Leng et al.

Light: Advanced Manufacturing (2024)5:5 Official journal of the JHL 2689-9620

https://doi.org/10.37188/lam.2024.005 www.light-am.com

Review Open Access

Meta-device: advanced manufacturing

Borui Leng1 , Yao Zhang4 , Din Ping Tsai1,2,3,* and Shumin Xiao4,5,*

Abstract
Metasurfaces are one of the most promising devices to break through the limitations of bulky optical components.
By offering a new method of light manipulation based on the light-matter interaction in subwavelength
nanostructures, metasurfaces enable the efficient manipulation of the amplitude, phase, polarization, and
frequency of light and derive a series of possibilities for important applications. However, one key challenge for the
realization of applications for meta-devices is how to fabricate large-scale, uniform nanostructures with high
resolution. In this review, we review the state-of-the-art nanofabrication techniques compatible with the
manufacture of meta-devices. Maskless lithography, masked lithography, and other nanofabrication techniques are
highlighted in detail. We also delve into the constraints and limitations of the current fabrication methods while
providing some insights on solutions to overcome these challenges for advanced nanophotonic applications.
Keywords: Meta-device, Metasurface, Nanofabrication, COMS-compatible fabrication

Introduction two-dimensional interface. These desirable features reduce

Metasurfaces are artificially designed electromagnetic the intensity attenuation caused by material absorption and
components with subwavelength scale unit structures. It is improve the working efficiency of metasurface-based
a novel functional device that can reshape optical devices with more degrees of freedom for optical response
nanoscale properties, commonly named meta-devices. manipulation. In 2011, metasurface was experimentally
Traditional optical devices mainly utilize optical path verified, achieving unparalleled anomalous optical
accumulation to cause reflection, refraction, and diffraction manipulation in the infrared band and began to receive
of light, often requiring support from larger sizes and widespread attention from scholars1. In the following
precision optical processing methods. Unlike the decade, the fundamentals, design, fabrication, and
macroscopic structure of traditional optical components, applications of metasurface have been well studied. Many
metasurfaces are special two-dimensional metamaterials applications can be realized based on meta-devices. By
with the advantages of being flat, ultra-thin, lightweight, controlling the phase of the incident light, metasurfaces
and compact, etc. By designing the geometry and layout of have realized beam steering1–3, imaging4–10, hologram11–16,
nanostructures, metasurfaces can simultaneously tailor the and vortex beam generation17, etc. Polarization control and
amplitude, phase, and polarization of incident waves at the analysis were demonstrated in metasurfaces by adopting a
polarization-sensitive unit cell design18–21. By carefully
Correspondence: Din Ping Tsai ([email protected]) or Shumin Xiao
([email protected])
manipulating the optical resonance, applications such as
1
Department of Electrical Engineering, City University of Hong Kong, lasing22–25, and sensing26,27, are exhibited. Thanks to the
Hong Kong, 999077, China great design flexibility of metasurface, they have also been
2
Centre for Biosystems, Neuroscience and Nanotechnology, City
applied to tunable devices28–31, artificial intelligence (AI)
University of Hong Kong, Hong Kong, 999077, China
Full list of author information is available at the end of the article.
enhanced meta-devices32–37, communications38,39, biomedical
These authors contributed equally: Borui Leng, Yao Zhang applications40–44, quantum light sources45, and other novel

© The Author(s) 2024

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Leng et al. Light: Advanced Manufacturing (2024)5:5 Page 2 of 16

applications. heavily desired to fully utilize the advantages of

Compared with conventional metamaterials, the metasurface.
reduction in structural dimensions has significantly reduced In this review, we focus on the recent advances in the
the complexity of metasurface fabrication. Thanks to the fabrication technologies for meta-devices. First, we
well-developed nanofabrication technologies, metasurfaces introduce maskless fabrication methods such as electron
can be patterned using techniques widely used in beam lithography, focused ion beam lithography, and laser
semiconductor integrated circuit manufacturing, such as lithography. Second, we discuss mask-required fabrication
electron-beam lithography46–48, laser direct writing49, and techniques, for example, photolithography, nanoimprint
photolithography50. To meet the repaid demands for lithography, and self-assembly lithography. Third, we
nanofabrication of meta-devices with various requirements, illustrate other meta-device fabrication technologies, such
more techniques have been developed and applied in the as two-photon polymerization lithography and laser
fabrication of metasurface, such as self-assembly51 and ablation. The merits and challenges of these methods are
nanoimprint lithography52,53. Additional fabrication steps summarized. Finally, we discuss the future perspective of
are usually required to transfer patterns to the working meta-devices and their corresponding advanced fabrication
layer of the metasurface. The process of pattern transfer technologies.
utilizes top-down etching process or bottom-up deposition
and stripping processes. The etching process helps build Nanofabrication Methods
dielectric metasurfaces with high aspect ratios, and The fabrication of meta-devices is a COMS-compatible
recently, there have been works to develop a tilted etching progress. To the authors’ knowledge, a majority of
process which demonstrates the flexible characteristics of nanofabrication techniques used in semiconductor
the metasurface and produces unique functionalities. industries can be applied to the manufacturing of
However, challenges still lie in the research of metasurface. metasurfaces. These technologies are divided into three
For example, high throughput fabrication with low cost and categories: maskless lithography, masked lithography, as
high resolution is still challenging. In the meantime, well as other technologies that have gained attention with
despite the ultra-compact nature of metasurface, most the emergence of metasurfaces. The comparison between
works still combine metasurfaces with other bulky different fabrication technologies is summarized in Table 1
elements. Compact metasurface integrated systems are to facilitate the reader’s quick review. The categories are

Table 1 Summary of metasurface fabrication methods

Strength Weakness

Low throughput
E-beam lithography High resolution
High cost

High resolution Low throughput

Focused ion beam lithography One-step fabrication High cost
Maskless Freeform patterning Ion contamination
lithography
Low cost
Laser direct write lithography None batch production
Large area

Large area
Laser interference lithography Periodic patterns only
Low cost

Large area
Photolithography High cost
High throughput

High throughput
High resolution master mold
Masked Nanoimprint lithography Low cost
Residual imprint layer
lithography Large area

Large area
Periodic patterns only
Self-assembly lithography Low cost
Mask defects
Simple

Two-photon polymerization
3D structure patterning Low throughput
Other Lithography
techniques Low cost
Laser ablation Uniformity
High throughput
Leng et al. Light: Advanced Manufacturing (2024)5:5 Page 3 of 16

derived based on the way the subwavelength-scale patterns the proposed meta-lens, as depicted in Fig. 1a. In the first
are first created. Fabrication steps that help pattern transfer, step, a layer of GaN, which acts as the desired meta-atom
for example, etching procedures, are included in the layer, is grown on the sapphire substrate by metalorganic
discussion of fabrication process flow and only a few chemical vapor deposition (MOCVD). Then, a SiO2 layer,
outstanding etching works are highlighted here. which serves as a hard mask for etching high aspect ratio
GaN nanopillar, is deposited by plasma enhanced chemical
Maskless lithography vapor deposition (PECVD). In the third step, a layer of
resist is spin-coated on the SiO2 layer. After exposure
Electron-beam lithography under EBL, followed by the development process, a layer
Electron-beam lithography (EBL) is one of the most of chromium (Cr) is deposited using e-beam evaporation.
common fabrication techniques used in the manufacture of The pattern is transferred to the Cr layer after the lift-off
metasurface. A focused electron beam is directly adopted process. The SiO2 layer is then dry etched using reactive
to define the nanostructure patterns on the electron beam- ion etching (RIE) with Cr as the etching mask. Using
sensitive resist. EBL provides the desired patterns with etched SiO2 layer as a hard mask, the GaN is etched by
ultra-high resolution in a mask-free exposure process. inductively coupled plasma reactive ion etching (ICP-RIE).
Depending on the metasurface design, further fabrication After removing the remaining SiO2 layer using buffered
steps (e.g., etching) are generally required to transfer the oxide etch (BOE), the desired nanostructures that provide
EBL-defined pattern to the target working layer. the required optical response are finally defined. Fig. 1b
Wang et al. proposed a broadband achromatic meta-lens shows the scanning electron microscope (SEM) images of
working in the visible region54. EBL is adopted to fabricate the fabricated achromatic meta-lens with a numerical

a b

PR
SiO2 SiO2
GaN GaN GaN
Sapphire Sapphire Sapphire Sapphire

Double-polished sapphire MOCVD Hard mask deposition Spin-coating resist 500 nm

SiO2 SiO2
GaN GaN GaN
Sapphire Sapphire Sapphire Sapphire

EBL & development Metal evaporation Hard mask etching ICP-RIE & BOE 500 nm
& lift off

200 nm 1 μm

1 μm 1 μm
0.5 μm
Fig. 1 Electron-beam lithography. a The process flow for the fabrication of GaN achromatic meta-lens working in the visible. b The corresponding
SEM images of GaN nanopillars (top) and the inverse nanostructures (bottom)54. c The tilted view SEM images of the TiO2 nanostructures,
including circular pillars, crosses, and rectangle pillars9.
Leng et al. Light: Advanced Manufacturing (2024)5:5 Page 4 of 16

aperture (NA) of 0.15. The GaN nanopillars and the removed by the lift-off process. After dry etching the
inverse nanostructures are seen from the SEM images. The silicon substrate using CF4, the planar metal nanostructures
minimum feature size of the design is 45 nm, proving that are spontaneously folded by the higher tensile stress in the
EBL can offer high-resolution fabrication. top Au layer than in the bottom Ni layer. The fabricated
Titanium dioxide (TiO2) is currently one of the most fourfold-symmetric SRRs are exhibited in Fig. 2e. The
commonly used materials for metasurfaces in the visible proposed metamaterial shows great potential in generating
and near-infrared bands, but most of the preparation of a bi-anisotropic response. These fabrication techniques also
TiO2 metasurfaces still used the bottom-up atomic layer apply to other lithography methods for complex pattern
deposition (ALD) on EBL patterned resist, followed by dry creation.
etching the top TiO2 layer and removing the residual EBL also acts as a one-step fabrication technique
resist55,56. The height and aspect ratio of nanopillars without further pattern transfer steps. Huang et al.
prepared by this method are limited to 600 nm and 15, experimentally demonstrated an all-dielectric metasurface
respectively. Despite the seemingly high aspect ratio given supporting ultrahigh Q resonance61. In their design, a
by this method, the allowed fabrication limit is only patterned resist, ZEP520, is directly utilized as the top
suitable for Huygens metasurface57,58 and propagation- perturbation structure, which avoids the etching steps and
based metasurface. A much higher aspect ratio is preferred ensures a higher fabrication accuracy. However, unlike
for applications such as chromatic aberration elimination. conventional photolithography, EBL is a pixel-by-pixel
Xiao et al. have redeveloped a more efficient top-down dry technology, which means EBL only writes a small pixel at
etching method for TiO29. Similar to the preparation a time. The high cost, long processing time, and highly
process in Fig. 1a, the metasurface pattern is applied to the stable requirements prevent EBL from large area and high-
resist using EBL, and then the pattern is transferred to the volume manufacturing. Owing to the electron scattering in
Cr layer through the lift-off process. The dry etching the resist and substrate, the resolution of EBL is mainly
method by RIE is used to obtain the TiO2 nanostructures determined by electron scattering instead of beam size of
array. As shown in Fig. 1c, the structure has almost vertical incident electrons62.
sidewalls with record-high aspect ratios of 37.5. This
etching technology provides strong support for the large- Focused ion beam lithography
scale and efficient production of TiO2-based meta-devices. Instead of using electrons to expose the surface resist,
More complicated geometries can be realized by focused ion beam (FIB) lithography applies heavy ion
combining other techniques with the EBL process. Chen et beams to bombard the sample surface, resulting in the
al. developed a kind of metasurface based on TiO2 with direct removal of neutral and ionized atoms from the
inclined nanopillar distribution by combining EBL and RIE surface63. FIB provides a maskless one-step milling process
dry etching techniques59. The process flow is shown in with nanometer-scale precision. Through the combination
Fig. 2a. EBL is still used to pattern the trapezoidal arrays in of FIB with SEM to form the dual-beam system, direct
the resist, and the pattern is then transferred to the Cr layer imaging and analysis of the target sample can be realized.
through dry etch by ICP-RIE. In the RIE dry etching step, Tseng et al. experimentally realized a 3D chiral
the etched sample is tilted and covered with Faraday cages metasurface by FIB adopting gallium ions64. As illustrated
to orient the plasma distribution on the sample surface. in Fig. 3a, the metasurface consists of an array of
Fig. 2c shows the side-view and cross-sectional SEM Archimedean spiral lines made of Si3N4/Au bilayer film.
images of the inclined metasurface. The use of adjustable The Archimedean spiral patterns are obtained by one-step
tilt etching technology breaks the traditional mirror milling across both Si3N4 and Au thin film using FIB. Due
symmetry of metasurfaces, unleashing the flexible to the stress and defects introduced in the milling process,
characteristics of metasurfaces, and providing innovative the planar spiral lines stretch towards the out-of-plane
ideas for the development and application of meta-devices. direction and form the 3D ones. The top and tilted SEM
3D nanostructures are also possible with advanced dry images of fabricated spirals are shown in Fig. 3b. The
etching technologies. An uniaxial isotropic metamaterial linewidth of the spiral is 80 nm. Materials, film thickness,
composed of 3D metallic split-ring resonators (SRRs) is quality of the ion beams, and milling directions determine
experimentally demonstrated by EBL process, as given in the final geometry of the 3D nanostructures. The
Fig. 2d60. A layer of positive e-beam resist, PMMA, is spin- experimental results show that the spirals have strong
coated on the silicon substrate, followed by EBL process to chiral dissymmetry over a broad infrared region and can be
define the ring pattern. Au/Ni double metal layers are applied to chiral photomechanical sensors. The shape of
deposited on the patterned sample. Additional Au/Ni are 3D nanostructures can further be precisely manipulated by
Leng et al. Light: Advanced Manufacturing (2024)5:5 Page 5 of 16

a (1) Film deposition (2) EBL and development (3) Cr film etching b RF source
PMMA
Cr
TiO2
SiO2 Ion beams

Screen

Sapmle Aperture

(4) Slanted RIE etching (5) Cr film remove (6) PMMA cover Wedged substrte

c
φ=0.1

d e− beam
e

PMMA

Si

Ni/Au
Au Lift-off

Ni

g
CF4 plasma
d h

25 μm

Fig. 2 Electron-beam lithography. a The process flow for the fabrication of inclined metasurface. b Schematic illustration of the slanted RIE
system. c Side-view (left) and cross-sectional (right) scanning electron microscope images of inclined metasurface. Scale bar, 300 nm59. d The
fabrication process for 3D SRR using EBL. e The SEM images of 3D SRRs with four-fold symmetry60.

controlling the ion beam irradiation65. patterns with vertical side walls, the meta-atoms have
FIB shows its great potential in etching difficult-to-etch geometry with smoothly varying height and four-fold
materials. For example, lithium niobate (LN) is hard to rotational symmetry. Gholipour et al. also adopted FIB in
etch and faces challenges in realizing vertical sidewalls and the fabrication of a perovskite metasurface72. FIB is a more
large etching depth66–69. Fig. 3c depicts the SEM images of flexible patterning method than EBL. However, it suffers
an LN metasurface, which boosts the second harmonic in from high costs and low throughput and cannot be applied
the visible region70. The LN thin film is milled directly by to massive manufacturing. Ion doping, sample damage, and
FIB. The side walls of LN nanopillars have an angle of sample displacement during milling will degrade the
83.6°. performance of the fabricated samples.
FIB is suitable for freeform surface patterning.
Gorkunov et al. show a chiral metasurface on crystal Laser Lithography
silicon film fabricated by digitally controlled FIB71, as Despite the high resolution of patterning with focus
given in Fig. 3d. The SEM images show that, instead of flat beams of particles, maskless fabrication techniques with
Leng et al. Light: Advanced Manufacturing (2024)5:5 Page 6 of 16

a b
80 nm
Ion
beam

500 nm
Ion beam
Air
Si3N4 (50 nm)
Au (50 nm) 1 μm 1 μm
Air
80 nm

c P
d

Si
z Al2O3
y 500 nm
600 nm
x
Fig. 3 Focused ion beam lithography. a Schematic of Archimedean spiral metasurface fabrication process by FIB. b The corresponding top (left
panel) and tilted (right panel) SEM images of the fabricated metasurface64. c SEM images of LN maetasurface for second harmonic enhancement70.
d Schematic configuration of the metasurface unit cell and the corresponding SEM images71.

flexibility, high throughput, and large-area fabrication are of a metasurface beam splitter77. The periodic grating
heavily desired. The direct application of laser into pattern nanostructures are fabricated by LIL. More complicated
writing provides a competitive solution. structures other than periodic line shapes can be realized
Laser direct writing (LDW) lithography is a common via LIL. Berzinš et al. experimentally show metasurface
technology adopted in mask writing in the semiconductor supporting Mie resonance using four-beam LIL78. The
industry. As it is named, LDW applies laser to expose the fabrication setup is given in Fig. 4d. A diffractive optical
photoresist directly. The exposure position is controlled by component is applied to split the incident light into four
the moving stage. Zhang et al. demonstrated a plasmonic beams, which reach the sample surface after passing
metasurface by LDW73. After the multiple depositions of through the lens system. The four beams interfere and form
gold, GST, and MgF2 films on the glass substrate, followed a square-shaped lattice pattern. Single pulse laser is
by spin-coating the photoresist, the laser beam writes on adopted to provide high power for melting the silicon thin
the top to define the geometry of the plasmonic film. As shown in Fig. 4e, the melted silicon diffuses to the
nanoantenna. Fig. 4a shows the SEM image of the dark region in the interference and reshapes to a hemi-
plasmonic metasurface. The metasurface achieves spherical configuration to minimize the surface energy.
reconfigurable beam shaping within wavelengths ranging The SEM images of the intermediate and final pattern of Si
from 8.5 μm to 10.5 μm. Based on the LDW technique, an nano-resonator are depicted in Fig. 4f. Despite the fact that
all-dielectric metasurface which produces polarization- more complex configurations can be fabricated by applying
sensitive optical vortices is also fabricated74. As given in more interference beams or controlling the beam intensity
Fig. 4b, Si nanorods with various geometric configurations distribution79, LIL still cannot draw arbitrary or non-
are clearly observed. The expense for LDW technique is periodic patterns.
relatively low. Through the integration with other optical
components, such as spatial light modulators (SLM), large- Masked lithography
area manufacturing with high throughput is realized75,76.
However, each sample must be prepared independently, Photolithography
making it difficult to carry out large-scale batch Photolithography, as the most widely used
production. nanofabrication method in semiconductor industries, is
Laser interference lithography (LIL) applies two or more compatible with the manufacturing of metasurfaces. This
coherent laser beams to create interference patterns with method uses light passing through the patterned photomask
bright and dark regions. Such configurations ensure large- to transfer patterns to the photo-sensitive photoresist. An
area periodic nanostructure manufacturing without the additional focusing lens can be applied to demagnify the
requirement for masks. Fig. 4c illustrates the SEM image feature size. Park et al. fabricated meta-lenses with a
Leng et al. Light: Advanced Manufacturing (2024)5:5 Page 7 of 16

a b 10 μm
c

200 nm

1 μm
10 μm
10 μm

d SHG Attenuator e Laser energy density/temperature

module
Mirror
Laser 532 nm Film Intermediate Mie resonators
1064 nm,
300 ps Local Mass
minimum center R
Beam expander
Mirror
Local
maximum
(hotspot)
Mirror
Diffractive Intensity pattern Lowest surface energy
optical element h Surface diffusion & hydrodynamic flow R
2 3
a-Si p-Si p-Si
Lens
Glass Glass Glass
1 4
Spatial
filter θ f

Lens

Positioning
table z P
y x
Fig. 4 Laser lithography. a SEM image of plasmonic metasurface fabricated by LDW73. b SEM image of the LDW-fabricated dielectric
metasurface for optical vortices generation74. c SEM image of metasurface beam splitter manufactured by LIL77. d Schematic setup for four beam
interference lithography. e, f Schematic of dewetting process for Mie resonator formation e and the corresponding SEM images f. Scale bar:
1 μm78.

diameter of 10 mm on a 4-inch fused silica wafer using a diameter of 80 mm, which exceeds the maximum
248 nm KrF deep-ultraviolet (DUV) projection exposure area for DUV. Multiple exposures are adopted to
lithography80. Fig 5a depicts the fabrication process of the obtain the full meta-lens pattern. After dry etching through
meta-lens. A layer of Chromium (Cr) is first deposited on the silicon film, the meta-lens is fabricated. The
the fused silica wafer, followed by DUV photoresist photograph and SEM images of the wafer-scale meta-lens
coating. After projecting the photoresist using DUV are given in Fig. 5d. The stitching errors are observed at
lithography, the patterns with 4:1 reduction of the feature the edges between the exposing areas, but the errors cause
size on the reticle are transferred to the resist layer. The Cr little effect on the optical performance of the meta-lens.
layer is dry etched to serve as a hard mask for silica Fig. 5e shows a 2 mm meta-lens made on a 12-inch wafer
etching. After removing the residual Cr, the silica with the corresponding SEM images given in Fig. 5f82. 193
nanopillars with a height of 2 μm are obtained. The optical nm ArF DUV immersion lithography is adopted for pattern
image of the whole silica wafer and the SEM image of the definition. Other meta-devices are also fabricated on the
corresponding nanostructures are shown in Fig. 5b. The same wafer, as given in Fig. 5e. Photolithography provides
tapered side wall is caused by plasma etching on the hard a way for large-scale, massive production of meta-devices.
mask layer. However, DUV lithography has limited resolution, and a
Photolithography has the potential for large-area shorter wavelength is desired to make metasurface with
fabrication with a high volume. Fig. 5c illustrates the finer feature sizes, such as extreme-ultraviolet (EUV)
process flow for wafer-scale meta-lens81. The meta-lens has lithography, which increases the cost dramatically.
Leng et al. Light: Advanced Manufacturing (2024)5:5 Page 8 of 16

a b
4-inch glass wafer

Cr deposition DUV lithography Resist develop Dry etch Cr

(resist as etch mask)

2 μm

Strip resist Dry etch SiO2 1 μm

Dry etch residual Cr
(Cr as etch mask)

c λ=248 nm e

Central die

e
ticl
Re

90° 90° 90° 5 cm

ns
tiv e le
jec
Ob

DUV lithography Dry etch

r Amorphous silicon
fe
Wa
Fused silica

d f

10 μm 1 μm

Fig. 5 Photolithography. a Process flow for fabricating large area all-glass meta-lens using DUV. b The corresponding optical image of meta-
lenses on full 4-inch wafer and the SEM image of meta-lens80. c The fabrication process for 80 mm meta-lens with multiple exposures by DUV.
d The optical image and the SEM images of the meta-lens81. Scale bar: 1 μm (middle), 2 μm (right). e Meta-lens and other meta-devices on 12-inch
wafer manufactured by 193nm DUV. f The corresponding SEM images of the meta-lens82.

Nanoimprint lithography indicated in Fig. 6a. A soft mold with an inverse pattern is
Nanoimprint lithography (NIL), unlike fabrication replicated from the master mold. The resin containing Si
techniques mentioned previously, creates patterns on the particles is coated on the soft mold. Then, the soft mold is
imprint resist through mechanical deformation. A patterned pressed with the substrate under high temperature to cure
master mold is contacted to the resist-coated substrate. By the resin. After demolding the soft mold from the substrate,
applying certain pressure with heat (Thermal-NIL) or UV the original patterns on the mater mold are replicated to
light (UV-NIL), the resist is cured with an inverse pattern form the desired meta-lens. The SEM images of mater
against the master mold. NIL provides an alternative high- mold (left), soft mold (middle), and meta-lens (right) are
volume fabrication method with cost efficiency. To extend depicted in Fig. 6b. The same idea for refractive index
the lifetime of master mold, additional soft molds are increasing in resin also applies to the visible spectrum,
usually utilized as intermediate molds to transfer patterns where TiO2 nanoparticles are mixed with resin84.
to the resist. Chen et al. demonstrated a chiral bilayer meta-device
Yoon et al. use one-step NIL to print the meta-lens using the printing method85. The process flow for
working in the near-infrared region83. Thermally printable fabricating bilayer patterns using NIL is shown in Fig. 6c.
resin with Si nanoparticles embedded in it is utilized to A layer of SU-8 is first deposited on the glass wafer and is
increase the refractive index of the nanostructures, which cured to serve as adhesive layer. A second SU-8 layer is
enables a higher optical efficiency. The process flows are imprinted with UV light to replicate the inverse pattern
Leng et al. Light: Advanced Manufacturing (2024)5:5 Page 9 of 16

a Pressure & heat

Master mold Substrate

Mold replication Nanocomposite coating Priting Demolding Complete

PDMS h-PDMS Si nanoparticle Resin (before annealing) Resin (after annealing)

2 μm 2 μm 2 μm

c Bottom layer d
90 °C, 30 bar
65 °C, 2 min UV off, UV on, UV off
95 °C, 2 min 65 °C, 2 min 1 min each
365 nm photons, 1 min 95 °C, 2 min 150 °C, 10 min
150 °C, 10 min
tamp
20 sccm O2, 0.13 mbar, 80 W, 40 s ted s
e-coa
Silan
lay er
sive SU8
adhe
SU8 Glass

2 μm
Coat 180 nm thick SU-8 on glass Coat 350 nm thick SU-8 on top Imprint with ultraviolet (UV) Thermal treatment

Stack top layer

20 sccm O2, 0.13 mbar, 365 nm photons, 45 °C, 5 bar, 10 s
80 W, 40 s 80 °C, 40 bar, 2 min 150 °C, 10 min

SU8 stamp
ated
e-co
Silan
Coat 350 nm thick SU-8 on Plasma treatment of Reversal imprint onto bottom Thermal treatment 1 μm
glass silane-coated IPS as top layer bottom layer layer with twist angle

Fig. 6 Nanoimprint lithography. a The process flow for one-step NIL on meta-lens fabrication. b The SEM images of master mold (left), soft mold
(middle), and fabricated meta-lens (right)83. c The NIL fabrication process for bilayer chiral meta-device. d The corresponding top and cross SEM
images of bilayer meta-device85.

from stamp. For the top layer, SU-8 is directly coated on experiment is performed, which indicates that high feature
the stamp with UV exposure to crosslink the SU-8. After fidelity is maintained for at least 15 imprints per stamp.
inverting the coated stamp with a twisted angle, the SU-8 NIL for large-area metasurface fabrication is also
layer is detached to form the bilayer magic angle pattern. successfully demonstrated. Kim et al. reported cm-scale
The top and cross-section SEM images are illustrated in meta-lenses fabrication on 12-inch wafer by one-step
Fig. 6d. NIL87. A thin layer of TiO2 is deposited to compensate for
Einck et al. developed ink mixed with TiO2 the low refractive index resin. NIL is also applied to
nanoparticles for UV-NIL fabrication86. A meta-lens pattern definition followed by etching process. A full-color
working in visible wavelengths is demonstrated to verify reflective metasurface was realized with NIL only for resist
the performance of the TiO2 ink. Fig. 7 shows that a meta- patterning88. A silicon meta-lens using NIL only for etching
atom with aspect ratio larger than 8 is experimentally mask definition was also performed89. NIL is a competitive
achieved. Shrinkages on the nanostructures are found, candidate for high-resolution massive manufacturing.
which is due to the nature of sol-gel imprint materials. The However, a high-resolution mold fabricated by other
shrinkages are reduced to about 10% by mixing the technology is required before processing the NIL
materials with solid TiO2 nanoparticles. A lifetime fabrication. The low refractive index of imprinting
Leng et al. Light: Advanced Manufacturing (2024)5:5 Page 10 of 16

Master 100 nm Imprint 1 136 nm Imprint 10

30 μm 30 μm 30 μm

Imprint 15 Imprint 15

30 μm 20 μm 3 μm

5 μm 1 μm

Fig. 7 Meta-devices fabricated by NIL. SEM images of multiple imprinted metasurfaces using the same mold86.

resin/ink limits their light manipulation capabilities. This of PS monolayer, PS coated substrate is then inserted into
issue can be improved by adding high-index particles into DI water with PS staying on the air-water interface while
the low-index resin83,86. The residual imprint layer is the substrate is sunk to the bottom. Another hydrophilic
unavoidable and requires additional etching steps to substrate is applied to scoop the monolayer and form a
remove it90. Lately, it was shown that the residual layer can high-quality monolayer mask on the substrate. The pattern
also be utilized under specific designs. Instead of the is transferred to the substrate, followed by etching steps
tedious removal process of the residual layer, Kim et al. with PS as etching mask. The SEM images of the PS mask
used the residual layer as an antireflection layer by (top) and the fabricated sample (bottom) are shown in
optimizing its thickness91. Fig. 8b.
Zheng et al. developed a novel manufacturing method
Self-Assembly lithography based on the combination of nanosphere self-assembly and
Self-assembly lithography is a simple nanofabrication grayscale lithography94. Fig. 8c and Fig. 8d depict the
method which controls the assembly of micro or fabrication process of the metasurface and the SEM images
nanoparticles to form the devices92. Nanosphere of patterned bilayer photoresist, respectively. By using
lithography (NSL) provides a low-cost solution to build self-assembled nanospheres on the surface of the
hard mask consisting of self-assembled colloidal photoresist as microlenses for grayscale lithography, the
nanoparticles for the following pattern transfer steps. exposure area under each nanosphere can be precisely
Polystyrene spheres (PS) are usually adopted as the controlled by adjusting the exposure dose, thus obtaining
nanospheres for a hard mask. Fig. 8a shows a PS sphere masks with different sizes, as shown in Fig. 8e. Using this
mask-making process with high monolayer quality93. PS technology, fabrication of large-size meta-lenses and
mixed solution, which is typically available as an aqueous holograms is achieved. Fig. 8f shows the optical image of
suspension, is injected into the substrate and forms PS the meta-lens and the tilted SEM image of partial
monolayer at the air-liquid interface. To ensure the quality nanopillars.
Leng et al. Light: Advanced Manufacturing (2024)5:5 Page 11 of 16

a i b

Mixed PS Interface ii
solution line
Water

20 μm 5 μm
iii iv v

Sink

Insert Scoop

1 μm 500 nm

c Self-assembly UV exposure d
microsphere monolayer
Double layer photoresist
Silicon on substrate

Silicon LOR 1A Nanosphere

Quartz S1805 Al2O3

Reactive ion etch Lift off Hard mask deposition Develop

e 600 f
Fitting
Measured
500
Mask diameter (nm)

400

300

200
50 100 150 200 250
Grayscale level (a.u.)
Fig. 8 Self-Assembly lithography. a Schematic diagram of mask making for self-assembly lithography. b SEM images of PS mask (upper) and the
fabricated metasurface (bottom)93. c The fabrication process of the nanosphere self-assembly assisted grayscale lithography process step. d Cross-
sectional SEM images of bilayer photoresist structure before lithography (upper) and after lithography (bottom). Scale bar: 400nm. e The diameter
of the Al2O3 hard mask against the grayscale level of the pattern. Insets are SEM images of the hard masks fabricated under different exposure
doses. Scale bar: 500 nm. f The corresponding optical image of the fabricated large-sized meta-lens. Scale bar: 200 μm. Inset is a tilted SEM image
of the silicon nanopillars. Scale bar: 2.5 μm94.

The fabrication of complex geometry configurations is mask96. Nemiroski et al. demonstrated complex
also possible using NSL95. Instead of using monolayer PS metasurface patterning by applying multiple-angle
as common, PSs are stacked to form bilayer structures with deposition97. Self-assembly lithography is a simple but
moiré patterns. Then, the moiré pattern is transferred to the effective method for large-scale meta-device fabrication.
bottom substrate with PS bilayer as hard mask for gold However, self-assembly lithography is only limited to
deposition. This chiral metasurface has great potential for homogenous patterns, and it is hard to avoid defects on the
biochemical sensing. Tuning the deposition angle is nanoparticle array.
another way to create various patterns on a fixed PS
Leng et al. Light: Advanced Manufacturing (2024)5:5 Page 12 of 16

Other techniques Discussion

In summary, the advanced nanofabrication technologies
Two-photon polymerization lithography for meta-device fabrication are presented. The fabrication
Two-photon polymerization lithography (TPL) is a kind of meta-devices is a COMS-compatible process, indicating
of additive manufacturing method that also belongs to the that a large number of fabrication techniques used in
category of 3D printing. TPL provides rapid prototyping semiconductor industries can be applied to the fabrication
without restrictions on geometry configurations, which is of meta-devices. The fabrication techniques are divided
suitable for prototype verification and research proposes. into three categories: maskless lithography, masked
As depicted in Fig. 9a, a femtosecond laser is focused on lithography, and other techniques. The advantages and
the target resist. The exposed resin is cured only at the challenges of each method are discussed. Paying attention
focal spot, where light intensity exceeds the curing to the fabrication limit is crucial for meta-device
threshold. The uncured resin is removed in the realization. One should consider the fabrication resolution,
development process, leaving only the desired structures98. allowed writing area, cost, fabrication time, and available
Liang et al. adopted TPL for fabricating anisotropic materials to find the optimized method for performing the
plasmonic metasurface working in the middle infrared fabrication.
region99. After curing the negative resist with femtosecond Through a decade of development, meta-devices have
laser, a layer of gold is sputtered on the top to realize shown significant advancements in light manipulation
plasmonic metasurface, as shown in Fig. 9b. This compared to traditional optical devices. Novel functions
metasurface achieves sharp resonance mode in reflection and applications of meta-devices still remain to be
spectra, which significantly enhances the light-matter explored. For instance, wide field-of-view meta-lenses
have already been realized104, but a double-layer structure is
interaction. McLamb et al. presented a metasurface
required to achieve the wide field of view. A wide field of
working in the infrared spectrum fabricated by TPL, which
view realized by a monolayer meta-lens is still a challenge.
can be applied for chemical sensing and beam steering100. A
Many efforts have been devoted to the study of nonlinear
meta-grating with free-form design was also fabricated
optics combined with metasurfaces, such as nonlinear
through TPL, which acts as a polarization beam splitter in
generation105–109, nonlinear hologram110,111, and nonlinear
near-infrared101.
imaging112. Expanding the nonlinear metasurface to
vacuum ultraviolet or even extreme ultraviolet region is
Laser ablation
desired for light source miniaturization, nanofabrication113,
Laser ablation is an alternative technology with low cost
biomedical technology114, and material analysis115.
and high throughput for preparing large-area metasurfaces.
However, material loss is an unavoidable problem when
The surface material is ablated or modified using a
moving to an extremely short wavelength range. Meta-
femtosecond laser system and subsequently etched to form devices for optical vortices are also realized, which are
a periodically arranged nanoarray. Yuan et al. take expected to be implemented on orbital angular momentum
advantage of the different etching rates of the GST material multiplexing communication systems116–119. Meta-devices
in the amorphous phase and the laser-induced crystalline for quantum state manipulation have also been
phase, as shown in Fig. 9c102. The disc and ring structures reported120–122, proving the great potential of meta-devices in
of the GST material are prepared through laser ablation, quantum computing and communication.
and the GST ring resonator cell is used to carry out In the meantime, integration is the key step for
centimeter-level large-area preparation, realizing tunable metasurfaces to function as compact devices. For example,
multiband meta-absorbers in the mid-infrared spectrum, as integrating metasurfaces on optical receivers and
shown in Fig 9d. Huang et al. improved the laser ablation transmitters improves efficiency and enhances
technology named patterned pulse laser lithography performance53,123,124; integrating metasurfaces with
(PPLL), as shown in Fig. 9e103. Reflective SLM was used to electrically tunable components (MEMS, liquid crystals
phase-control the femtosecond laser for patterning, and the and heaters) achieves tunable functions125–127; integrating
roughness of the pattern boundary was improved through metasurfaces with traditional refractive optical elements,
polarization filtering. These result in the metasurface of planar waveguides, and optical fibers accurately controls
arbitrary shapes and arrangements, as shown in Fig. 9f. wavefront and dispersion128–130. It is crucial to focus on
This technology can work well in the infrared band, but improving the cost-effectiveness of integrated metasurfaces
achieving fine and highly uniform nanostructures suitable in future research.
for the visible light band is still a big challenge. To put forward the progress of meta-devices, improving
Leng et al. Light: Advanced Manufacturing (2024)5:5 Page 13 of 16

a Uncured resist Laser b

Threshold

Focal spot
Substrate
Cured resist
Absorption 3 μm 3 μm

c Ta d
Tc
500 nm

1st laser direct writing

Crystallization Crystallization spot

spot array array with ablation
crater
2nd etching
5 μm

Disk array Ring array

e f3 f3 f4 f4 f σ=0 100×

Max
HWP Beam
profiler σ=π
SLM
Lens2 Sample

Min
QWP1 Polarizer QWP2 Lens1
f2 f2
f1 f1
100×
Hi
g
for h-spe
pu ed
lse sc
sep ann 100×/0.80
ara ing
tio
n

100×

Film

Substrate

Fig. 9 Other meta-device fabrication techniques. a Schematic of two-photon polymerization98. b SEM images of plasmonic metasurface supporting
bound states in the continuum99. c Laser ablation is used to create two different shapes in the GST material, and the metasurface is obtained
through etching. d SEM images of the micro-ring structures and partial enlargement (left), as well as optical photos of the complete sample
(right)102. e Schematic diagram of the optical path of the PPLL system and high-speed scanning and separated pulse ablation. f SEM images of
fabricated structural arrays with sub-wavelength feature size and fine recast layers on boundaries. Scalar bars: 5 μm103.

existing technologies and developing novel fabrication nanoimprint lithography, is a feasible solution. They are
methods with low cost, high throughput, uniformity, the widely used techniques for microelectronics fabrication
repeatability, large area, and high resolution is desired. As with high throughput. However, as commercial lithography
for the commercialization of meta-devices, masked devices are mainly prepared for Si substrate, developing
lithography, such as DUV/EUV lithography and new progress flow to utilize high index material in the
Leng et al. Light: Advanced Manufacturing (2024)5:5 Page 14 of 16

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Acknowledgements near-ir biological imaging window. Nature Communications 12,
Authors acknowledge the support from the University Grants
5560 (2021).
Committee / Research Grants Council of the Hong Kong Special
10. Chen, C. et al. Bifacial-metasurface-enabled pancake metalens with
Administrative Region, China [Project No. AoE/P-502/20, CRF Project:
polarized space folding. Optica 9, 1314-1322 (2022).
C1015-21E; C5031-22G; and GRF Project: CityU15303521; CityU11305223;
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CityU11310522; CityU11300123], the Department of Science and
extreme angle tolerance. Light:Science & Applications 7, 78 (2018).
Technology of Guangdong Province [Project No. 2020B1515120073], and
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7005867]. S.M. Xiao acknowledges financial support from National Key
holograms from dielectric nanoarc metasurfaces. Small 15, 1900483
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Natural Science Foundation of China (Grant Nos. 62125501, and 13. Huang, Y. W. et al. Aluminum plasmonic multicolor meta-hologram.
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Projects (Grant Nos. JCYJ20220818102218040). encryption. Nature Communications 11, 5484 (2020).
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Author details
Nature Communications 13, 6687 (2022).
1
Department of Electrical Engineering, City University of Hong Kong, 16. Ren, H. R. et al. Metasurface orbital angular momentum holography.
Hong Kong, 999077, China. 2Centre for Biosystems, Neuroscience and Nature Communications 10, 2986 (2019).
Nanotechnology, City University of Hong Kong, Hong Kong, 999077, 17. Ahmed, H. et al. Optical metasurfaces for generating and
China. 3The State Key Laboratory of Terahertz and Millimeter Waves, City manipulating optical vortex beams. Nanophotonics 11, 941-956
University of Hong Kong, Hong Kong, 999077, China. 4Ministry of (2022).
Industry and Information Technology Key Lab of Micro-Nano 18. Dorrah, A. H. et al. Metasurface optics for on-demand polarization
Optoelectronic Information System, Guangdong Provincial Key transformations along the optical path. Nature Photonics 15, 287-
Laboratory of Semiconductor Optoelectronic Materials and Intelligent 296 (2021).
Photonic Systems, Harbin Institute of Technology, Shenzhen 518055, 19. Wu, P. C. et al. Versatile polarization generation with an aluminum
China. 5Pengcheng Laboratory, Shenzhen 518055, China plasmonic metasurface. Nano Letters 17, 445-452 (2017).
20. Rubin, N. A. et al. Matrix fourier optics enables a compact full-stokes
Author contributions polarization camera. Science 365, eaax1839 (2019).
B.R. Leng and Y. Zhang contributed equally to this work. B.R. Leng and 21. Liu, W. W. et al. Design strategies and applications of dimensional
Y. Zhang proposed the framework of this review. S.M. Xiao and D.P. Tsai optical field manipulation based on metasurfaces. Advanced
supervised the work. All authors contributed to the writing and Materials 35, 2208884 (2023).
discussion of the manuscript. 22. Huang, C. et al. Ultrafast control of vortex microlasers. Science 367,
1018-1021 (2020).
Conflict of interest 23. Sun, W. Z. et al. Lead halide perovskite vortex microlasers. Nature
The authors declare no competing interests. Communications 11, 4862 (2020).
24. Hwang, M. S. et al. Ultralow-threshold laser using super-bound states
in the continuum. Nature Communications 12, 4135 (2021).
Received: 30 September 2023 Revised: 27 December 2023 Accepted: 03
25. Ha, S. T. et al. Directional lasing in resonant semiconductor
January 2024
nanoantenna arrays. Nature Nanotechnology 13, 1042-1047 (2018).
Accepted article preview online: 10 January 2024
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Published online: 07 March 2024
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