Received: 20 March 2020 Revised: 5 May 2020 Accepted: 7 May 2020

DOI: 10.1002/inf2.12148

REVIEW ARTICLE

Enhancing light-matter interaction in 2D materials

by optical micro/nano architectures for high-performance
optoelectronic devices

Li Tao1 | Zefeng Chen1 | Zhiyong Li1 | Jiaqi Wang2 | Xin Xu1 |

Jian-Bin Xu1

1
Department of Electronic Engineering,
The Chinese University of Hong Kong, Abstract
Hong Kong, SAR, China Two-dimensional materials are a promising solution for next-generation
2
Shenzhen Key Laboratory of Sensor electronic and optoelectronic devices due to their unique properties. Owing to
Technology, College of Physics and
the atomic thickness of 2D materials, the light-matter interaction length in 2D
Optoelectronic Engineering, Shenzhen
University, Shenzhen, China materials is much shorter than that in bulk materials, which limits the perfor-
mance of optoelectronic devices composed of 2D materials. To improve the
Correspondence
Zefeng Chen and Jian-Bin Xu,
light-matter interactions, optical micro/nano architectures have been introduced
Department of Electronic Engineering, into 2D material optoelectronic devices. In this review, we present a concise
The Chinese University of Hong Kong, introduction and discussion of various strategies for the enhancement of light-
Hong Kong SAR, China.
Email: zfchen@ee.cuhk.edu.hk (Z. C.),
matter interaction in 2D materials, namely, the plasmonic effect, waveguide, opti-
Email: jbxu@ee.cuhk.edu.hk (J.-B. X.) cal cavity, and reflection architecture. We have outlined the current advances in
high-performance 2D material optoelectronic devices (eg, photodetectors, electro-
Funding information
Innovation and Technology Commission, optic modulators, light-emitting diodes, and molecular sensors) assisted by these
Grant/Award Number: ITS/390/18; enhancement strategies. Finally, we have discussed the future challenges and
Research Grants Council, University
opportunities of micro/nano photonic structure designs in 2D material devices.
Grants Committee, Grant/Award
Numbers: 14203018, 14204616, KEYWORDS
AoE/P-02/12, N_CUHK438/18
light-matter interaction, micro/nano architecture, 2d material, photodetector,
Raman enhancement, modulator

1 | INTRODUCTION confinement effects arising from the 2D limit impart

unique electronic and optical properties to 2D materials.
Since the discovery of graphene in 2004,1 atomically thin For instance, the band structure of monolayer graphene
2D-layered materials have attracted considerable atten- at low energies manifests a Dirac cone, which indicates
tion for applications in optoelectronic devices owing to the zero bandgap, Dirac fermion behavior of electron and
their unique optical and electronic properties.2-4 To date, low density of states.5 Apart from the zero bandgap of
various kinds of 2D materials beyond graphene, such as graphene, 2D semiconductors exhibit variable band struc-
hexagonal boron nitride (hBN), transition metal tures with tunable finite bandgaps.6-8 As the TMDC
dichalcogenides (TMDCs, for example, MoS2 and WSe2) material thickness is reduced to the 2D limit, the dielec-
and black phosphorus (BP) have been realized via tric screening effect also becomes weaker and stronger
bottom-up and top-down approaches. The large quantum Coulombic interactions occur, which results in novel
This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided
the original work is properly cited.
© 2020 The Authors. InfoMat published by John Wiley & Sons Australia, Ltd on behalf of UESTC.

36 wileyonlinelibrary.com/journal/inf2 InfoMat. 2021;3:36–60.

TAO ET AL. 37

physical phenomena, for example, valley-dependent 2.1 | Graphene

circular dichroism.9-12
Compared to conventional bulk material, 2D materials
show significant advantages for optoelectronic devices.8,13-16
First, their optical responses cover most of the electromag-
netic (EM) wavelengths, ranging from ultraviolet to ter-
ahertz, and even the microwave region.17-19 Second, the
electronic and optical properties of 2D materials can be eas-
ily tuned because of the high ratios of exposed surface
atoms.20-22 Third, conventional lattice matching is not
required in van der Waals heterostructures composed of 2D
materials while excellent electronic transport properties
remain at the interface.2,4 As a result, atomically thin-
layered 2D materials can be integrated with many other
materials and structures.23-38 However, because of their 2D
nature, the light-matter interaction length in 2D materials
is much shorter than that in the bulk counterparts, which
inherently limits the performance of the devices that use 2D
active materials.
To improve the light-matter interaction, micro/nano
optical structures can be introduced into 2D material
optoelectronic device. On integration with micro/nano
photonic structures (such as plasmonic structures, photonic
crystals, and metamaterials/metasurfaces), the EM waves
can be manipulated with flexibility, resulting in light con-
finement, directional propagation, wavelength selection,
and so on. Further, conventional optical designs (ie, wave-
guides, fibers, and reflection geometries) allow manipula-
tion of light propagation in broadband wavelength region.
In this review, we have discussed the photonic
structural designs for the enhancement of light-matter
interaction in 2D material-based optoelectronic devices
and their applications. A brief overview of the optical
properties of 2D materials is presented, following by opti-
cal designs in 2D material-based optoelectronic devices
categorized by the light harvesting mechanism: plasmonic
effect, waveguide coupling, optical cavity, and reflection
architecture. At last, we have discussed the future chal-
lenges and opportunities relating to micro/nano photonic
structural designs in 2D material devices.
The permittivity of graphene is given by the following
function39,40:
 

 2
e2
i 4ћ θ ω −ћ2EF − 2πi ln ðω + 2E2EFF=ћ2Þ
ðω − ћ Þ
ε=
ω 
−e2 kB T EF  EF 
−k T
+ + 2ln e B + 1 ,
πћðω2 + iωτ − 1 Þ kB T
where the first and second terms are the contributions
from the interband and intraband transitions, respectively.
For the interband transition, the step function θ(ω) reflects
the photon energy condition for the excitation of an elec-
tron from the valence band to the conduction band: the
photon energy should be more than twice that of Fermi
energy, ωћ > 2EF. For intraband transition, the function
reflects the free electrons model and it can be simplified to
σintra = πћðωie +jμiτj − 1 Þ . Once the permittivity/complex conduc-
2
tivity is known, the absorption and reflection as function
of wavelength can be derived according to Maxwell's
equations:
   2
 Z 0 σ 2  
R =   , A =  2  Z0 σ,
2 + Z0 σ   2 + Z0 σ 
where σ = −iεω is the complex conductivity and Z0 is
the impedance of free space. The absorption and reflec-
tion spectra are calculated according to this permittivity,
depicted in Figure 1. The absorption spectrum can be
divided into three different regions in terms of frequency:
1. For photon energy larger than twice the Fermi energy
(ωћ > 2EF), commonly in the visible to near infrared
region, the optical properties of graphene are domi-
nated by the interband transition, which provides
2.3% absorption of the incident light.41,42 In this

Visible-NIR Mid-IR THz

2 | O P T I C A L P R O PER T IES OF 2 D 60 60

MATERIALS
Absorption (%)

Reflection (%)

40 40

Relative permittivity (or dielectric constant) in electro-

20 20
magnetism is commonly used to describe how an electric
field is affected by a material, and how it influences the
0 0
charged particles in the material. In other words, the per-
1 10 100 1000
mittivity of a material reflects the light-matter interac- Wavelength (μm)
tion. In this section, we provide a brief overview of the
permittivity of three typical kinds of 2D materials, that is, F I G U R E 1 Absorption (black line) and reflection (blue line)
graphene, TMDCs and BP. spectra of graphene
38 TAO ET AL.

region, graphene can be used as a light absorption
material for broadband photodetectors and electro-
absorption modulators.
2. In the mid- and far-infrared region, the plasmonic
effect can be excited on graphene because of the nega-
tive permittivity arising from the vibration of free car-
riers. In this region, graphene is a promising material
for tunable plasmonic devices because of its tunable
carrier density and low absorption rate.
3. In the THz to microwave region, graphene exhibits
tunable reflection and absorption because of its tun-
able complex conductivity and it can function as an
active material for THz modulator. However, because
of the atomic thickness of graphene, the interaction
between the THz wave and graphene is too weak to
realize a high modulation depth.
TMDC monolayers, the two peaks with lower energy in
imaginary permittivity correspond to the excitonic oscil-
lation associated with the interband transitions at the
K (K0 ) point in the Brillouin zone, which originate from
the valence band splitting as a result of the spin-orbit
coupling. The permittivity of 2D TMDCs near the exci-
ton peak can be described as a Lorentz oscillation:
εðEÞ = 1 + E2 − Ef2k− iEγ , where Ek, fk, and γ k are the exciton
k k
energy, the oscillator strength and the linewidth of the
kth excitonic oscillator, respectively. The absorption near
the exciton peak mainly originates from the nonradiative
loss of excitonic oscillation and can be described by the
imaginary part of permittivity. The strong exciton effect
also exhibits a high reflection at the exciton peak. This is
pffiffiffi
because of the large optical impedance (1= ε ) mismatch
between the TMDC and air due to the high permittivity
(eg, the permittivity of WS2 is up to 32 at the photo
energy of 2.01 eV).

2.2 | TMDCs
The bandgaps of semiconducting 2D TMDCs can be trans-
formed from indirect to direct when they become thinner
from the bulk to the monolayer, owing to the quantum
confinement effects. The permittivity of monolayers of
MoS2, MoSe2, WS2, and WSe2 were measured by Li et al by
analyzing their reflection spectra using the Kramers-Kronig
relation.43 The reflection spectra and complex permittivity
are shown in Figure 2. For all the aforementioned four
2.3 | BP
BP has a direct bandgap that ranges from 0.3 (for bulk) to
1.5 eV (for monolayer) depending on its thickness, which
spans the near to mid-infrared regions.44-47 Typically, the
bandgap is 0.8 eV, corresponding to the telecommuni-
cation band of 1500 nm, when its layer number decreases
to three. Strong in-plane anisotropy for both optical
absorption and photoluminescence (PL) is another

MoSe2 MoS2 WSe2 WS2

Absorption (%)

20
15
10
5
0
40
30
Re (ε)

20
10
0

40
30
Im (ε)

20
10
0
1.5 2 2.5 3 1.5 2 2.5 3 1.5 2 2.5 3 1.5 2 2.5 3
Photo energy (eV) Photo energy (eV) Photo energy (eV) Photo energy (eV)

F I G U R E 2 Absorption spectra and complex permittivities of MoSe2, MoS2, WSe2, and WS2. Reproduced with permission from
Reference 43. Copyright 2019, American Physics Society
TAO ET AL. 39

feature of BP, which originates from its buckled lattice
structure. The absorption rate of few-layer BP (layer
number 1-5) is very low (<5%).44 Therefore, if BP is used
as an absorption material for optoelectronics, optical
structures should be introduced into the device to
increase light absorption and improve the efficiency. In
recent years, some BP-analogue monoelemental 2D
materials (Xenes, for example, silicene, germanene,
arsenene, antimonene, bismuthene, and tellurene) have
emerged as promising candidates for optoelectronics
because they display unique properties, such as high car-
rier mobilities, direct and tunable band structures, and
large anisotropic effects.48-51
3 | C O U P LI N G W I T H P LA S M O N I C
STRUCTURES
Metallic nanostructures with localized surface plasmon
resonances (LSPRs) have attracted considerable attention
in materials science because of the significantly boosted
local EM fields generated from the collective oscillations
of high-density conduction electrons. 2D materials, with
atomic flat surfaces, can be well coupled with the
metallic LSPR structures. Such coupling dramatically
enhances the light-matter interaction in 2D materials,
rendering great benefits for various applications, such as
light emission, photodetection, optical modulation,
Raman enhancement, biosensing, and catalysis.
3.1 | Metallic nanostructures with
plasmonic effects
LSPR occurs when the frequency of incident light
matches the resonance frequency of the collectively oscil-
lating electrons in the metallic nanostructure, as sche-
matically illustrated in Figure 3A.52 The electric field
generated upon illumination drives the mobile electrons
to move through the metal, causing polarization of the
nanostructure. The ionic background in the metal, on
the other hand, provides a “friction” force, that impedes
the carrier displacement (purple in Figure 3A). Mean-
while, the accumulation of surface charges on the metal
generates a restoring force that depolarizes the metal
charge distribution. Thus, similar to the oscillator driven
by a spring with a mass (Figure 3B), the coherent elec-
tronic cloud on the metal surface oscillates in response to

F I G U R E 3 Dynamics of metallic plasmonic structures. A, Illustration of the dynamics of a plasmonic nanoparticle under
illumination. B, Illustration of a mechanical harmonic oscillator, analogous to the coherent electronic cloud on the metal surface.
Reproduced with permission from Reference 52. Copyright 2019, American Chemical Society. C, Field distribution that affects the LSPR
frequency of different metal structures, including nanospheres (symmetric and antisymmetric plasmon modes) in different dielectric media,
nanoshells with different thicknesses, and nanorods (parallel and perpendicular polarizations) with different aspect ratios. Reproduced with
permission from Reference 55. Copyright 2006, American Physical Society
40
the external field and restoring force, with a damping
effect caused by the “friction” force.
For a sphere of radius a in the quasi-static limit
regime (the nanostructure is significantly smaller in size
than the incident light wavelength), the electric field out-
side the nanoparticle is53:
   
εin − εout 3 z^ 3z
E out ðx, y,zÞ = E 0 x^− ^
a E 0 3 − 5 ðx x + y^
y + z^
εin + 2εout r r
where εin and εout are the dielectric functions of the metal
and environment medium, respectively, E0 is the magni-
tude of the incidence electric field, x, y, and z are the spa-
tial coordinate relative to the center of the particle, r is
the distance from the center, and x^, y^, z^ are the unit
vectors. The permittivity of a metal is given as
ω20
εðωÞ = ε1 + ε2 = 1 + ωp2 − ω2 − iωγ , where ωp is the plasmonic
ffiffiffiffi
p
frequency and ωp / N (N is the free electron concentra-
tion). At a certain frequency, the real permittivity is nega-
tive ( ε1 < 0) and meets the resonance condition
ε1 = − 2εm, resulting in a highly amplified EM field local-
ized in a subwavelength nanoscale region on the metal
surface.
Typically, noble metals such as Au and Ag with high
free electron concentration (>1021 cm−3) are used for
fabricating plasmonic nanostructures in the visible and
near-infrared spectral range. The greatly enhanced and
subwavelength confined EM field caused by LSPR can
improve the light absorption, excitation rate of excitons,
and other light-matter interactions in 2D material-
plasmonic hybrid structures. Additionally, sub-
wavelength scattering in the metallic nanostructures can
enhance the coupling of light into 2D materials.54 A con-
siderable efforts has been made to develop hybrid struc-
tures of 2D materials coupled with different plasmonic
nanostructures, such as metal nanoparticles (NPs),
nanoarrays, nanotrenches, nanoprisms, and nanocubes.
The resonance frequency is affected by several factors
such as geometry, size, type of material, and dielectric
environment of the metallic nanostructures, which
allow tuning of LSPR over a wide frequency range
(Figure 3C).55 The LSPR hot spots can lie on sharp
geometry features such as tips, edges, and nanogaps in
the plasmonic nanostructures, at which the local EM
field becomes highly intense.
Various fabrication techniques, such as physical depo-
sition, chemical treatment, and electrochemical deposition
methods, have been developed to obtain hybrid structures
of 2D materials and plasmonic metallic nanostructures.
For certain applications, the nanostructures must fulfill
some specific requirements, such as high tunability of the
geometry and size of the plasmonic structures and scalable
surface areas of the hybrid structures.
TAO ET AL.
3.2 | Enhancing the optical properties
of 2D materials by plasmonic structures
Owing to the strong light-matter interaction confined in
the subwavelength region in 2D material-plasmonic
hybrid structures, the intrinsic optical responses of 2D
materials, such as PL, absorption, and nonlinear signals,
can be highly augmented. The light-matter interaction in
zÞ ,
pristine 2D TMDC material is limited by the low optical
absorption rate and PL quantum yield, resulting in rela-
tively low PL intensities. Researchers have demonstrated
that the PL intensities of monolayer TMDCs can be sig-
nificantly enhanced by the strong optical near-fields gen-
erated by plasmonic structures. The LSPR accelerates the
radiative decay rate in 2D materials and improves the PL
quantum efficiency via the Purcell effect.56 Additionally,
the radiative and nonradiative transitions of the excited
carriers in TMDCs can be tailored by LSPR, which is
highly dependent on the spacing of the 2D material and
metal plasmonic structures.57 Direct contact favors non-
radiative transition (ie, charge transfer), and leads to the
quenching of PL intensity; while appropriate spacing
favors radiative transition, and results in PL enhance-
ment. Thus, suppressing the nonradiative transition in
TMDC-plasmonic hybrid structures can further enhance
the PL intensities. Furthermore, the strong coupling of
excitons in TMDCs and plasmons leads to the formation
of exciton-plasmon polaritons, which can be observed at
room temperature owing to the large exciton binding
energy of monolayer TMDC.58-60
A simulation study showed that by designing a
plasmonic nanocavity structure Ag NPs/NiOx/Al, the
monolayer MoS2 on the cavity could absorb 37% of the inci-
dent light in the 400-700 nm spectral range, while the
absorption was only 8% for pristine MoS2.61 The optical
absorption enhancement in TMDCs by plasmonic effect is
important for the PL enhancement. By transferring chemi-
cal vapor deposition (CVD) grown monolayer MoS2 onto
Au nanoantenna patterns, the PL collected from the hybrid
structure at the resonance excitation was significantly
enhanced in its intensity (65%) with respect to the bare
MoS2.62 Further, PL peak broadening and red-shift were
observed owing to illumination-induced heating. Similarly,
the PL intensity of monolayer WS2 was reportedly
enhanced by one order of magnitude upon coupling WS2
with an Au plasmonic nanoantenna.63 By carefully design-
ing the plasmonic structures with nanogaps that highly
localized the EM field, the PL intensity from TMDCs was
boosted even higher. For example, Wu et al demonstrated a
hybrid structure of monolayer MoS2 and plasmonic
nanogaps between Ag shell-isolated NPs and Au film. The
EM field was squeezed into the nanogaps, leading to a
110-fold PL intensity enhancement.64 By adopting angle-
TAO ET AL. 41

resolved shadow deposition with an ultrathin porous
anodic aluminum oxide (AAO) mask, Hao et al fabricated
nanodimer arrays with sub-10 nm gaps, and found that the
monolayer MoS2 transferred onto the nanogap structures
exhibited 160-fold PL intensity enhancement.56 Remark-
ably, by suspending the monolayer WSe2 onto nanoscale
trenches in gold film, Wang et al reported the enhancement
of WSe2 PL intensity by a large factor of 20 000 (Figure 4A
and B).65 The simulation results clearly showed that the
EM field was highly concentrated in the nanotrenches,
responsible for the PL enhancement (Figure 4C). By using
core-shell NP structures, the 2D materials could be sepa-
rated by a thin dielectric layer, thus restraining the non-
radiative transition in TMDC and preventing the unwanted
PL quenching effect. Akselrod et al reported a nanocavity
structure consisting of Au nanocubes coated with poly-
4-vinylpyridine and an Au film spaced with a thin HfO2
layer.66 The sandwiched monolayer MoS2 showed a
2000-fold PL intensity enhancement. However, the PL
enhancement factor decreased considerably when the
spacer was either not involved or too thin, indicating that
the spacer played a key role in reducing the nonradiative
quenching pathway. The competition between PL enhance-
ment and quenching in TMDC-plasmonic hybrid structures
was intentionally tuned by changing the TMDC thickness
and size of the metal NPs.67
TMDC materials are attracting attention in nonlinear
optics owing to their broken inversion symmetry and large
second-order nonlinear susceptibility. However, the atomi-
cally thin nature of TMDCs inherently results in noticeably
short light-matter interaction lengths, and thus inefficient
nonlinear optical signals. The light-matter interaction in
TMDCs was significantly enhanced by integration with the
plasmonic structures that enable localized near-field and
thus, the nonlinear optical effects, such as second-harmonic
generation (SHG), were significantly boosted. The SHG of

F I G U R E 4 Enhancing the optical outputs of 2D materials by plasmonic coupling. A, SEM image of monolayer WSe2 transferred onto
Au film patterned with nanotrenches. Scale bar: 1 μm. B, WSe2 PL intensity map of the WSe2-plasmonic hybrid structure. Scale bar: 1 μm.
C, Simulated electric field distribution of the nanotrench with monolayer WSe2 suspended over it. Scale bar: 20 nm. Reproduced from
Reference 65 under the Creative Commons License. D, E, SEM image of monolayer WSe2 on Au film with patterned nanotrenches, and the
corresponding SHG map of WSe2 with laser polarization perpendicular to the nanotrenches. Reproduced with permission from Reference 68.
Copyright 2018, American Chemical Society
42
WSe2 was enhanced by a factor of 7000 when WSe2 was
placed on sub-20 nm Au nanotrenches (Figure 4D, E).68
Peak broadening was not observed, and the large SHG
enhancement (by three orders of magnitude) was
maintained within a large pump wavelength range
(800-900 nm). In addition, the SHG signal could be tuned
by changing the excitation laser polarization.
3.3 | Enhancing the performance of 2D
material-based photodetectors by
plasmonic structures
As discussed above, plasmonic structures result in
enhancement of light absorption in 2D materials via
strongly enhanced localized EM fields, and sub-
wavelength scattering, which augments the light cou-
pling. As a result, the photocurrent collected from 2D
materials can be boosted by coupling with plasmonic
structures. In addition, the hot electrons generated via
the plasmon decay process can contribute to the perfor-
mance improvement of 2D material photodetectors.
Graphene is an appealing candidate for high-speed
and broadband photodetection. However, the responsivity
of a pristine graphene photodetector is limited owing to
the low absorption rate (2.3% for monolayer). Coupling
with plasmonic structures is promising because it
enhances the performance of graphene-based photodetec-
tors. Fang et al reported a plasmonic antenna coupled
graphene photodetector.69 In addition to the antenna-
induced near-field, the hot electrons generated in the
antenna due to plasmon decay were transferred into
graphene, and enhanced the photocurrent. An 8-fold
enhancement of the photocurrent was detected, and the
internal quantum efficiency of the graphene-antenna pho-
todetector increased up to 20% (Figure 5A). By coupling
plasmonic Au NP arrays with graphene, Liu et al demon-
strated that the photocurrent and external quantum effi-
ciency of the graphene photodetector were enhanced by a
factor of 15.70 Furthermore, the LSPR frequency was tuned
by varying the dimensions of the Au NPs, enabling multi-
colour photodetection in graphene, while the pristine
graphene photodetector had no spectral selectivity. Chen
et al have developed a novel graphene/silicon photodetec-
tor working in the photoconductive mode with plasmonic
coupling (Figure 5B and C).71 The absorption of short-
wave infrared light (1550 nm) by graphene increased 10
times owing to the LSPR generated by the plasmonic Au
NP arrays. Additionally, the vertical graphene/silicon
junction provided a built-in field that trapped the
photogenerated electrons in graphene, resulting in a large
photoconductive gain. Owing to the synergistic contribu-
tions of plasmonics and carrier trapping, the responsivity
TAO ET AL.
of the hybrid graphene photodetector reached up to
83 A W−1 for 1550 nm light, and the speed remained
high (response time  600 ns). Ni et al fabricated a
graphene photodetector coupled with silicon quantum
dots (QDs) doped with boron.72 The QD structure not
only rendered LSPR that enhances the light coupling,
but also provided additional light absorption which led
to photogating effects in the graphene channel. As a
result, the designed QD/graphene photodetector was
highly responsive to wavelengths ranging from ultravio-
let to mid-infrared, along with high gain and specific
detectivity.
Photodetectors based on semiconducting 2D materials
also exhibit improved responsivity on coupling with
plasmonic structures. As shown in Figure 5D,E, Au
plasmonic nanostructures were coupled on a few-layer
MoS2 phototransistor.73 A 2-fold photocurrent enhance-
ment was observed in the MoS2 photodetector with 4 nm-
thick Au NPs, and a 3-fold photocurrent enhancement
was detected when coupled with periodic Au nanoarrays.
Adjusting the size of plasmonic NPs resulted in a tunable
response spectral range for the MoS2 photodetector.74
Using a highly confined gap-mode LSPR coupling, the
photocurrent collected from monolayer MoS2 was
enhanced by 880%.64 Wang et al demonstrated that in
bilayer MoS2 integrated with plasmonic antenna array
structure, the plasmon-induced hot electrons overcame
the MoS2/electrode Schottky barrier, and achieved a high
photogain of 105.75 The responsivity was as high as 5.2
A W−1 at near-infrared excitation (1070 nm). BP is a promis-
ing 2D active material for infrared photodetection, and its
responsivity was enhanced by 70% upon integration with
plasmonic bowtie structures.76 Interestingly, the polarization
selectivity of the BP photodetector coupled with bowtie aper-
tures was also enhanced, with a high anisotropy photocur-
rent ratio of 8.7. An InSe photodetector coupled with Au NP
arrays was also reported, with a photocurrent enhancement
of 1200% at a wavelength of 685 nm.77 Dual-band wave-
length detection was observed in the InSe photodetector
owing to the coupled quadrupole plasmon resonance.
Van der Waals heterostructures consisting of two differ-
ent 2D materials were fabricated to extend the photo-
detection band through interlayer transition.78 The low
light absorption of the interlayer transition can be
boosted by plasmonic structures. Figure 5F shows a WS2/
MoS2 photodiode functionalized by Au NP patterns.79
While the interlayer coupling in the WS2/MoS2
heterostructure allowed infrared absorption (with photon
energy lower than bandgaps of individual WS2 and
MoS2), the transition rate was limited.80,81 By employing
the LSPR enhancement, the infrared photoresponsivity
improved 25-fold at 1030 nm, while the response speed
remained high.
TAO ET AL. 43

F I G U R E 5 2D material-plasmonic hybrid photodetectors. A, Photocurrent measurements of the graphene-antenna sandwich

photodetector obtained along the line-scan direction with different antenna geometries. Data from the control device without an Au antenna
are also presented. The inset is a schematic of the device, with the zero point indicated. Reproduced with permission from Reference 69.
Copyright 2012, American Chemical Society. B, Schematic of the Au NP-coupled graphene/silicon infrared photodetector. C, Photoresponse
of the graphene/silicon device at various illumination powers (1550 nm) with and without Au NPs. Reproduced with permission from
Reference 71. Copyright 2017, American Chemical Society. D, Schematic of the few-layer MoS2 photodetector coupled with periodic Au
nanoarrays. E, Photocurrent vs drain voltage of the few-layer MoS2 device with and without Au nanoarrays. Reproduced with permission
from Reference 73. Copyright 2015, Wiley. F, Schematics of the WS2/MoS2 photodiode coupled with Au NPs and the absorption processes
for visible and near-infrared lights, and the switching photoresponses of the device with and without plasmonic coupling under 1030 nm
illumination. Reproduced with permission from Reference 79. Copyright 2018, Wiley

3.4 | 2D material-plasmonic hybrid
structures for molecular sensing
Surface-enhanced Raman scattering (SERS) is a promising
technique for sensitive and nondestructive analytical
detection. Conventional SERS platforms are based on
metallic plasmonic nanostructures, where the EM fields at
the hot spots are considerably enhanced. The analytes on
metallic SERS substrates show Raman signals that are
enhanced by a factor of >106. Nevertheless, the plasmonic
SERS substrates have drawbacks such as the low unifor-
mity and reproducibility of the SERS signals, photo-
bleaching effect, and other unwanted side reactions.
Recently, a few groups have found that 2D materials,
including graphene, MoS2, hBN, and MoTe2, can serve as
substrates for SERS applications.82-85 In contrast to
plasmonic structures, the SERS effects on 2D materials
mostly stems from chemical enhancement, that is, the
charge transfer between analytes and 2D materials.86 In
addition, the atomic flat surfaces enable the 2D materials
to uniformly adsorb the probe molecules. The 2D material
SERS substrates reportedly have promising uniformity,
stability and cleanness of the detected SERS signals.
When 2D materials are integrated with plasmonic
structures, the hybrid platform is expected to exhibit better
Raman enhancement for the analyte, owing to the combi-
nation of EM and chemical enhancements. Furthermore,
2D materials can serve as inert shields for protecting the
44 TAO ET AL.

metallic plasmonic structures from being oxidized, fluo-
rescence quenchers which make the signals cleaner, and
molecule enrichers (such that more molecules can be
adsorbed on the 2D material surface). Graphene-
plasmonic hybrid structures have been demonstrated to
show promising SERS detection performance.87-90 As
shown in Figure 6A, in the Au nanoisland structure cov-
ered by monolayer graphene, the LSPR created hot spots
in the nanogaps between the Au islands could pass
through the atomically thin graphene layer, rendering a
unique flat “hot surface” for SERS detection.87 The
hybrid SERS platform displayed highly sensitive, uni-
form and clean SERS responses. In contrast to the large
photobleaching induced SERS signal degradation
observed in the bare Au structure, the graphene-Au
hybrid structure provided very stable SERS intensities
against prolonged illumination (Figure 6B). The sup-
pression of photo-induced damage to the analyte was
attributed to the physical separation of the analyte and
Au by graphene, and the strong π-π interaction between
the analyte and graphene that resulted in efficient
charge transfer. A flexible and transparent SERS tape
based on the graphene-Au structure was developed as
well for real-world applications.
As an insulating 2D material, hBN has been used to
improve the SERS effect of metal structures as well.
Cai et al demonstrated that the hBN veiled Ag NP plat-
form increased the SERS sensitivity by two orders of
magnitude.91,92 Also, the high thermal and chemical
stability, impermeability, and insulating nature of hBN
made the hBN-Au hybrid structure highly stable and
reusable for SERS. Kim et al reported that hBN acted
as an atomically thin insulating shield for Au NPs,
which reduced the photocatalytic reaction
(Figure 6C).93 The strong π-π interactions gave hBN
superior molecular adsorption capability in contrast to
bare Au NPs. Thus, the number of surface adsorbed
probe molecules on the hBN-Au structure was largely
enriched, resulting in highly enhanced SERS signal
intensities (Figure 6D). This is particularly important
for the detection of specific molecules that do not
adsorb effectively on bare Au. Plasmonic metallic
structures hybridized with other 2D materials, such as
MoS2, GaTe, MXene, and 2D heterostructures also
exhibit good SERS effects in terms of sensitivity,
stability, and signal uniformity.94-97
SPR sensors have been widely adopted for investigat-
ing molecular interactions and clinical application by
monitoring the change in refractive index on the chip
surface (usually Au film).98 However, their sensitivity is
limited owing to the poor adsorption of analytes on the
Au surface. The strong molecular adsorption capacity of
2D materials provide an alternative path for sensitivity
enhancement. SPR sensors based on various kinds of 2D
materials, including graphene, TMDCs, and Xenes were
successfully applied for the ultrasensitive detection of
molecules such as DNA and miRNA, showing potential
in bio-medical applications.99-101

F I G U R E 6 2D material-plasmonic hybrid platforms for SERS. A, Schematics of probes adsorbed on conventional SERS substrate
(Au NPs) and on graphene veiled SERS (G-SERS) substrate. B, CuPc SERS signals collected from conventional SERS substrate and G-SERS
substrate under prolonged illumination time. The inset shows the Raman intensities of the CuPc characteristic peaks (953 and 1451 cm−1)
with increasing acquisition time. Reproduced with permission from Reference 87. Copyright 2012, National Academy of Sciences. C,
Schematic of the hBN shielding effect for avoiding the photocatalytic reaction on bare Au NPs. D, Schematic illustration showing probe
adsorption on bare Au NP and hBN/Au NP substrates. Reproduced with permission from Reference 93. Copyright 2016, American Chemical
Society
TAO ET AL. 45

3.5 | Optically chiral coupling of valley

excitons in TMDCs with metasurfaces

In contrast to LSPR, surface plasmon polaritons (SPPs)

can propagate along a metal/air surface. When valley
excitons in 2D TMDCs are coupled with SPP, the spin-
valley polarization lights become spatially controllable
(emission direction can be manipulated), which provides
another degree (apart from intensity) to distinguish the
valley excitons in TMDCs. A model of dipole emitter near
a metal surface can be used to describe the coupling of an
exciton and SPP at the metal surface. With a 2D geome-
try, two orthogonal dipoles px and pz are placed in a
metal groove to excite the SPP in the metal wall, as
shown in Figure 7A. The SPP field at one metal wall is
then expressed as follows102,103:

*
E n = A px + pz Γ v expð −iωt Þ
F I G U R E 7 A, Illustration of a dipole in a groove. B,

 Schematics of optically addressable valleys and spatial separation of
expðik spp x Þ valley excitons by an asymmetric groove array. C, Simulated
where Aðz,x, Þ = pffiffiffiffiffiffiffiffi expðik z,n jzjÞ expðikz,1 jdjÞ M,
  kspp x electric field intensity distribution induced by a σ + (−) dipole on
kspp
and Γ = kz,1 . The function A(z, x) represents the ampli- an asymmetric groove. D, Color plots of valley polarization contrast
tude of the SPP wave, which is related to the position of in real space measured for a MoS2 asymmetric groove array. A-D,
the dipole exp(ikz,1|d|) , and the couple constant M. The Reproduced with permission.103 Copyright 2019, Nature
Publication Group. E, Illustration of the relationship between the
index n ∈ {1,2} is used to denote air and metal, respec-
σ+(−) dipole position and propagation direction. F, Fluorescence
tively. kspp is the SPP wave-vector and kz,n is the wave-
images of the emission of valley polarized excitons (top) and line
vector in the air or in metal. The term (px + pzΓ) repre-
* * * cuts of the intensity profiles (bottom) along the silver nanowire
sents the dipole property. The wave-vector v = x − Γ z , under left right-handed circularly polarized excitation. Reproduced
describes the polarization of the SPP field. The total with permission.104 Copyright 2018, AAAS
z-component of the electric field radiated along the
groove in the forward and backward directions should
be the sum of contributions from up and down metal asymmetric groove array.103 Simulations and experimen-
walls: tal results showed that owing to the breaking of mirror
symmetry, the SPP wave excited by valley exciton σ + (−)




E zðF Þ = Aup px + pz Γ ð − Γ Þ + Adown px −pz Γ Γ expð −iωt Þ, preferentially propagates in one direction (Figure 7C and
D). The above dipole excitation mode is also suitable for



the coupling of metal nanowires and TMDC excitons.
E zðBÞ = Aup − px + pz Γ ð − Γ Þ + Adown − px + pz Γ Γ expð − iωt Þ,
where Aup and Adown represent the SPP amplitude on the
upper and lower metal walls. If the groove is symmetric
and the dipole is excited in the middle of the groove,
Aup = Adown, then |Ez(F)|2 = |Ez(B)|2, which means that
the forward and backward electrical fields are equal. If
the groove is asymmetric or the dipole is not excited
in the middle of the groove, then Aup ≠ Adown, and
|Ez(F)|2 ≠ |Ez(B)|2, which means that the propagating
direction is selective. Sun et al proposed a subwavelength
asymmetric groove array for spatially separating valley
exciton emission at room temperature, as shown in
Figure 7B, where a monolayer MoS2 covered an
When a circularly polarized emitter is excited but not at
the longitudinal center of a metal nanowire (as shown in
Figure 7E), the propagation direction of the SPP wave on
the nanowire is preferentially to a specific side. This phe-
nomenon was reported by Gong et al in an Ag nanowire
and WS2 coupling system.104 The valley-controlled direc-
tional emission was achieved by selectively exciting the
WS2 excitons along the longitudinal direction, as shown
in Figure 7E and F. The valley excitons in TMDCs have
also been coupled with spin-momentum locked surface
plasmons,105 which leads to valley-momentum locked
chiralitonic states. As a result, the valley exciton σ+(−)
can be launched in counter-propagating directions at
room temperature.104
46
4 | INTEGRATION ON
WAVEGUIDES
Integration of a 2D material on a waveguide or optical
fiber is another strategy to achieve strong optical interac-
tion. In this coplanar configuration, the interaction
length is determined by the device length, rather than
the thickness of the 2D material in the case of normal
incidence. Because the 2D material interacts with the
evanescent field of the guided mode of the waveguide,
the unit-length absorption rate is lower than that of the
normal incidence configuration. However, the interaction
length can be designed to be long enough to realize com-
plete optical absorption.
The absorbed optical power in a 2D material can be
understood as resistive
Ð dissipation (or Ohmic loss); it is
expressed as A = σ 12 E 2 ds, where σ is the real part of the
optical conductivity σ = Re( − iωε). When the 2D material
is placed on a waveguide parallel to the x-z plane and has
a width of W in the x direction and length of L in the
z direction, the absorption becomes
ÐLÐ ÐW=2
A = σ 12 0 E ðx,y,zÞ2 dxdz: 106 Figure 8A shows the
− W =2
finite-difference time-domain (FDTD) simulated absorp-
tion of the graphene/waveguide coplanar configuration as
a function of the length when graphene is on the surface
of the waveguide. It can be seen that the absorption is up
to 80% when the length is over 100 μm. The inset shows
the quasi-transverse electric (TE) mode of a typical silicon
waveguide, where the maximum electric intensity is in
the middle of the waveguide. If graphene is sandwiched
in the middle, the absorption can be further increased to
100% at a length of 100 μm, as shown in Figure 8B.
(A)
100
80
Absorption (%)
60
40
20
0 20 40 60 80 100
Length (μm)
F I G U R E 8 Simulated absorption of graphene/waveguide coplanar configuration as a function of the length when graphene is atop the
waveguide, A, and sandwiched in the middle of the waveguide, B. The insets are the electrical intensity fields of quasi-TE mode waveguide
TAO ET AL.
4.1 | Photodetector based on 2D
materials with waveguide-integration
In the waveguide-integrated coplanar configuration, the
light absorption of a 2D material is enhanced and high-
performance photodetectors can be obtained.27,28,107-112
Gan et al demonstrated a high-performance graphene
photodetector based on a waveguide-integrated configu-
ration with asymmetric electrodes,27 as shown in
Figure 9A-C. The asymmetric metal doping of graphene
led to a surface potential difference on graphene, which
could separate the photogenerated electron-hole pairs
and generate a photocurrent. The photoresponsivity of
the detector exceeded 0.1 A W−1 and a nearly uniform
response between 1450 and 1590 nm under zero-bias
operation was observed. Owing to the high carrier mobil-
ity and ultrafast electron-hole pair recombination rate, a
response speed of over 20 GHz was achieved. Wang et al
reported a mid-infrared graphene/silicon photodiode pre-
pared by integrating graphene onto a silicon optical
waveguide, in which graphene and silicon formed a
Schottky junction for extracting the photocurrent and
suppressing the dark current at room temperature.28 Ilya
et al further studied the graphene/silicon waveguide
Schottky photodiode and showed that the high response
could be attributed to both the elongated interaction
length in the waveguide integrated configuration and the
plasmonic effect of the gold electrode on the
waveguide,113 as shown in Figure 9D-F. At a wavelength
of 1.55 μm, this on-chip integrated metal graphene-
silicon plasmonic Schottky photodetector exhibited a res-
ponsivity of 85 mA W−1 at a reverse bias of 1 V. Owing to
the low dark current, this device showed a noise
(B)
100
80
Absorption (%)
60
40
20
120 0 20 40 60 80 100 120
Length (μm)
TAO ET AL. 47

F I G U R E 9 2D material-based photodetector integrated on waveguides. A, Schematic of the waveguide-integrated graphene

photodetector. Graphene is in contact with two asymmetric electrodes, which creates a potential difference in graphene. B, Top: potential
profile (black solid line) across the graphene channel. Photon-induced carriers are separated by the potential gradient around the boundaries
of the gold electrodes. Bottom: simulated electric field of the TE waveguide mode. The red line shows the electrical field intensity at
graphene. C, Photoresponsivity as a function of bias voltage. A-C, Reproduced with permission.27 Copyright 2013, Nature Publication
Group. D, Schematic of the graphene/silicon waveguide Schottky photodiode. E, Top: cross-section of the graphene/silicon Schottky
photodiode. Bottom: corresponding electrical field distribution. F, Photoresponse of the graphene/silicon waveguide Schottky photodiode
under different incident powers. D-F, Reproduced with permission.113 Copyright 2016, American Chemical Society. G, Schematic of a BP
waveguide photodetector. H, Photoresponse when the optical signal is off (black line) and at various power levels at a gate voltage of −8 V.
Inset: normalized photocurrent-to-dark current ratio. I, Broadband frequency response of the BP photodetector. G-I, Reproduced with
permission.114 Copyright 2015, Nature Publication Group

equivalent power of  1.1 × 10−12 W Hz−1/2, which is sim-
ilar to that of a state-of-the-art Si Schottky photodetector.
Similar to graphene, 2D-layered BP can also be inte-
grated with waveguides. Youngblood et al demonstrated
a gated multilayer BP photodetector integrated with a sil-
icon photonic waveguide operating in the near-infrared
telecommunication band,114 as shown in Figure 9G-I.
Unlike the high dark current of graphene due to the zero
bandgap, BP photodetectors can operate under a bias
with a very low dark current by depleting the carriers by
gating. This waveguide structure delivered an intrinsic
responsivity up to 135 mA W−1 in the 11.5 nm-thick
device with a high response bandwidth exceeding 3 GHz
at room temperature. Apart from graphene and BP, pho-
todetectors based on silicon waveguides integrated with
MoTe2 (a TMDC semiconductor with an infrared
bandgap) have also been studied.115,116
4.2 | Waveguide-integrated electro-optic
modulators based on 2D materials
The evanescent coupling between graphene and light
propagating in the waveguide enhances the optical
48 TAO ET AL.

interaction and allows high-efficiency electro-optic mod-
ulation. In the waveguide-integrated configuration, the
complex refractive index (RI) of the waveguide mode is
modulated by electrically tuning the Fermi energy of
graphene, thus leading to electro-absorption modulation
or electro-refractive modulation. In 2011, Liu et al first
experimentally demonstrated a broadband, high-speed,
and waveguide-integrated electro-absorption modulator
based on monolayer graphene,24 in which the modula-
tion was achieved by actively switching the Fermi energy
of graphene in/out of the half photon energy of the
incident light (ωћ > 2EF or ωћ < 2EF ). As shown in
Figure 10A, the silicon-on-insulator waveguide was cov-
ered by a CVD-grown graphene sheet, which was electri-
cally gated by the Al2O3 layer. When the Fermi energy of
graphene was less than half of the photon energy (middle
regime of Figure 10B), the incident light was absorbed by
graphene through interband transition, and this absorp-
tion was enhanced by the waveguide length. When the
Fermi energy was tuned to be higher than half of the
photon energy, the interband transition was forbidden,
and thus the absorption of incident light was reduced. In
the right-hand region (VD > 3.8 V), the interband
transition was also forbidden because the electrons in res-
onance with the incident photons (hν) were occupied.
The modulator showed a noticeable modulation effi-
ciency of 0.1 dB um−1 with a gigahertz modulation speed
for a broad range of wavelengths from 1.35 to 1.6 μm
under ambient conditions. Calculations from Koester
et al showed that the electro-absorption optical modula-
tor based on bilayer graphene could perform 3-dB band-
widths over 120 GHz (30 GHz) at near- (λ = 1.55 μm)
and mid- (λ = 3.5 μm) infrared bands. The bandwidth,
modulation depth, and insertion loss were highly affected
by the quality of graphene.117
According to the permittivity function of graphene,
the Fermi energy can tune both the imaginary and real
parts of the permittivity, which correspond to the absorp-
tion and RI, respectively. Therefore, with electrical gating
to tune the Fermi energy of graphene, the effective RI of
the graphene-on-waveguide mode and the phase of the
propagating light can be significantly modulated, which
is detected by interference and resonant photonic struc-
tures. Sorianello et al developed a graphene phase modu-
lator integrated in a Mach-Zehnder interferometer (MZI)
based on the electro-refractive effect,118 as shown in

F I G U R E 1 0 A, Schematic of the waveguide-integrated electro-absorption modulator. B, Static electro-optical response of the device at
different drive voltages, which is divided into three parts. C, Optical micrograph of the graphene modulator based on the MZI configuration.
A and B, Reproduced with permission.24 Copyright 2012, Nature Publication Group. D, Cross-section of the graphene modulator. E,
Extinction ratio at the bar port at a wavelength of 1550 nm. When 4.1 V and 7.25 V DC biases were applied to the shorter and larger arms,
respectively, the extinction ratio was maximized. C-E, Reproduced with permission.118 Copyright 2018, Nature Publication Group
TAO ET AL. 49

Figure 10C-E. The effective RI and optical loss of mono-
layer graphene-integrated Si waveguide could be tuned
by applying voltage to the graphene capacitor, resulting
in a phase difference between the two arms of the MZI.
The phase modulation could be tuned up to π and had a
high extinction ratio of 35 dB in the output of the inter-
ferometer. This modulation depth was much higher than
that based on the electro-absorption effect. The mono-
layer TMDC also exhibited an electro-refractive effect. By
embedding monolayer WS2 on silicon nitride waveguide
structures to enhance the light-matter interaction, a
strong electro-refractive response of WS2 at near-infrared
wavelengths was observed, which showed great potential
for application in photonic modulators.119
5 | C O U P LI N G W I T H T H E
OPTICAL RESONANCE CAVITY
The optical resonance cavity is an optical microstructure
that forms a standing wave cavity resonator for light
waves. It can realize light confinement both in space
(in cavity volume, V) and in time (long photon lifetime/
high quality factor Q), which leads to large light-matter
interaction. Consequently, this microstructure is widely
adopted in photonic circuits and optoelectronic devices.
There are three types of optical resonance cavities120: (a) a
Fabry-Perot (F-P) type cavity, where the light is reflected
multiple times by two metallic mirrors and transforms into
standing waves at specific resonance frequencies. In fact,
the metal mirror can be replaced by a Bragg mirror, for-
ming a so-called 1D photonic crystal cavity (Figure 11A);
(b) a 2D photonic crystal (PhC) cavity, which is fabricated
by introducing a dot or line defect in a 2D photonic crystal
(Figure 11B); (c) a microcavity based on the whispering
gallery mode (Figure 11C), in which light is confined by
“continuous total internal reflection (TIP)” in a dielectric
sphere or disc through the standing wave effect.
To discuss the EM wave enhancement, we have cho-
sen the F-P cavity as an example. The intensity of the EM
field in the F-P cavity can be expressed as follows121,122:
 
1 −r 2 j1 + r 2 j2
2 1 2
jE max j = 2 jE in j ,
j1 −r 1 r 2 ejð2βL + φ1 + φ2 Þ j
where r1 and r2 are the reflection coefficients of the top
and bottom mirrors, respectively, φ1 and φ2 are the
corresponding reflection phases of the two mirrors, Ein is
the amplitude of the incident light, and L is the length of
the cavity. β = 2πn/λ0 is the propagation constant in the
cavity, where n is the refraction index and λ0 is the wave-
length in vacuum. When the cavity satisfies the reso-
nance condition (2βL + φ1 + φ2 = 2mπ) and the cavity
exhibits symmetric behavior, the EM field becomes
jE max j2 = jj11 +− rr11jj jE in j2 , which is amplified by a factor of
j1 + r 1 j
j1 − r 1 j and increases rapidly as r1 increases.
5.1 | Enhancing the optical properties of
2D materials by optical cavity
When a 2D material is coupled with an optical cavity,
strong interaction between the 2D material and EM field

F I G U R E 1 1 Schematic illustrations of three typical optical resonance cavities. A, Fabry-Perot type cavity. Two metal mirrors were
replaced by Bragg mirrors (1D photonic crystals) to reduce heat loss. L is the length of the cavity and the two Bragg mirrors induce
additional reflection phases φ1 and φ2. B, Top: A 2D PhC cavity constructed by dry etching of a hexagonal array of holes with a defect at the
center. Bottom: The electrical field contribution at the resonance wavelength. C, Top: Whispering gallery microcavity based on a disk with a
high refraction index. Bottom: The corresponding electrical field distribution of the whispering gallery mode
50 TAO ET AL.

is expected, which leads to high absorption. As discussed

above, owing to the atomic thickness, only 2.3% of the
incident light can be absorbed by graphene. It was shown
that when graphene is sandwiched in a Bragg mirror F-P
microcavity, the optical absorption is enhanced 26-fold,
reaching values higher than 60% of incident light.123 The-
oretical results show that the absorption can reach almost
100% at a given frequency when graphene is integrated
into double F-P cavities.124
Owing to the strong light-matter interaction confined
in the optical cavity, the PL of 2D semiconducting mate-
rials can be highly augmented by the Purcell effect.125-129
Wu et al reported the control of excitonic light emission
of WSe2 coupled with a planar photonic crystal (PPC)
nanocavity, in which a Purcell factor of 14 for WSe2 spon-
taneous emission was found,129 as shown in Figure 12A
and B. Other optical properties (eg, SHG) of 2D materials
are also enhanced when the atomically-thick material is
coupled with optical cavity.130,131
As discussed in Section 2, TMDC materials have a
F I G U R E 1 2 A, SEM image of the photonic crystal nanocavity
unique spin-valley effect, which provides a possible plat-
covered by WSe2. B, PL of WSe2 at three locations in A. The red,
form for controlling the valley pseudo spin.9-11 However, black, and green spectra correspond to on-PhCC, on-PhC, and off-
the spin-valley effect, which is reflected by the circular PhC excitation, indicated by the red, black, and green circles in A,
polarization light of spontaneous transitions, is very weak respectively. The peak emission at 756 nm corresponds to the
and difficult to observe at room temperature. Surpris- spontaneous emission enhancement of the Purcell effect in the PhC
ingly, when the TMDC material is coupled to the optical cavity. The total PL intensity of on-PhC is also enhanced compared
cavity, in which a hybrid exciton-polariton is formed, the to that of off-PhC owing to the suspending effect of WSe2 on the
valley-polarized emission becomes observable at room hole. A and B reproduced with permission.129 Copyright 2014,
temperature,132-134 as shown in Figure 12C and D. The Institute of Physics. C, Schematic of valley-polarized exciton-
enhancement mechanism of emission polarization is as polaritons in a distributed Bragg reflector cavity. D, From top to
follows. For bare excitons, the polarization of the emitted bottom, PL spectra of MC-MoS2 pumped at 8 and 294 K, and the
polarization spectrum of MC-MoS2. The PL polarization is extracted
light is described by the rate equation of the exciton
by p = II ++ +−II−− , where I+/− is the PL intensity of right/left circularly
relaxation rates (Γ ex) and intervalley scattering rate (Γ v):
polarized light. C and D reproduced with permission.132 Copyright
p = 1 +A2Γv .132 For the exciton polariton, the emission polar- 2017, Nature Publication Group
Γ ex
A
ization becomes p = 1 + 2Γ v because the relaxation is
Γ ex + Γ c

through both the exciton and cavity channels. Generally,
the relaxation rate of strongly coupled exciton polaritons
(Γ ex + Γ c) is higher than the relaxation rate of the bare
exciton. As a result, the emission polarization increases
and can be observed at room temperature.
5.2 | Performance enhancement for 2D
optoelectronic devices by optical cavity
The optical cavity can enhance the absorption of 2D
materials via a strongly localized EM field. As a result,
the photocurrents collected from 2D materials can be
enlarged by coupling with the optical cavity.123,135-137
Furchi et al demonstrated a graphene-based microcavity
photodetector with a responsivity of 21 mA/W, which
benefited from the highly localized EM inside a resonant
cavity.123 The monolayer graphene in the Bragg cavity
showed 60% optical absorption at the resonance wave-
length, which was 26 times higher than the 2.3% absorp-
tion of monolayer graphene in free space. The
corresponding photocurrent was improved by 20 times
and showed a high wavelength dependence (Figure 13A).
The concept of enhancing light-matter interactions by
optical cavity can be applied to not only photodetectors,
but also electro-absorption modulators.26,138-140 Gao et al
demonstrated an electro-optic modulator based on a
graphene-BN heterostructure integrated with a photonic
crystal cavity.138 Light absorption was amplified by the
EM confinement effect in the photonic crystal cavity and
modulated by the electrostatic potential based on the
Pauli blockade effect in graphene. As a result, a maxi-
mum modulation depth of 3.2 dB and a response speed of
1.2 GHz were achieved in the device, as shown in
TAO ET AL. 51

Figure 13B. Integrating with an optical cavity can also
improve the performance of light-emitting diodes (LEDs).
Several groups have demonstrated the integration of elec-
troluminescence (EL) devices with various optical cavi-
ties, which can increase the EL efficiency by the Purcell
effect.141,142 Liu et al demonstrated a van der Waals
heterostructure tunneling emitting diode integrated with
a PhC cavity,142 as shown in Figure 13C. Owing to the
coupling of the in-plane dipoles of WSe2 with the TE
mode of the cavity, a 4-fold enhancement of EL was
obtained, as well as linear polarization EL along the cav-
ity mode, which was indicative of the increase in sponta-
neous emission by the Purcell effect.
6 | O P T I C A L RE F L E C T I O N
GEOMETRY
Apart from the abovementioned micro/nano photonic
structures, conventional reflection geometry (internal
total reflection and Brewster reflection) can also enhance
the interaction between the 2D material and EM field.
When the incident light is reflected, there is a Goos-
Hänchen shift at the interface, in which light travels a
small lateral propagating length LG. Under Total Internal
Reflection (TIR), the length of the Goos-Hänchen shift
can be up to λ (where λ is the wavelength of incident
light). As a result, the interaction length between the 2D
material and EM wave is greatly enlarged, from atomic
length to LG, which in turn enhances absorption.143-147 In
previous reports, although the TIR configuration is simi-
lar to the traditional surface plasmon designs, the mecha-
nisms are completely different. In the TIR modulator, the
2D material on the surface acts as a conducting layer but
is not involved in excitation of the surface plasmon wave.
Consequently, it shows an ultra-broadband response.
Harada et al have reported a significant enhancement of
terahertz-wave absorption in monolayer graphene with
TIR geometry.145 Maximum absorption (up to 70%) has
been found for s-polarized radiation when the THz beam
enters at the critical angle, as shown in Figure 14A-C.
The Goos-Hänchen shift is maximum at the critical angle

F I G U R E 1 3 A, Top: schematic diagram of a graphene microcavity photodetector; Bottom: spectral response of the graphene device
sandwiched by a Bragg cavity. The dashed lines represent the calculated reflection R (red), transmission T (green), and absorption A (blue).
The solid lines represent the measurement results: reflection (red) and photocurrent (blue). A strong and spectrally narrow photoresponse
was observed at the cavity resonance (855 nm wavelength). Reproduced with permission.123 Copyright 2012 American Chemical Society. B,
Top: Schematic diagram of the cavity-graphene electro-optic modulator; Bottom: Cavity reflection spectrum as a function of wavelength and
gate voltage. At the two resonance modes of the photonic crystal cavity, 1551 and 1570 nm, the intensity increased significantly when the
gate voltage |Vg| was increased. Reproduced with permission.138 Copyright 2015 American Chemical Society. C, Top: schematic diagram of
the van de Waals heterostructure covered by a photonic crystal cavity for emission enhancement; Bottom: The cross-polarized EL spectra
from the device at a gate voltage of 2.6 V. The blue and red spectra correspond to the along and orthogonal directions to the cavity mode,
respectively. Inset shows the microscopic image of the photonic crystal cavity. Reproduced with permission.142 Copyright 2017 American
Chemical Society
52 TAO ET AL.

and performs the largest lateral propagating evanescent
THz wave at the surface of the prism. As a result, the
interaction length between graphene and THz wave is
markedly enlarged, and more dissipation of Joule heating
occurs.
For the THz region, graphene is a promising material
for modulators because of its highly tunable conductivity.
However, because of its atomic thickness, the modulation
depth is limited. Although novel optical micro/nano struc-
tures (plasmonic effect, optical cavity, and metamaterial)
can be used to improve the light-matter interaction, the
broadband response is difficult to achieve because these
assisted strategies are based on the resonance effect of the
EM wave. In contrast, conventional optical reflection
geometry is independent of the frequency of the EM wave,
which is useful for realizing an ultra-broadband response.
When graphene is sandwiched between two media with
refraction indices n1 and n2 (n1 > n2) and the THz beam is
incident at angle θi, the reflection coefficient from the
Fresnel equation can be expressed as:
pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
n1 cosθi −i n1 2 sin2 θi −n22 −Z 0 σ g
rs = pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi ,
n1 cosθi + i n1 2 sin2 θi −n22 + Z 0 σ g
where Z0 is the impedance of air and σ g is the conductiv-
ity of graphene. It is evident that if the incident angle is
equal to the critical angle of TIR (ie, sinθi = nn21 ), the reflec-
tion amplitude can be tuned from 0 to 1 when σ g varies
from n1 Zcosθ
0
i
to 0. Based on the physical model, a broad-
band graphene THz modulator with a modulation depth
higher than 90% between 0.15 and 0.4 THz was devel-
oped by Liu et al.144 As shown in Figure 14D and E, a
THz beam was incident from one side of the quartz prism
and reflected by the quartz surface covered with
graphene. Compared to the resonance structure (eg,
metamaterials), both high modulation and broadband
response could be achieved simultaneously.
Analogous to TIR, the Brewster reflection can also
improve the performance of 2D material devices.148-151
As shown in Figure 15A, if the incident beam travels
from medium 1 to medium 2 with refraction indices n1
and n2 (n1 < n2), respectively, and a 2D material with
conductivity σ2D is sandwiched between them, then the
reflection coefficient for the p-polarization wave can be
expressed as follows:
n2 cosθi −n1 cosϕ −Z 0 σ 2D cosϕcosθi
rp = ,
n2 cosθi + n1 cosϕ + Z 0 σ 2D cosϕcosθi
where ϕ is the refraction angle. The Brewster angle in
this reflection geometry should satisfy the relation
n2cosθi − n1cosϕ − Z0σ 2Dcosϕcosθi = 0, and should be
tunable by varying the conductivity of the 2D material.

F I G U R E 1 4 A, Schematic illustration of the TIR architecture for the THz beam. The inset shows the reflection diagram at the
interface. B, Experimental and C, theoretical angular dependence of the THz output. A-C, Reproduced with permission.145 Copyright 2017,
American Chemical Society. D, Graphene THz modulator based on TIR geometry with an ion-gel gate for tuning the conductivity of
graphene. E, Corresponding MD of the TIR-graphene device at different gate voltages in the frequency domain. F, Reproduced with
permission.144 Copyright 2017, Wiley
TAO ET AL. 53

The tunable Brewster angle effect based on graphene has 7 | O UT L O O K

been demonstrated in different wavelength regions and
also used in different optical devices.149-151 Majérus et al
experimentally realized a Brewster angle shift in the
ultraviolet-visible to near-infrared range by covering
mono-, bi-, and trilayer graphene on the substrate, as
shown in Figure 15B.152 Chen et al showed an electrically
tunable Brewster device in THz for the first time, in
which the Brewster angle could be electrically tuned
from 65 to 72 (Figure 15C and D).150 The Brewster
device was operated as both an intensity and phase mod-
ulator. If the incident THz beam was fixed at 65 , the
device became an intensity modulator with a modulation
depth of 99.3% over the frequency range of 0.2 to 1.5
THz, as shown in Figure 15E. The graphene-based Brew-
ster device functioned as both a THz modulator and
ultrahigh-sensitivity gas sensor.153 The carrier density of
graphene is weakly modified by hydrogen gas. However,
this weak change is enlarged dramatically in the reflec-
tion phase spectrum when the light is incident at the
Brewster angle. A hydrogen gas sensor was developed
with aerial mass sensitivity of 1 fg mm−2 based on the
Brewster reflection.
By integrating 2D materials with various kinds of optical
structures, light-matter interaction in 2D materials can
be significantly improved and lead to high performance
of optoelectronic devices (Figure 16). Each type of optical
structure has advantages and disadvantages, which
necessitates that the structure to be coupled with 2D
materials should be chosen carefully depending on the
application requirements. Typically, metallic plasmonic
structures provide large local EM enhancement for boo-
sting the light-matter interaction in 2D materials. How-
ever, such architecture suffers from plasmonic losses
owing to energy dissipation. Moreover, the LSPR fre-
quency is fixed once the plasmonic structure is fabri-
cated, leading to a narrow band enhancement.
Waveguide-integrated structures with graphene are
favored for high-speed applications at telecommunication
wavelengths, but the on/off ratios are not sufficiently
high in photodetectors and modulators. Optical reso-
nance cavities can realize efficient light confinement with
high Q factors, but are not suitable for broadband appli-
cations. Integrating with optical reflection geometry, on

F I G U R E 1 5 A, Schematic of optical reflection on a substrate covered by a 2D material sheet. B, Brewster angle for a glass substrate,
and mono-, bi-, and trilayer graphene. Reproduced with permission.152 Copyright 2018, Institute of Physics. C, Graphene THz device based
on Brewster reflection. The conductivity of graphene is tuned by an Al2O3 dielectric gate with TiOx as the back electrode. D, Reflection
amplitude as a function of incident angle. The symbols represent experimental data. The solid curves are theoretical calculations. E,
Modulation depth in the frequency domain when the incident angle was 65 . C-E Reproduced from Reference 150 under the Creative
Commons License
54 TAO ET AL.

the other hand, can deliver an ultra-broadband response,
but with lower enhancement efficiency. In addition,
devices based on reflection geometry are usually of large
size, which hinders integrated chip applications.
Although there are still limitations for 2D material-based
micro/nano photonic devices, they have great potential
for many applications. For example, the response speed
of a waveguide-based graphene photodetector has been
demonstrated to be higher than 128 GHz, which is
beyond the bandwidth of 120 GHz of the best germanium
photodetectors integrated on silicon waveguide.154 In
addition to the optoelectronic devices discussed in the
main text such as photodetectors, modulators, LEDs and
molecular sensors, some novel optical memory/synaptic
devices based on 2D materials are attracting attentions
for artificial intelligence applications, whose perfor-
mances are expected to be further improved by micro/
nano photonic integration.155-157 Mennel et al demon-
strated a 2D semiconductor photodiode array that consti-
tutes an artificial neural network, which can be trained
to classify and encode images with a throughput of
20 million bins per second.157
In addition, 2D materials have intriguing physical
properties that are quite different from those of bulk mate-
rials, leading to both opportunities and challenges in
future studies on the optical-structure-integrated 2D mate-
rial devices. For instance, 2D materials are all-surface
materials, which necessitates careful interface engineering
while integrating 2D materials with optical structures to
enhance the coupling efficiency and to avoid unwanted
effects such as quenching of optical signals of 2D mate-
rials. The all-surface nature also makes the carrier concen-
trations in 2D materials highly tunable by electrostatic
gating. As a result, electrically tunable optical-structure-
integrated 2D material coupling devices can be achieved.
Wen et al demonstrated that electrostatic gating can
dynamically tune the plasmon-exciton coupling in a
hybrid structure of monolayer WS2 and gold nanorods.158
It is expected that more tunable devices based on hybrids
of 2D materials and optical structures can be realized in

F I G U R E 1 6 Scheme of enhancement strategies for light-matter interaction in 2D materials and related devices. Four common
enhancement strategies are introduced, including the plasmonic effect, waveguide, optical cavity, and reflection architecture. Some novel
optoelectronic devices are presented, such as photodetectors, electro-optic modulators, LEDs, and molecular sensors
TAO ET AL.
the future, which are promising for electrically driven inte-
gration applications. Another interesting topic is the inclu-
sion of interlayer excitons in 2D heterostructures. The
interlayer exciton energy is lower than the bandgaps of
individual 2D materials, and relies on the band alignment
at the heterostructure interface, which is electrostatically
tunable.159-162 Light harvesting and emission devices based
on interlayer excitons have attracted attention for infrared
applications. However, the interlayer transition rate in 2D
heterostructures is typically quite low because the transi-
tion is indirect both in real and reciprocal spaces. By cou-
pling the 2D heterostructures with various optical
structures, the light absorption/emission efficiency based
on interlayer transitions can be greatly improved, deliver-
ing high-performance infrared devices such as photodetec-
tors and LEDs. Some recently developed 2D optoelectronic
materials, such as Xenes and III-VI semiconductors (InSe,
GaSe, etc.), are also expected to be coupled with optical
architectures for device performance improvement.48,163
ACK NO WLE DGE MEN TS
Li Tao and Zefeng Chen contributed equally to this work.
The work is in part supported by Research Grants Coun-
cil of Hong Kong SAR, particularly, via Grant Nos.
AoE/P-02/12, 14204616, 14203018, N_CUHK438/18, and
CUHK Group Research Scheme, CUHK Impact Postdoc-
toral Fellowship, and ITS/390/18 by Innovation and
Technology Commission, Hong Kong SAR Government.
CONFLICT OF INTEREST
The authors declare no conflict of interest.
ORCID
Li Tao https://orcid.org/0000-0002-7757-1149
Jian-Bin Xu https://orcid.org/0000-0003-0509-9508
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AUTHOR BIOGRAPHIES
Li Tao is a postdoctoral fellow in the
Department of Electronic Engineer-
ing, The Chinese University of Hong
Kong (CUHK). He received his BS
and MS in Physics from Hunan Uni-
versity and National Center for
Nanoscience and Technology, CAS,
respectively, and PhD in Electronic Engineering from
CUHK. His research interests include CVD growth,
optoelectronic devices and light-matter interaction of
two-dimensional materials.
Zefeng Chen is currently postdoc-
toral research fellow at Department
of Electronic Engineering, The Chi-
nese University of Hong Kong. In
2017, Zefeng Chen graduated from
The Chinese University of Hong
Kong with a PhD in Electronic Engi-
neering. Before that, he received his BSc in physics
from HanShan Normal University in 2009, and master
degree in electronic Engineering from South China
Normal University in 2012. His research area is two-
dimensional materials with a particular focus on light
matter interaction applications.
Jian-Bin Xu received his BSc and
MSc from Nanjing University in 1983
and 1986, China, respectively, in
physics and information physics, and
doctorate degree in physics from The
University of Konstanz, Germany.
Afterwards, he joined the Depart-
ment of Electronic Engineering, The Chinese Univer-
sity of Hong Kong (CUHK). He has been a Professor
there since the mid of 2002. His research interests
include hybrid perovskites for optoelectronics, two-
60 TAO ET AL.

dimensional layered materials and devices, organic How to cite this article: Tao L, Chen Z, Li Z,
semiconductors, nanomaterials and nanoscopic char- Wang J, Xu X, Xu J-B. Enhancing light-matter
acterization, and high thermal conductive materials. interaction in 2D materials by optical micro/nano
He is a Fellow of IEEE and HKIE, and recipient of architectures for high-performance optoelectronic
Vice-Chancellor's Outstanding Fellow of devices. InfoMat. 2021;3:36–60. https://doi.org/10.
Engineering, CUHK. 1002/inf2.12148