known electric or
6pi magnetic dipole polarizabilities. This can be explicitly obtained from
with Zd the impedance of the background medium. Then, all the the point of intersection (coincidence) between the real part of the cor-
details described above can be expressed in polarizabilities and responding inverse dipole polarizability of an individual building block
Cartesian multipole moments. Besides the numerical analysis, semi- (meta-atom) and the real part of the corresponding lattice sum, taking
analytical expressions for observables that provide valuable insights into account inter-particle interaction in the metasurface. In particular,
can also be obtained. it is shown that to obtain a bound state in the continuum at the reso-
In the framework of the analytical treatment discussed above, for nant wavelength kR of an individual meta-atoms, the period of a meta-
example, for metasurfaces composed of identical isotropic meta- surface with a square cell must be equal to 0:71kR .1200 In the case of
atoms, the electric field coefficients of reflection r and transmission t at including the resonant contribution of multipoles of various orders
the condition of the normal incidence of an external linear x-polarized into the metasurface model, the approximation of effective polarizabil-
plane wave can be represented as1194 ities and lattice sums makes it possible to study the lattice-induced

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interaction between these multipoles in a semi-analytical form.1199 In metasurfaces. Generally, the multipolar decomposition of the optical
some cases, such coupling can lead to the suppression of contributions response of meta-atoms allows one to understand and engineer nota-
from certain groups of multipoles and the implementation of anapole ble and beneficial effects, such as directional radiation. As understood
states or quasi-bound states in the continuum. by Kerker et al.,1210 the interference of the fields radiated by an electric
dipole and a magnetic dipole can result in highly directional far-fields.
2. Multipolar interface conditions The effect has been engineered and demonstrated in different fre-
quency bands for samples under far-field illumination962,1211 and for
In parallel to the elaboration of the T-matrix mentioned above dipolar emitters near the nanostructures.1212 Understanding these
method, an alternative metasurface modeling technique has been effects is a major challenge and many open questions remain, partially
developed based on generalized sheet transition conditions mentioned in this contribution to the roadmap but partially also in
(GSTC).1201–1205 This modeling technique relies on the premise that a other contributions.
metasurface acts as a discontinuity that may be modeled as a homoge- Moreover, the formalism introduced here cannot just be applied
nous polarizable sheet whose response is described in terms of effective to artificially structured macroscopic materials but also to other (nano-)
material parameters. For this purpose, the concept of polarizabilities is photonic systems. A major stream of efforts goes into developing
generally replaced by that of susceptibilities, as the latter is more com- metasurfaces with molecular building blocks.1213 From a gigantically
monly used to describe the response of a material from the perspective large chemical space, the individual molecules can be chosen that are
of a Cartesian lattice. The main difference between these two modeling periodically arranged using different techniques, and materials can be
techniques is that the T-matrix approach focuses on the scattering provided that inherit their linear, bianisotropic, or nonlinear properties
response of individual meta-atoms to build up to the response of the from the individual molecules. In a multi-scale effort, the framework
overall metasurface by including the coupling between the meta-
described here can be used to express the properties of these materials
atoms. In contrast, the GSTC method ignores the granular response of
from first principles and to study their interaction with light. To reach
the meta-atoms and rather directly relates the fields interacting with
such a description, quantum-chemical tools, mostly time-dependent
the metasurface to its susceptibilities, which intrinsically includes the
density functional theory, compute the T-matrix of an individual mole-
coupling between the meta-atoms.1202–1205
cule or an aggregate. Afterward, periodically arranged molecules accessi-
Fundamentally, the GSTC models how the fields and their spatial
ble, e.g., with surface-anchored metallic organic frameworks can be
derivatives interact with a metasurface. This model is derived by
studied in detail. The detailed and accurate description of the molecules
expanding these fields, along with the metasurface polarization densi-

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that surpasses a phenomenologically motivated description of a mole-
ties, in terms of a series of derivatives of the Dirac delta distribution.
cule as a polarizable two-level system provides unprecedented insights.
This rigorous foundation makes the GSTC ideal for modeling conven-
Furthermore, hybrid systems can be explored where molecular and tra-
tional dipolar metasurfaces and opens the door for including more
ditional scatterers are seamlessly blended.
complex interactions. As such, they now include second-order nonlin-
Moreover, the metasurfaces can be homogenized in some cases,
ear polarizations,1206 time-varying modulations,1205 multipolar contri-
and effective properties can be assigned to a film so that the optical
butions, and nonlocal responses.1207,1208 Another strength of the
response from the metasurface and the effectively homogenous
GSTC is that they can be used for both synthesis, i.e., finding the meta-
medium agree.1214 This unlocks novel possibilities when integrating
surface susceptibilities in terms of specified fields, and for analysis, i.e.,
metasurfaces into the design of more traditional optical elements.
computing the fields scattered by a metasurface with known suscepti-
While the theory is well-established in dipole approximation, nonlo-
bilities. For instance, it has been demonstrated using the GSTC that
cal metasurfaces are within reach and are currently being discussed.
nonlocal responses are required to synthesize perfectly refractive meta-
In these metasurfaces, higher-order multipolar components have a
surfaces.1169 Several numerical schemes have been developed for the
significant contribution. The complexity in their description advan-
analysis, such as finite-difference frequency- and time-domain techni-
ques, a finite element method, and a spectral-domain integral-equation ces, and more sophisticated properties are in reach. The nonlocal
technique, that can compute the fields scattered by a metasurface character, generally, leads to an angle dependent response, that can be
under arbitrary illumination conditions.1209 used for image processing purposes. In addition, it unlocks the oppor-
Finally, connecting the susceptibilities to the geometry of actual tunity to multiplex the response depending on, e.g., the angle of inci-
meta-atoms is typically achieved using equations that relate these suscep- dence. Such a multiplexing can add enhanced functionality to the
tibilities to the metasurface full-wave simulated scattering parameters.1205 devices. Additionally, deriving generalized impedance, admittance, or
While effective, this approach remains slow and cumbersome. For this even susceptibility tensors from the T-matrices or polarizabilities
reason, a methodology to connect the susceptibilities directly to the renormalized by the two-dimensional lattice interactions can be of
T-matrix of meta-atoms, which should significantly simplify the meta- practical benefit. It allows us to study and exploit the renormalization
surface practical implementation procedure, is being actively devel- of the properties of the scatterer due to the lattice interaction and ena-
oped. Note that it is currently already possible to map the dipolar bles shaping the optical response actually not just by choosing a spe-
polarizabilities of a metasurface with its corresponding dipolar cific meta-atom, but rather by combining the meta-atom and the
susceptibilities.1205 lattice. Exploiting the renormalization can lead to effects such as a
giant magnetic dipolar moments, which may in turn find applications
3. Further developments
when perceiving impedance-matched optical devices with vanishing
reflection losses.
Finally, we wish to reflect on selected advanced topics currently Finally, significant efforts are currently in place to solve the
under development in the context of the multipolar description of inverse problem, i.e., instead of quantifying the optical response of a

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given metasurface, we aim to identify the metasurface that provides an efficiency, as these coupling effects need to be considered. The general
optical response on demand.1106 We have touched on that issue framework described here can handle these effects, but efforts are
already in Sec. XX C 3. Yet/However it can also be done with estab- needed to formulate everything in a differentiable form and to use it in
lished methods from inverse design, such as topology optimization or an inverse design framework.
Bayesian optimization, tools that effectively exploit gradient informa- Furthermore, the combination of the optical properties of the
tion, genetic algorithms, or particle swarm optimization. Moreover, metasurface with other physical phenomena would tremendously
techniques from the field of machine learning are explored. However, widen the range of use cases. One example would be photothermal
for individual design problems, the efforts in generating data used for behavior, where the dissipation of energy changes the temperature of
training artificial neural networks (ANNs) usually exceed by far the the medium, which in turn changes the material properties, which
efforts to solve the inverse problem directly. Yet/However independent changes the optical response. In general, many other effects could be
of that, the community actively explores scenarios where using ANNs considered to work toward switchable and tunable metasurfaces.
is appealing. Finally, the extension of the formalism to treat nonlinear effects
can safely be foreseen as a direction for future developments. Many of
D. Conclusions the other contributions in this roadmap will also serve as a guide for
This mini-review gave an overview of a highly flexible approach open issues that can be tackled with dedicated improvements to the
to theoretically and computationally explore the optical response of framework sketched in this contribution.
metasurfaces. It resides on the language of scattering theory, where ini-
tially, the interaction of light with a localized object, i.e., the meta- ACKNOWLEDGMENTS
atom, is studied on semi-analytical grounds. That can be done with the C.R. and U.L. acknowledge support through the Deutsche
T-matrix or the polarizability matrix, depending on whether a spheri- Forschungsgemeinschaft (DFG, German Research Foundation)
cal or Cartesian coordinate system is considered. Thanks to the effi- under Germany’s Excellence Strategy via the Excellence Cluster 3D
cient evaluation of lattice sums, the interaction among the meta-atoms Matter Made to Order (EXC-2082/1, Grant No. 390761711). A.B.E.
forming the metasurface is assessed, and the optical response in terms acknowledges support through the Cluster of Excellence PhoenixD
of reflection and transmission from metasurfaces can be evaluated. It (EXC 2122, Project ID No. 390833453). I.F.-C. and C.R.
needs to be emphasized that the computational approach is highly effi- acknowledge support through the CRC Waves: Analysis and
cient, and the design and analysis of metasurfaces is tremendously Numerics (SFB 1173, Grant No. 258734477. K.A. acknowledges

12 April 2025 [Link]

accelerated. Yet/however it is also a framework that can be reduced to funding from the Swiss National Science Foundation (Project No.
obtain handy analytical expressions to discuss numerical observables PZ00P2_193221). We all wish to acknowledge contributions to this
on analytical grounds. Multiple current developments were sketched. work from our past and current group members, for which we are
What remains is to elaborate shortly on open issues. One aspect deeply grateful.
concerns densely packed metasurfaces made from asymmetric objects.
The scattering formalism assumes that the circumscribing spheres of AUTHOR DECLARATIONS
adjacent objects do not penetrate, as otherwise, the Rayleigh hypothesis
Conflict of Interest
breaks down. That restriction limits the types of metasurfaces that can
be considered. The problem can be circumvented with concepts such The authors have no conflicts to disclose.
as distributed T-matrices, where multiple origins are considered to
expand the field into vector spherical harmonics, but the approach is Author Contributions
yet premature. Moreover, combining the considered framework with S.A.S., R.F.O., and M.K. conceived and organized this roadmap,
methods from inverse design is ongoing, and we can expect much pro- including selecting the section topics and lead authors. These three
gress in this field. One aspect needs to be highlighted here, and it con- authors contributed equally and may claim first authorship. The fol-
cerns the simulation of metasurfaces made from a spatially lowing authors led individual sections (in order of the sections):
inhomogeneous arrangement of meta-atoms, which can be handled by Andrea Alu, Isabelle Staude, Rupert F. Oulton, Alasdair W. Clark,
considering rather large supercells. Spatially inhomogeneous metasur- Maria Kafesaki, Anatoly V. Zayats, Stefan Maier, Xianzhong Chen,
faces are needed for many applications, e.g., meta-lenses, meta-holo- Andrea Di Falco, Maria V. Chekhova, Ren-Min Ma, Rachel Grange,
grams, and other optical meta-devices. The design of these devices Mohsen Rahmani, Andrei Faraon, R. Sapienza, Philippe Lalanne,
usually follows a three-step procedure. First, the complex transmission Sebastian A. Schulz, Willie J. Padilla, Patrice Genevet and Carsten
function at each spatial location is identified by suitable means. Rockstuhl. These authors supervised the writing of their relevant sec-
Second, the optical response from a periodically arranged unit cell tions, selected their coauthors and determined the overall direction of
with varying geometrical parameters is simulated and stored in some their perspectives. All other authors contributed to the perspective
lookup table. Last, the particles are fetched from the lookup and placed articles under which they are listed. The author list is in order of
to the position of the unit cell where they shall provide the desired appearance in the document.
complex response. However, this approach does not consider the fact Sebastian A. Schulz, Rupert. F. Oulton, Mitchell Kenney con-
that the response of the meta-atom in an inhomogenous environment ceived and coordinated the roadmap together. All three act as joint
is not the same as that of the same meta-atom in a periodic arrange- corresponding and joint first authors for the full document.
ment. In consequence, the metasurface shows a degraded efficiency.
Optimizing the spatial details of the unit cell by methods from the field Sebastian A. Schulz: Conceptualization (equal); Writing – original
of inverse design is potentially the key to reach devices of very high draft (equal); Writing – review & editing (equal). Rupert F. Oulton:

Appl. Phys. Lett. 124, 260701 (2024); doi: 10.1063/5.0204694 124, 260701-95
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Conceptualization (equal); Writing – original draft (equal); Writing – draft (equal); Writing – review & editing (equal). S. M. Kamali:
review & editing (equal). Mitchell Kenney: Conceptualization (equal); Writing – original draft (equal); Writing – review & editing (equal). E.
Writing – original draft (equal); Writing – review & editing (equal). Arbabi: Writing – original draft (equal); Writing – review & editing
Andrea Al u: Conceptualization (supporting); Writing – original draft (equal). Andrei Faraon: Conceptualization (supporting); Writing –
(equal); Writing – review & editing (equal). Isabelle Staude: original draft (equal); Writing – review & editing (equal). A. C.
Conceptualization (supporting); Writing – original draft (equal); Harwood: Writing – original draft (equal); Writing – review & edit-
Writing – review & editing (equal). Ayesheh Bashiri: Writing – origi- ing (equal). S. Vezzoli: Writing – original draft (equal); Writing –
nal draft (equal); Writing – review & editing (equal). Zlata Fedorova: review & editing (equal). Riccardo Sapienza: Conceptualization
Writing – original draft (equal); Writing – review & editing (equal). (supporting); Writing – original draft (equal); Writing – review &
Radoslaw Kolkowski: Writing – original draft (equal); Writing – editing (equal). Philippe Lalanne: Conceptualization (supporting);
review & editing (equal). A. Femius Koenderink: Writing – original Writing – original draft (equal); Writing – review & editing (equal).
draft (equal); Writing – review & editing (equal). Xiaofei Xiao: Alexandre Dmitriev: Writing – original draft (equal); Writing –
Writing – original draft (equal); Writing – review & editing (equal). review & editing (equal). Carsten Rockstuhl: Conceptualization
John Yang: Writing – original draft (equal); Writing – review & edit- (supporting); Writing – original draft (equal); Writing – review &
ing (equal). William J. Peveler: Writing – original draft (equal); editing (equal). Alexander Sprafke: Writing – original draft (equal);
Writing – review & editing (equal). Alasdair W. Clark: Writing – review & editing (equal). Kevin Vynck: Writing – original
Conceptualization (supporting); Writing – original draft (equal); draft (equal); Writing – review & editing (equal). Jeremy Upham:
Writing – review & editing (equal). George Perrakis: Writing – origi- Conceptualization (supporting); Writing – original draft (equal);
nal draft (equal); Writing – review & editing (equal). Anna C. Writing – review & editing (equal). M. Zahirul Alam: Writing –
Tasolamprou: Writing – original draft (equal); Writing – review & original draft (equal); Writing – review & editing (equal). Israel
editing (equal). Maria Kafesaki: Conceptualization (supporting); De Leon: Writing – original draft (equal); Writing – review &
Writing – original draft (equal); Writing – review & editing (equal). editing (equal). Robert W. Boyd: Writing – original draft (equal);
Anastasiia Zaleska: Writing – original draft (equal); Writing – review Writing – review & editing (equal). Willie J. Padilla:
& editing (equal). Wayne Dickson: Writing – original draft (equal); Conceptualization (supporting); Writing – original draft (equal);
Writing – review & editing (equal). David Richards: Writing – origi- Writing – review & editing (equal). Jordan M. Malof: Writing –
nal draft (equal); Writing – review & editing (equal). Anatoly Zayats: original draft (equal); Writing – review & editing (equal). Aloke
Conceptualization (supporting); Writing – original draft (equal); Jana: Writing – original draft (equal); Writing – review & editing

12 April 2025 [Link]

Writing – review & editing (equal). Haoran Ren: Writing – original (equal). Zijin Yang: Writing – original draft (equal); Writing –
draft (equal); Writing – review & editing (equal). Yuri Kivshar: review & editing (equal). Remi Colom: Writing – original draft
Writing – original draft (equal); Writing – review & editing (equal). (equal); Writing – review & editing (equal). Patrice Genevet:
Stefan Maier: Conceptualization (supporting); Writing – original draft Conceptualization (supporting); Writing – original draft (equal);
(equal); Writing – review & editing (equal). Xianzhong Chen: Writing – review & editing (equal). Karim Achouri: Writing –
Conceptualization (supporting); Writing – original draft (equal); original draft (equal); Writing – review & editing (equal). Andrey
Writing – review & editing (equal). Muhammad Afnan-Ansari: B. Evlyukhin: Writing – original draft (equal); Writing – review &
Writing – original draft (equal); Writing – review & editing (equal). editing (equal). Ulrich Lemmer: Writing – original draft (equal);
Yuhui Gan: Writing – original draft (equal); Writing – review & edit- Writing – review & editing (equal). Ivan Fernandez-Corbaton:
ing (equal). Arseny Alexeev: Writing – original draft (equal); Writing Writing – original draft (equal); Writing – review & editing
– review & editing (equal). Thomas F. Krauss: Writing – original draft (equal).
(equal); Writing – review & editing (equal). Andrea di Falco:
DATA AVAILABILITY
Conceptualization (supporting); Writing – original draft (equal);
Writing – review & editing (equal). Sylvain D. Gennaro: Writing – Data sharing is not applicable to this article as no new data were
original draft (equal); Writing – review & editing (equal). Tomas created or analyzed in this study.
Santiago-Cruz: Writing – original draft (equal); Writing – review &
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27
AFFILIATIONS ETH Zurich, Department of Physics, Institute for Quantum
1 Electronics, Optical Nanomaterial Group, Auguste-Piccard-
SUPA, School of Physics and Astronomy, University of St
Hof 1, 8093 Zurich, Switzerland
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7
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24
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