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REVIEW ARTICLE | APRIL 19 2022
2D materials-enabled optical modulators: From visible to

terahertz spectral range
Xuetao Gan  ; Dirk Englund ; Dries Van Thourhout ; Jianlin Zhao
Appl. Phys. Rev. 9, 021302 (2022)

https://doi.org/10.1063/5.0078416
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2D materials-enabled optical modulators:

From visible to terahertz spectral range
Cite as: Appl. Phys. Rev. 9, 021302 (2022); doi: 10.1063/5.0078416
Submitted: 12 November 2021 . Accepted: 15 March 2022 .
Published Online: 19 April 2022
Xuetao Gan,1,a) Dirk Englund,2 Dries Van Thourhout,3,4 and Jianlin Zhao1
AFFILIATIONS
1
Key Laboratory of Light Field Manipulation and Information Acquisition, Ministry of Industry and Information Technology,
and Shaanxi Key Laboratory of Optical Information Technology, School of Physical Science and Technology, Northwestern
Polytechnical University, 710129 Xi’an, China
2
Research Laboratory of Electronics, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA
3
Photonics Research Group, INTEC, Ghent University-IMEC, Ghent B-9000, Belgium
4
Center for Nano-and Biophotonics (NB-Photonics), Ghent University, Ghent B-9000, Belgium
a)
Author to whom correspondence should be addressed: xuetaogan@nwpu.edu.cn
ABSTRACT
02 November 2023 14:02:46

Two-dimensional (2D) materials with layered structures have a variety of exceptional electronic and optical attributes for potentially
developing basic functions of light wave technology from light-emitting to -modulating and -sensing. Here, we present state-of-the-art 2D
materials-enabled optical intensity modulators according to their operation spectral ranges, which are mainly determined by the optical
bandgaps of the 2D materials. Leveraging rich electronic structures from different 2D materials and the governed unique light–matter inter-
actions, the working mechanisms and device architectures for the enabled modulators at specific wavelength ranges are discussed. For
instance, the tunable excitonic effect in monolayer transition metal dichalcogenides allows the modulation of visible light. Electro-absorptive
and electro-refractive graphene modulators could be operated in the telecom-band relying on their linear dispersion of the massless Dirac
fermions. The bendable electronic band edge of the narrow bandgap in few-layer black phosphorus promises the modulation of mid-infrared
light via the quantum-confined Franz–Keldysh or Burstein–Moss shift effect. Electrically and magnetically tunable optical conductivity in
graphene also supports the realizations of terahertz modulators. While these modulators were demonstrated as proof of concept devices, part
of them have great potential for future realistic applications, as discussed with their wavelength coverage, modulation depth, insertion loss,
dynamic response speed, etc. Specifically, benefiting from the well-developed technologies of photonic chips and optical fibers in telecom and
datacom, the 2D materials-based modulators integrated on these photonic structures are expected to find applications in fiber and chip opti-
cal communications. The free-space mid-infrared and terahertz modulators based on 2D materials can expect application in chemical bond
spectroscopy, free-space communications, and environment/health sensing.
C 2022 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://
V
creativecommons.org/licenses/by/4.0/). https://doi.org/10.1063/5.0078416
TABLE OF CONTENTS V. TERAHERTZ MODULATORS BASED

I. INTRODUCTION . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1 ON 2D MATERIALS . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19
II. EXCITONIC MODULATION OF VISIBLE LIGHT VI. SUMMARIES . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 22
IN THE TMDCS MONOLAYER . . . . . . . . . . . . . . . . . . . . 3
III. GRAPHENE OPTICAL MODULATORS
I. INTRODUCTION
OPERATING AT TELECOM-BAND. . . . . . . . . . . . . . . . 7
A. On-chip graphene electro-absorptive modulators . 7 Optical modulators play a crucial role in optical information
B. On-chip graphene electro-refractive modulators . . 11 processing systems, including optical communication, interconnect,
C. On-chip graphene thermal modulators . . . . . . . . . . 13 computing, and sensing, etc. In the operations, modulations of a light
D. Graphene-enabled fiber-based modulators . . . . . . . 15 beam could be realized by altering its amplitude, phase, or polarization
IV. MID-INFRARED OPTICAL MODULATORS BASED via the variations of absorption or refractive index of optical materials.
ON GRAPHENE AND BLACK PHOSPHORUS . . . . . . 16 According to the actuation methods, optical modulators are typically
Appl. Phys. Rev. 9, 021302 (2022); doi: 10.1063/5.0078416 9, 021302-1

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developed with the electro-optic, acoustic-optic, magneto-optic, thermo- compositions, or stacking behaviors of heterostructures.31–36 Relying on
optic, all-optical effects, and mechanical deformations. There are a these electrical and optical properties, it is possible to fabricate electro-
variety of commercial optical modulators manufactured with mature optic modulators in 2D materials operating over a broad spectral range
technologies, and the active media are normally chosen from semi- by employing the quantum confined Franz–Keldysh effect and Pauli-
conductors, ferroelectric oxides, ferromagnetic oxides, liquid crystals, blocked Burstein–Moss shift effect.37–39 The quantum confined carrier
etc. For example, lithium niobate-based modulators exploit its linear dynamics and small substance volume in 2D materials also promise
electro-optic effect to achieve low-power consumption and high-speed strong modifications of their optical responses under optical radiations
operation, which have been widely employed in high-speed optical com- by injecting high-density photon-generated carriers, enabling the all-
munications and microwave photonics.1,2 To be complementary with optical modulations.40–42 2D materials also harbor ferromagnetism
the on-chip optical interconnects, reliable optical modulators are inte- with high transition temperatures to support optical modulators with
grated onto silicon photonic chips using silicon’s strong thermo-optic the magneto-optic effect.43–45 Even for the insulating BN without ferro-
and plasma dispersion effects, which enable reconfigurable integrated magnetism or ferroelectricity, its polar crystal structure could be
photonic devices and single-chip microprocessor communicated directly exploited to excite the phonon polaritons for high efficient acoustic-
with light.3–5 optical modulation.46,47
Recently, two-dimensional (2D) materials with layered structures 2D materials also have other unique attributes to endow their
have emerged as an attractive active medium for constructing optoelec- benefits in applications of optical modulators. While there are only
tronic devices.6–14 It has been reported that versatile single-elementary mono- or few-atomic-layer thickness, light–matter interactions in 2D
and compound materials have layered stacking forms, which could be materials are extremely strong due to the reduced dielectric screening
exfoliated into a 2D material with a thickness of few-atom layer. and effective many-body interaction. For instance, graphene mono-
Therefore, plentiful electrical, optical, magnetic, and mechanical prop- layers absorb the single-passed light with an efficiency of 2.3% over a
erties could be acquired from 2D materials.15–21 These physical attrib- wavelength range from visible to mid-infrared.48,49 Molybdenum
utes provide possibilities to modulate optical signals via various disulfide (MoS2) monolayers could yield an absorption coefficient of
mechanisms with 2D materials. The family of 2D materials has a rich 10% around the excitonic resonances.50–52 The ultrathin flakes with
variety of electronic properties, including semi-metallic graphene, insu- reduced dielectric screening also allow easy tuning of their electrical
lating boron nitride (BN), semiconducting transition metal dichalcoge- and optical properties via electrostatic field, chemical doping, strain,
nides (TMDCs), and black phosphorus.22–26 Determined by this, the and pressure,53–59 which are difficult to realize in bulk materials. In
02 November 2023 14:02:46

optical responses of 2D materials could span a broad region of the elec- addition, 2D materials’ surfaces are naturally passivated without any
tromagnetic spectrum,15,27–30 ranging from microwave to ultraviolet dangling bonds.60–62 It is possible to construct vertical heterostructures
wavelengths, as schematically shown in Fig. 1. In addition, their optical using different 2D materials via the weak van der Waals force,
bandgaps could be engineered by controlling the layer numbers, alloy which thereby gets rid of issues of lattice mismatch and enables band
FIG. 1. 2D materials-enabled optical modu-

lators could operate in various spectral
ranges from visible to terahertz benefiting
from rich electronic structures in 2D materi-
als and the governed unique light–matter
interactions, which are actuated by electro-
optic, acoustic-optic, thermo-optic, all-optical,
and magnetic-optic effects.
Appl. Phys. Rev. 9, 021302 (2022); doi: 10.1063/5.0078416 9, 021302-2

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structure engineering.33,63 This also facilitates the integrations of 2D mainly exploited in optical telecom and datacom, the discussions of
materials with photonic elements or chips, ensuring that the integrated 2D materials-based modulators integrated on them will focus on the
optical modulators be applied in wide areas.64 possible applications in optical communications. For the 2D
In this Review, we present the state-of-the-art 2D materials-based materials-based modulators operated in the mid-infrared and tera-
optical modulators according to their operation spectral ranges, which hertz wavelength ranges, the 2D materials were normally integrated
are mainly determined by the optical bandgaps of the 2D materials. with plasmonic structures to enhance light–matter interactions and
For example, graphene’s zero-bandgap and linear dispersion endow the resulted modulators were operated in the free-space configuration
electro-optic modulations over a range from visible to terahertz band; for potential applications in chemical bond spectroscopy, free-space
electro-optic modulators of TMDCs or black phosphorus have opera- communications, environment/health sensing, etc. The corresponding
tion wavelength ranges from visible to mid-infrared due to their lim- performance merits evaluated on these modulators will mainly include
ited bandgaps. In addition, in those 2D materials, the main the wavelength coverage, modulation depth, insertion loss, dynamic
contributions of light–matter interactions arise from different physical response speed, etc.
mechanisms, including the strong many-body interactions, tunable
band structures of quasi-2D electron gas, etc. Wherein the working
II. EXCITONIC MODULATION OF VISIBLE LIGHT
principles of those 2D materials-based optical modulators will be illus-
IN THE TMDCS MONOLAYER
trated carefully, their modulations on optical intensity are considered
as the scope of this review. In addition, integrations of those modula- Group-VI TMDC monolayer, MX2 (M ¼ Mo, W; X ¼ S, Se, Te),
tors with various photonic structures are discussed as well, such as on- have received great research interest due to their strong photolumines-
chip waveguides, resonators, plasmonic nanoantenna, and optical cence (PL),31,65–67 current on–off ratios exceeding 108 in field-effect
fibers. The photonic structures could enhance light–matter interac- transistors,68 and efficient valley and spin control by optical helic-
tions in 2D materials significantly to get over the drawback caused by ity.69–72 In a TMDC monolayer, a single layer of transition metal
their intrinsically ultrathin material substance, which facilitates the atoms is sandwiched between two layers of chalcogen atoms in the tri-
high modulation performances. On the other hand, those well-studied gonal prismatic structure, as shown in Fig. 2(a). It has out-of-plane
photonic structures provide mature platforms for carrying out electro- mirror symmetry and broken in-plane inversion symmetry. Their
optic, thermo-optic, all-optical effects in 2D materials. Considering the bulk materials are commonly stacked by monolayers in the ABAB…
well-developed technologies of photonic chips and optical fibers are sequence, forming 2H polytype, which have inversion symmetry and
02 November 2023 14:02:46

FIG. 2. (a) Schematic of the trigonal pris-
matic structure of a monolayer TMDC. (b)
Illustration of a two-particle charge-neutral
exciton, two three-particle trions, and a
four-particle bi-exciton. (c) Simplified pic-
ture of the electronic bands near the K
and K 0 points of the Brillouin zone, which
are spin–split by the spin–orbit interac-
tions. (d) Absorption spectrum of mono-
layer MoS2 with two prominent resonance
peaks, known as the A and B excitons.
Reproduced with permission from Mak
et al., Nat. Mater. 12, 207 (2013).
Copyright 2013 Nature Publishing Group.
Appl. Phys. Rev. 9, 021302 (2022); doi: 10.1063/5.0078416 9, 021302-3

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indirect bandgap. In contrast to graphene, TMDC monolayers have another on-resonance channel for strongly enhanced light–matter inter-
direct bandgaps in the near-infrared and visible wavelength regions.9 action. By switching the oscillating strength between excitons and trions
Because of the reduced dielectric screening and relatively heavy in TMDC monolayers using electrical or chemical doping, the resonant
particle band masses associated with the Mo or W d-orbitals, charge optical responses could be modified readily.
carriers in TMDC monolayers have strong Coulomb interactions to As shown in Fig. 3(a), a back-gated field-effect transistor device
form tightly bound excitons, trions, and bi-excitons [Fig. 2(b)].51,73,74 could be constructed to apply a vertical electrostatic field across the
The binding energies of excitons are reported to vary from 0.5 to 1 eV, MoS2 monolayer. With different gate voltages (Vg), representative
which are nearly one order of magnitude larger than those found in absorption and PL spectra of the MoS2 monolayer were acquired, as
conventional quasi-2D systems.51,67 These many-body oscillators are shown in Figs. 3(b) and 3(c), respectively.51 Because of intrinsic doping
so robust that they could be clearly resolved at room temperature. by the substrate, the charge neutrality of the MoS2 monolayer was
Even with a relatively high carrier density, TMDC monolayers are still obtained around Vg ¼ –70 V. There are two absorption peaks with
strong many-body interacting systems. By injecting carriers into or values close to 8% around the photon energies of 1.9 and 2.05 eV,
dissipating carriers from the TMDC monolayers, it is easy to switch which are related to the two excitons determined by the spin-split
the many-body oscillators among these states. With that, desirable valence bands. As Vg increases to 80 V gradually, the high doping
modulation of excitonic optical responses in TMDC monolayers are density in the MoS2 monolayer would charge the excitons into trions,
expected, such as photoluminescence, absorption, and reflection. In which, therefore, reduces the two absorption peaks greatly to 4% and
addition, as shown in Fig. 2(c), the edge of the direct bandgap locates at 6%, respectively. On the other hand, the increased trion density results
the K (and K0 ) point of the Brillouin zone. The large spin-orbital inter- in the observable absorbance around the photon energy of 1.85 eV
action splits the highest valence bands at the K (and K0 ) point by (3%). Corresponding to the electrically controlled switching between
0.16 eV,69 which also lifts their spin degeneracy. The lack of inversion excitons and trions, the variations of PL emissions are displayed in
symmetry in TMDC monolayers results in couplings of valley and spin Fig. 3(c). Thanks to large binding energies of excitons and trions, these
degrees, which allows the optically controlled single valley and spin via electrically modified absorptions could be clearly distinguished even at
circularly polarized light.69,75–77 This attribute provides another degree room temperature. This facilitates realistic applications of exciton-
to modulate the optical signal using TMDC monolayers.78 based optoelectronic devices in TMDC monolayers. Of course, much
The robust exciton behaviors in TMDC monolayers enable its narrower linewidths of absorption and PL peaks could be obtained at
02 November 2023 14:02:46

strong interactions with the on-resonance optical radiations even at lower temperatures for understanding the many-body physics.
room temperature. The solid line in Fig. 2(d) displays the experimentally An exciton-based electro-optic modulator of the MoS2 mono-
measured optical absorption spectrum from an undoped MoS2 monolayer was proposed and fabricated by Fang et al.,80 which was com-
layer.51 Two pronounced absorption peaks are observed, corresponding bined with a plasmonic nanostructure, as shown in Fig. 4(a). Surface
to the excitonic transitions from the highest spin–split valence bands to plasmons of metallic nanostructures have extremely high density of
the lowest conduction bands, known as the A and B excitons. They are photon states in a nanoscale. The few atomic layers of the MoS2
modified significantly by the strongly bounded excitons. The absorbance monolayer allows its tightly spatial overlap with the surface plasmon
could be high as 10% even only with a monolayer material. In contrast after its integration with the metallic nanostructures. If the photon
to what expected in a 2D system without the excitonic effect, this mea- energies in the monolayer’s exciton and plasmon are coincident as
sured absorption should have a step-function-like spectrum originated well, the two quasiparticle would realize a strong coupling to form
from the energy-independent joint-density-of-states and transition exciton–plasmon polariton, which is also called “plexciton.”
matrix elements near parabolic band edges. By modifying the charge Considering the electrical tunability of MoS2 exciton, the state of plex-
doping level in the TMDC monolayer, the exciton could be charged by citon resonance could be employed as modulator.
binding an additional electron or hole to form a tightly bound trions,79 To make the device, a MoS2 monolayer was mechanically exfoli-
which decreases the density of excitons. The trion’s transition provides ated onto a silicon substrate covered with 300 nm thick silicon oxide
FIG. 3. (a) Schematic of gated monolayer MoS2 for tuning its absorbance and PL. (b) Variation of absorbance measured from gated monolayer MoS2 at different voltages. (c)
Electrically controlled oscillations between exciton and trion emissions. Reproduced with permission from Mak et al., Nat. Mater. 12, 207 (2013). Copyright 2013 Nature
Publishing Group.
Appl. Phys. Rev. 9, 021302 (2022); doi: 10.1063/5.0078416 9, 021302-4

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02 November 2023 14:02:46

FIG. 4. (a) Schematic of the electro-optic modulator based on the exciton-plasmon polaritons by modulating the exciton in monolayer MoS2 coupled with an Au nanodisk. (b)
Scattering spectra of Au nanodisk, MoS2–Au nanodisk, and absorption of the monolayer MoS2, indicating the formation of exciton–plasmon polariton. (c) Variations of the scat-
tering signals from the MoS2–Au nanodisk when different gating voltages were applied. (d) Time response of the MoS2–Au nanodisk electro-optic modulator. (e) Electrically
controlled display by modulating an array of MoS2–Au nanodisks. Reproduced with permission from Li et al., ACS Nano 11, 9720 (2017). Copyright 2017 American Chemical
Society.
(SiO2). A metal electrode was deposited on MoS2 to implement the exciton and plasmon. By electrically gating the MoS2 monolayer with
back-gate via the silicon substrate. A gold nanodisk with a radius of different voltages, the scattering spectra of the MoS2-nanodisk were
60 nm and a thickness of 30 nm was fabricated on top of the MoS2 modulated, as shown in Fig. 4(c). Increasing Vgs from 0 to 8 V, the dip
monolayer by electron beam lithography and metal deposition. The of the Fano-resonance line shape increases gradually. It could be
scattering spectrum of a bare gold nanodisk presents a Lorentzian- attributed to the suppression of exciton-enhanced absorption in the
type resonance peak around 650 nm, which is close to the exciton reso- MoS2 monolayer after the carrier doping. Around the wavelength of
nance of the MoS2 monolayer, as displayed in Fig. 4(b). The integration 685 nm, the scattering intensities reduce as the voltage increases since
of the MoS2 monolayer modifies the scattering spectrum of the gold the trion-related absorption becomes prominent with the charged exci-
nanodisk into an asymmetric Fano-type resonance with a dip at the ton. If negative voltages were applied (from 0 to 8 V), the scattering
exciton wavelength, indicating the coherent coupling between the dips of the Fano-resonance become much deeper as more trions are
Appl. Phys. Rev. 9, 021302 (2022); doi: 10.1063/5.0078416 9, 021302-5

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decharged into excitons. By comparing the scattering spectra obtained lens or gratings would become active optical devices. In 2018, Park
under Vg ¼ 0 and 8 V, the modulation depth of the varied scattering et al. and Imamoglu et al. separately reported that a MoSe2 monolayer
intensities around the resonance wavelength is 47.6%. The electro- has a high level of reflectance.82,83 With different substrates, the mono-
optic response time of the exciton-plasmon modulator was exploited layer mirror has a reflectivity up to 85% and 41%, respectively. From a
further by applying a series of squared electrical voltage pulses in milli- view of quantum electrodynamics, the MoSe2 monolayer provides an
seconds. The reflection signal around the exciton resonance was array of electrical dipoles. With an optical excitation, the dipoles are
switched successfully when the applied Vg varied between 0 and 8 V, driven to oscillate and re-radiate light at the same wavelength of the
showing a response time less than 200 ms, as shown in Fig. 4(d). The incident light. Both forward and backward radiations are obtained
slow modulation speed is limited by the long integration time of the with respect to the direction of the incident light. A perfect mirror
signal-processing camera. The ultimate response speed is actually would be realized when the forward radiations destructively interfere
determined by the RC constant of the parallel plate capacitor composed with the incident wave, resulting in zero transmission. The excellent
of the MoS2 monolayer and silicon back-gate (estimated as 50 ns). coherent properties of excitons in the MoSe2 monolayer provide the
Based on this gate-dependent exciton–plasmon coupling, a 2D display homogenous distributions of dipoles to ensure the completely destruc-
device could also be constructed by patterning an array of nanodisks tive interference between the incident wave and exciton re-radiation.84
on a chemical vapor deposition-grown MoS2 monolayer [Fig. 4(e)], as Electrical tuning of the exciton oscillator strength, therefore, promises
detailed in Ref. 80. a switchable mirror. As shown in Figs. 5(a) and 5(b), a MoSe2 mono-
According to the Lorentz oscillator model, optical responses of layer was encapsulated between two hexagonal BN layers and con-
TMDC monolayers on-resonance with exciton not only present tacted with an electrode.82 Combined with the highly doped silicon
strongly enhanced optical absorption but also have great dispersion of substrate, the MoSe2 layer functions as one planar electrode of the par-
the refractive index. It was reported that the refractive index of the allel plate capacitor, which has a 285 nm thick SiO2 dielectric layer.
MoS2 monolayer could be higher than 6.5 at the visible spectral With Vg applied to the silicon back gate, the carrier densities in MoSe2
range,52 leading to potential applications for making ultrathin and can be tuned readily. Figure 5(c) displays the reflection images under
ultracompact optical elements. For instance, Lu et al. reported the the on-resonance illumination with Vgs of –20 and 30 V, respectively.
world’s thinnest optical lens and high-efficiency gratings using mono- From the intrinsic MoSe2 layer (Vg ¼ –20 V), its reflection in contrast
and few-layer of MoS2.81 If the MoS2 layers were electrically gated, the to the substrate was observed substantially. It disappeared in an
02 November 2023 14:02:46
FIG. 5. (a) Schematic of a monolayer MoSe2 mirror, which could be electrically switched by the back gating. (b) Optical microscopic image of the electrically tuned mirror,
including a monolayer MoSe2 sandwiched by two BN layers and contacted with a Pt electrode. (c) Reflection images of the mirror device under 750 nm on-resonance laser illu-
mination with Vg of –20 and 30 V. (d) Reflection spectra of a monolayer MoSe2 mirror at different Vg values. Reproduced with permission from Scuri et al., Phys. Rev. Lett.
120, 37402 (2018). Copyright 2018 American Physical Society.
Appl. Phys. Rev. 9, 021302 (2022); doi: 10.1063/5.0078416 9, 021302-6

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n-doped MoSe2 layer (Vg ¼ 30 V). From the gate-voltage dependent improved further, such as integrating with nanophotonic structures to
reflection spectra shown in Fig. 5(d), one can find at Vg ¼ 30 V that enhance the light-TMDCs interactions.
there is a trion-related reflection peak due to the charging of excitons.
III. GRAPHENE OPTICAL MODULATORS OPERATING
The reflection spectrum becomes flat around the wavelengths of the
AT TELECOM-BAND
exciton. Here, the reflection peaks around the exciton have asymmet-
ric Fano-type lineshapes originating from the interference of separated With the rapid development of optical communications and data
reflections from the MoSe2 monolayer and back silicon substrate. In communications, high-performance optical modulators operating in
the work reported by Imamoglu et al., the driven voltages for realizing telecom-band encounter a variety of challenges in power consump-
the maximum variation of the reflection intensity are much smaller tion, optical bandwidth, dynamic response, modulation depth, etc.
benefiting from the thin dielectric film of the 33 nm thick BN layer. Strong light–matter interactions, unique electrical properties, and the
The modulation depth of the reflection intensity was estimated around ease-of-integration in 2D materials have the potential to solve these
80% on the exciton resonance with an actuated voltage of 2 V.83 problems. Because electronic bandgaps of TMDCs mismatch with the
Though the dynamic responses of the demonstrated MoSe2 modula- photon energy of the telecom-band light wave, graphene is considered
tors were not demonstrated, a subnanosecond timescale is expected by to be a suitable material for modulations in the telecom-band relying
engineering the device with a small capacitance as well as the intrinsic on its broadband optical responses from ultraviolet to terahertz band.
low resistance Ohmic contacts of the MoSe2 monolayer.85 In addition, compared with TMDCs, graphene’s wafer-scale synthesis
These strong exciton-photon interactions in the TMDC mono- and transfer with high qualities are well developed, which paves the
layers have great potential to improve modulators with high-efficiency. way for real applications of graphene modulators. In this section, we
Furthermore, the light-matter coupling in the TMDC monolayers could mainly discuss the promise of graphene modulators for telecommuni-
be enhanced further by integrating them with photonic structures to cations. Since the telecommunication systems are mainly built on the
employ resonance and waveguiding modes, including photonic crystal optical fibers and photonic integrated chips, the reported graphene
cavities, waveguides, and microrings,86–89 which are attractive for chip- modulators in the telecom-band were mainly carried out with chip-
integrated optical modulators. In addition, since the lifetimes of excitons integration or fiber-integration. These integrations could also enhance
are in the scale of picoseconds, it is possible to carry out ultrafast opera- the light–graphene interactions with optical waveguides or resonators
tions in the exciton-based modulator. Note that exciton’s quasiparticle to facilitate the improvement of modulation performances. In Secs. III
properties with weak dielectric screening make it only respond to light and IV, graphene-based mid-infrared and terahertz modulators will be
02 November 2023 14:02:46

waves in a narrowband range, which makes it negative to perform as a involved, which were implemented in the free-space configuration by
broadband optical modulator. On the other hand, TMDC monolayers integrating graphene with plasmonic structures or patterning gra-
have large optical bandgaps. This limits the spectral range of TMDC phene with a plasmonic resonance response to enhance light–gra-
modulators to visible and near-infrared spectral range. For instance, as phene interactions. While visible free-space graphene modulators were
one of the monolayer TMDCs with the smallest bandgap, the MoTe2 also reported,94 there are unfortunately some disadvantages of requir-
monolayer has a bandgap still larger than 1.1 eV.67 While thicker MoTe2 ing high operation voltages for tuning the Fermi level and large inser-
has smaller bandgap around 1 eV,90 it loses the behavior of tightly bound tion loss. They will not be discussed here.
exciton, which would degrade its optical response significantly. As an
alternative routing, doping TMDC monolayers at wavelengths far from A. On-chip graphene electro-absorptive modulators
its exciton resonance could also be employed to carry out a modulator In the visible to mid-infrared range, graphene’s optical absor-
based on the electro-refractive response. While the modulation depths of bance is primarily attributable to interband transition, which is a con-
this off resonance modulator were not expected to be as high as those stant value determined by the fine-structure constant in pristine
governed by the exciton-modulated one, it could perform with negligible graphene.49 However, if a vertical electrostatic field is applied over gra-
insertion loss and broad bandwidth.91,92 phene, the increased carrier density would shift the Fermi level (EF)
Optical modulators in the visible spectral range are essential for and induce Pauli blocking of the optical transition,53,95 as schemati-
the applications of virtual-reality displays, visible light communication, cally shown in Fig. 6(a). For the telecom-band light wave with photon
and optogenetics, etc. The state-of-the-art visible modulators were energy around hv0 ¼ 0.8 eV, EF tuning larger than 0.4 eV would con-
normally realized by the technologies of the liquid crystal or micro- tribute to the reduced absorption, giving rise to an electro-absorptive
electromechanical system, which have the disadvantages of slow modulator.
operation speed, large operation voltages, and complex and bulky sys- With this principle of operation, Liu et al. transferred a graphene
tems.93 Though the reported modulators based on TMDC monolayers layer onto a silicon waveguide to fabricate the first graphene-based
are still in the state of proof of principle, they have the potential to modulator.39 Since the graphene layer is single atomic thin, it cannot
solve some of the problems. For example, by mechanically stacking couple with the surface illumination effectively. Its integration with an
TMDC monolayers with BN and graphene via their van der Waals optical waveguide extends the light-graphene coupling length, result-
forces, the modulators of TMDC monolayers could be constructed ing in reliably increased optical attenuation from 0.1 to about
with a thickness of few-atomic layers, which promise the device with 10 dB.96,97 By electrically suppressing graphene’s absorption, a modu-
high compactness and integration level. As discussed above, because lator with a high extinction ratio could be realized. As schematically
the operations of the TMDCs-based modulators are governed by the shown in Fig. 6(b), to electrically gate the graphene layer, an electrical
electrical actuations of the parallel capacitors, the dynamic response capacitor was built with the graphene layer and the silicon waveguide
speed could approach GHz. Note that to guarantee the future realistic as two plate electrodes. Figure 6(c) displays the scanning electron
applications of these modulators, their modulation depth should be microscopic (SEM) image of the fabricated device. Graphene
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FIG. 6. Broadband graphene electro-absorptive modulators integrated on silicon waveguides. (a) Band structures of graphene at different doping levels, where graphene
becomes transparent when the interband transition is Pauli blocked, as shown in the left and right images. (b) Schematic representation of a waveguide-graphene modulator,
where the graphene and silicon waveguides are separated by a thin alumina layer to form a parallel capacitor. (c) SEM image of a fabricated device. (d) Static electro-optic
response of the device shown in (c) at different drive voltages. (e) Transmission spectra of the device shown in (c) at different drive voltages. (f) Squared photon energy vs crit-
ical drive voltage for maximum transmission change rate extracted from (e). (g) Optical microscopic images of several graphene electro-absorptive modulators integrated on a
CMOS silicon photonic chip. (h) Optical eye diagrams measured at 1560 nm for one of the devices shown in (g) at 6, 8, and 10 Gb/s modulation speeds. (b)–(f) Reproduced
with permission from Liu et al., Nature 474, 64 (2011). Copyright 2011 Nature Publishing Group. (g)–(h) Reproduced with permission from Hu et al., Laser Photonics Rev. 10,
307 (2016). Copyright 2016 Wiley-VCH Verlag GmbH & Co. KGaA.
transferred onto the silicon waveguide was selectively etched to cover optical absorption of graphene, giving rise to waveguide’s high trans-
the waveguide. A 7-nm-thick alumina was inserted into them to work missions. At Vg ¼ 4 V, the modulation depth of the device is high
as the dielectric spacer. The silicon waveguide was electrically con- as 0.1 dB/lm. The asymmetric voltage-dependent transmissions result
nected by a 50-nm-thick silicon layer. The modulation performance from natural doping of the graphene by the substrate. Also, ideally,
was implemented by measuring the waveguide transmission of light at there should be a sharp transmission variation at EF ¼ hv0 =2.
1530 nm by applying different Vgs, as shown in Fig. 6(d). At low However, due to the defect and phonon perturbations in graphene, the
applied voltages (–1 V < Vg < 3.8 V), graphene’s Fermi level is close transition process of on and off state are gradual.
to the Dirac point. Its strong light absorption induces a quite low Since graphene has a linear dispersion electronic structure
transmission of the hybrid graphene-waveguide. For high drive vol- around the Dirac point, this electro-absorptive modulator could be
tages, the Fermi level was tuned to a level of hv0 =2 lower (higher) than realized over a broad spectral range. Because graphene’s Pauli-
the Dirac point, Pauli blocking of the interband transition forbids the blocking of optical transition depends on the relative values between
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the Fermi level and photon energies, the voltage thresholds for modu- materials considering their atomic layer thickness. Its planar structure
lating light waves at different wavelengths are varied. Figure 6(e) dis- is compatible with the integration of 2D materials without quality deg-
plays the electrically modulated transmission over a wavelength range radation, as well as the construction of electrical devices. Strongly
from 1350 to 1600 nm. The dashed line shows the trace for maximum enhanced absorption, Raman, PL, and nonlinear processes of 2D
transmission change rate with a quadratic function between the pho- materials have been realized with PC cavities.86,87,105–107
ton energies and drive voltage. It is governed by the relation between Gan et al. reported the monolayer graphene renders the reflection
Fermi level and drive voltage, as the extracted data shown in Fig. 6(f). of a PC cavity to be nearly opacity, about 20 dB attenuation,105 which
Relying on graphene’s high carrier mobility and large saturation indicates the implementation of optical modulators with high modula-
velocity, this graphene-waveguide modulator is expected to have high- tion depth by suppressing graphene’s absorption electrically. As shown
speed operation. Its dynamic response was estimated by applying a in Fig. 7(a), by integrating a silicon PC cavity with a graphene field
radio frequency electrical signal added on a static voltage. A fast-speed effect transistor, a high-contrast electro-absorptive modulator was pro-
photodetector was employed to monitor the waveguide output. The posed.108 To effectively tune graphene’s Fermi level, an electrolyte
3 dB bandwidth of the devices at different drive voltages were esti- layer was employed as the top gate. By forming two interface capaci-
mated. The highest modulation speed was about 1.2 GHz with a high tors, over the graphene layer, an extremely strong vertical electric field
drive voltage due to the large detectable extinction ratio.39 This limited is constructed, which could trap high carrier density. In the fabricated
bandwidth is not caused by the carrier transit time in graphene, but by device, a PC cavity with a slotted defect was exploited, providing more
the parasitic response of the device, which has a footprint of 25 lm2.98 optical field to couple with the coated graphene layer. Drain and
Similar graphene-waveguide capacitor geometry was employed by source electrodes were deposited on the graphene layer, and the gate
Thourhout et al. to fabricate a broadband and athermal modulator electrode was about 15 lm away from them, as shown in the optical
operating at a speed of 10 GHz,99 as shown in Figs. 6(g)–6(h). microscopic image displayed in Fig. 7(b). An electrolyte layer (PEO
Recently, several graphene-waveguide modulators were fabricated on plus LiClO4) was spin-coated on the entire wafer. After the whole fab-
a compact chip using the CMOS processing line. Wide open eye dia- rication, the Q factors of the three resonant modes of the PC cavity
grams with the dynamic modulation depth of 2.5 dB and low jitter decrease from (860, 2350, 3420) to (335, 610, 41,0) respectively, due to
were obtained at 6 and up to 10 Gb/s at the working wavelength of graphene’s absorption,108 which also reduced modes’ reflection inten-
1560 nm. This result constructively proved the possibility of graphene sities. By applying varied Vgs, the graphene-PC cavity’s reflection spec-
modulators for signal processing. The reduction of the dimension of tra were acquired, as shown in Fig. 7(c). From 0 to –7 V, graphene’s
02 November 2023 14:02:46

the graphene capacitor is required to improve the operation speed. Fermi level was tuned gradually to 0.8 eV, which is close to the photon
However, the modulation efficiency of the graphene-waveguide will be energies of the resonant modes around 1550 nm. The three resonant
sacrificed as the result of the shortened light-graphene coupling length. peaks of the cavity reflection spectrum become strong and separate
In regard to this trade-off, Liu et al. proposed a double-layer graphene from each other due to the increased Q factors, which are enabled by
optical modulator by integrating the silicon waveguide with a capacitor the Pauli-blocked optical absorption in graphene. The voltage-
consisting of two graphene layers, as schematically shown in Fig. 6(g). dependent red- and blue-shifted resonant wavelengths were observed
The waveguide’s evanescent field couples with two graphene layers, as well due to the variation of graphene’s refractive index. Note, while
which would improve the transmission attenuation over the same the Fermi level is much higher than 0.4 eV (half photon energy of the
device length. Indeed, a modulation depth of 0.16 dB/lm was obtained incident light), the intensities and Q factors of the resonant peaks can-
at a moderate drive voltage of 5 V.100 Another benefits of the dual- not completely recover to values of the original cavity. This might be
graphene structure is the simplified process of electrical contact with attributed to the presence of residual absorption caused by intraband
the absence of selective ion implantation on silicon. With the optimi- transition and defects in graphene. By changing Vg reversely, the
zation of this structure, the low graphene contact resistance and small strong resonant peaks lower and merge together, illustrating the elec-
capacitor dimension allow the high-speed modulation. A device with a trically controlled modulations. With the voltage changed from 0 to
bandwidth of 35 GHz was reported by the same group.101 6 V, similar variations of the resonant peaks were obtained as those
As discussed above, optical waveguides enhance graphene’s opti- with negative drive voltages. By comparing the reflection intensities at
cal absorption via its extended length, which unfortunately hinders the the resonant wavelength at different Vgs, a modulation depth of 10 dB
fabrication of high-speed modulators due to the large footprint. An was achieved, which satisfies the requirement of signal processing.
alternative photonic structure to enhance light-graphene coupling is Because of the small capacitance of such a graphene-PC cavity, low
optical cavities. Different from waveguides, optical cavities recirculate power consumption was also anticipated. For the current device, the
light wave in a confined mode for an extended time, which, therefore, switching energy is about 340 fJ from a calculation of the capacitive
maintains strong light–graphene interactions in a compact structure. charging energy. Also, the moderately broad linewidth of the resonant
Photonic crystal (PC) cavity is one of the optical resonators with the peak could promise better temperature tolerance than those devices
highest Q=Vmode . Here, Q and Vmode are the quality factor and mode with high Q resonators.
volume of the resonant modes in the PC cavity. The strength of the The response speed of electrolyte-gated modulator is restricted
optical fields in the resonant mode is proportional to the factor of by the low mobility of ions in the electrolyte. Gao et al. couples a PC
Q=Vmode . The PC cavity could provide high density of the electrical cavity with a dual-graphene capacitor to improve the operation
field to enhance light–matter interactions for the low-threshold micro- speed,109 as schematically shown in Fig. 7(d). A PC cavity was pre-
laser, bright single-photon source, and ultrasensitive microsen- cisely placed on the BN-graphene-BN-graphene-BN heterostructure
sor.102–104 The PC cavity fabricated in a subwavelength thick slab (graphene capacitor) to realize the coupling between cavity modes and
could provide a remarkable evanescent field to couple with 2D the graphene–capacitor. Figure 7(e) displays the static electrical tuning
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FIG. 7. High-contrast graphene electro-absorptive modulator integrated on a PC cavity. (a) Schematic illustration of an electrolyte gated graphene modulator integrated on a sil-
icon PC cavity. (b) Optical microscopic image of the graphene-PC cavity modulator. (c) Reflection spectra of the PC cavity modulated by the top graphene layer at different Vg
values, showing variations of the peak intensity and linewidth. (d) Schematic illustration of a modulator with a dual-graphene capacitor coupled with a PC cavity. (e) Static mea-
surement of the reflection spectra from the device in (d) at different Vg values. (f) Dynamic responses of the electrical modulation from the device in (d). (a)–(c) Reproduced
with permission from Gan et al., Nano Lett. 13, 691 (2013). Copyright 2013 American Chemical Society. (d)–(f) Reproduced with permission from Gao et al., Nano Lett. 15,
2001 (2015). Copyright 2015 American Chemical Society.
result. By applying voltages on the graphene–capacitor, the resonant an area of 100 lm2 and a capacitance of 320 fF. The switching energy
peaks of the PC cavity were modulated successfully with clear varia- is approximately 1 pJ/bit. For the PC cavity, the overlap between the
tions of intensity and linewidth. To evaluate the dynamic response, a resonant mode and the graphene capacitor could be smaller than
radio frequency network analyzer was used to apply a high-speed elec- 0.5 l2 . It is possible to reduce the dual-graphene capacitor to a size
trical signal on the device. The intensity modulation of a resonant matching with the cavity area to lower the capacitance by approxi-
peak was monitored, presenting 3 dB attenuation at the frequency mately 200 times. This optimization could decrease the switching
of 1.2 GHz [Fig. 7(f)]. The cutoff frequency is limited by the RC time energy to 5 fJ/bit and increase the 3 dB cutoff frequency to 70 GHz.
constant of the dual-layer graphene capacitor, as deduced by the Another widely employed on-chip optical resonator is a micror-
impedance measurement of the device. The graphene capacitor has ing, which has advantages in ease of design, compact footprint, and
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large fabrication tolerance. For real optoelectronic chips, microrings 40 V would give rise to a depth of 15 dB. The requirement of high Vg
coupled with a channel waveguide have functioned as filters, modula- originated from the thick dielectric layer between the two graphene
tors, and isolators. Graphene modulators constructed on microrings layers, which actually generates a small capacitance for supporting a
have more potentials for real device applications. A number of high-speed operation. The 3 dB bandwidth of the dynamic response
microring-based graphene modulators have been reported with capac- was evaluated as 30 GHz [Fig. 8(e)], which also promises a clear eye
itor structures consisting of dual-graphene layers or hybrid graphene– diagram in the real data stream testing (the inset). The power con-
silicon.110–112 There are resonant dips in the transmission of the sumption for per bit is estimated as 800 fJ, which is less than those
waveguide side-coupled with the microring, whose extinction ratio is reported in silicon-based modulators. Those pretty figure of merits
determined by the relative rates of the microring’s mode loss and make this modulator configuration has great potentials for future on-
waveguide-coupling loss. Ideally, the extinction ratio could be 100% chip signal processing.
with the critical coupling condition when the microring’s mode loss
equals to the waveguide-coupling loss. If a graphene layer is covered B. On-chip graphene electro-refractive modulators
on the microring, its absorption will induce more microring’s mode As discussed above, graphene electro-absorptive modulators
loss, breaking the critical coupling condition. Hence, the integrated were realized via the suppressions of graphene’s absorption due to the
graphene not only reduces the Q factors but also decreases the extinc- Pauli blocking. According to the Kramers–Kronig relation, the abrupt
tion ratios of the resonant dips. Under this condition, the intensity of variation of optical absorption is accompanied by a large change in the
waveguide-transmission at the resonant dip increases. By electrically refractive index. Hence, a graphene-based electro-refractive modulator
gating graphene to suppress the absorption, the critical coupling con- is also expected by electrically tuning its carrier density for a moder-
dition is recovered and the transmission intensity lowers, as schemati- ately large variation of its refractive index. Actually, in Refs. 108 and
cally shown in Fig. 8(a). Phare et al. fabricated a dual-graphene 110, while the authors focused on amplitude modulations caused by
capacitor on a silicon nitride microring [Figs. 8(b) and 8(c)]. Because the absorption-suppression, graphene’s refractive index was tuned suc-
of graphene’s absorption, the resonant dip has a low Q factor (800) cessfully, which had also induced considerable effects. For instance, as
and small extinction ratio (8 dB) at Vg ¼ 0 V. By gradually increas- shown in Figs. 7(c) and 8(d), when a resonant mode of a microcavity
ing Vg, the resonant dip red-shifts first and then blue-shifts with the couples with an electrically actuated graphene capacitor, the resonant
continuously narrowed linewidths. The resonant dips shown in Fig. wavelength red-shifts first and then blue-shifts as graphene’s Fermi
02 November 2023 14:02:46

8(d) indicate a modulation with a high depth could be obtained for a level is tuned away from the Dirac point gradually. According to the
narrowband incident light considering the combined effects of wave- perturbation theory of electromagnetic wave, the shifts of cavity’s reso-
length shift and critical coupling. A voltage variation from 30 to nant wavelength are attributed to the variation of graphene’s refractive
FIG. 8. Ultrafast graphene modulator integrated on a microring. (a) Schematic illustration of the graphene-modulated transmission from a microring side-coupled with a bus-
waveguide, which is determined by the critical coupling related to graphene’s absorption. ER: extinction ratio. (b) Optical microscopic image of the microring based graphene
modulator. (c) SEM image of the device with the dual graphene layers covering over the microring. (d) Transmission spectra of the microring side-coupled with the bus wave-
guide at different Vg values, indicating large modulation depth. (e) Dynamic response of the modulator with a 3 dB bandwidth of 30 GHz. Inset shows the open 22 Gbps 271
pseudo-random binary sequence non-return-to-zero eye diagram. Reproduced with permission from Phare et al., Nat. Photonics 9, 511 (2015). Copyright 2015 Nature
Publishing Group.
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index.108 For the result presented in Ref. 108, a resonant wavelength doping of graphene, its complex conductivity controlled by EF could
blue-shifted by 1.5 nm was obtained when the graphene field effect be estimated by a simple theoretical model based on both inter- and
transistor was gated with a voltage of –7 V. Considering that the reso- intraband transitions,113
nant peak has a linewidth of 1.8 nm, this electrically actuated wave-
length shift already enabled an electro-refractive modulator. rg ¼ r0 Hðhx 2EF Þ þ ir0 ½ð4EF Þ=ðphxÞ
For the semimetal graphene, its complex refractive index (ng) is
governed by its complex optical sheet conductivity (rg) in the form of 1=plnjð2EF þ hxÞ=ð2EF hxÞj (2)
sffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
irg with r0 ¼ e2 =ð4Þh. This model neglects finite temperature and finite
ng ¼ 1 þ ; (1) dephasing rates. In Ref. 108, doping-dependent complex conductivity
xdg e0
of graphene for the wavelength around 1550 nm was extracted by
where x is the operating wavelength, dg ¼ 0.34 nm is the thickness of referring to the Q factors and resonant wavelengths of the graphene-
graphene, and e0 is the permittivity of free space. With an electrostatic modulated resonant mode, as shown in Fig. 9(a). Equation (2) was
02 November 2023 14:02:46
FIG. 9. Graphene electro-refractive modulators integrated on waveguides. (a) Complex conductivity of graphene for the wavelength around 1550 nm at different doping lev-
els.108 (b) Device structure of a graphene-integrated MZI for experimental verification of electro-refractive phase modulation in graphene. (c) Transmission spectra of the device
in (b) at different drive voltage, showing the repeatability and spectrum shift. (d) Wavelength shift and the extracted refractive index variations from the device in (b) applied
with varied voltages. (e) Optical microscopic image of a MZI modulator with graphene-silicon hybrid capacitors on both arms. (f) Transmissions of a 1550 nm laser at the bar
port as functions of the shorter arm voltages when the longer arm voltage is fixed at different values. (g) Dynamic characterization of the MZI modulator in (e) showing 5 GHz
bandwidth at 3 dB and an open eye diagram at 10 Gb/s. (a) Reproduced with permission from Gan et al., Nano Lett. 13, 691 (2013). Copyright 2013 American Chemical
Society. (b)–(d) Reproduced with permission from Mohsin et al., Sci. Rep. 5, 10967 (2015); licensed under a Creative Commons Attribution (CC BY) license. (e)–(g)
Reproduced with permission from Sorianello et al., Nat. Photonics 12, 40 (2018). Copyright 2018 Nature Publishing Group.
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employed to predict these results with good agreement. When EF over the two graphene capacitors. By fixing the voltage applied on the
increases to values larger than 0.4 eV (half photon energy of the inci- longer arm, the device transmission was plotted as a function of the
dent light), the real part of the complex conductivity (Rerg) voltages applied on the shorter arm. For the minimum transmission
approaches to zero gradually, giving rise to the neglectable optical points, the phase difference between the two arms approaches p. For
absorption. The imagery part of the complex conductivity (Imrg), cor- instance, by applying 4.1 V to the shorter arm and 7.25 V to the longer
responding to the real part of the refractive index, presents an inflec- one, the phase difference between the two arms approaches p. The
tion point with EF close to 0.4 eV and has a larger dispersion for the modulation depth is maximized in this case, which is larger than
even higher doping level. This is very promising to implement a 35 dB. This Vp ¼ 7:25 V on the 400 lm long graphene capacitor cor-
graphene-based electro-refractive modulator with EF tuned larger than responds to Vp L ¼ 0:28 V cm, which is a fivefold improvement com-
0.4 eV. The intrinsic absorption in graphene is forbidden effectively to pared with state-of-the-art p-n junction-based silicon MZI
guarantee the low insertion loss, and the refractive index changes modulators. The dynamic response of this electro-optic modulator
greatly for the considerable phase shift. For example, calculated from was characterized using an electrical vector network analyzer. The S21
Eqs. (1) and (2), a variation of refractive index larger than 5 is possible parameter of the network analyzer presented a 3 dB roll-off frequency
if the EF is tuned from 0.4 to 1 eV.114,115 to 5 GHz. As discussed by the authors, the bandwidth was mainly lim-
The graphene electro-refractive modulator was verified specially ited by the RC time constant originating from the silicon-graphene
by integrating an electrically gated graphene layer on a silicon wave- capacitor and series resistances. For the real data stream processing, a
guide based Mach–Zehnder interferometer (MZI).116 Since the varia- non-return-to-zero eye diagram was implemented, as shown in Fig.
tion of graphene’s refractive index only results in a phase shift of the 9(g), which presented an open eye diagram at 10 Gb s1 with a 4 dB
hybrid graphene-waveguide, the MZI would convert the phase change modulation depth and a 6 dB signal-to-noise ratio. Calculated from
into an amplitude modulation. The device structure is schematically the energy consumption of the charging and decharging capacitor, a
shown in Fig. 9(b). On one of the MZI arms, a capacitor formed by value of 1 pJ per bit was obtained. While the reported device has disad-
dual-graphene layers was built. Due to the strong optical absorption in vantages in operation speed and energy consumption compared to the
graphene, the hybrid graphene-waveguide has a large attenuation of pure silicon modulators118 or III–V on silicon modulators,119 graphe-
the transmission.86 To maintain the extinction ratio of the MZI, the ne’s decent electrical and optical properties endow great potentials to
other arm of the MZI was covered by a graphene layer as well. Figure improve the performances of the proposed electro-refractive modula-
9(c) displays the monitored transmission spectra when the dual- tors. For instance, with a better graphene-preparing technique to
02 November 2023 14:02:46

graphene capacitor was biased at 40 and 40 V. A clear shift of the improve the material quality and the metal contact, the series resis-
minimum transmission was observed at the two voltages. The inset tance from the graphene channel could be reduced by more than one
indicates the repeatability of the electro-optic modulating effect. When order of magnitude. Furthermore, the two electrodes of the graphene-
the voltage between the two graphene layers was applied between 40 silicon capacitor could be designed in a traveling wave form to
and 40 V, the whole interference spectrum was shifted by 0.14 nm, cor- decrease the parasitic capacitance. The RF bandwidth could be greatly
responding to an effective refractive index change of 1.6 10–4, as dis- improved to a value around 50 GHz.110 By replacing the graphene-
played in Fig. 9(d). Graphene’s intrinsic absorption over the two arms silicon capacitor with a graphene-graphene capacitor over the silicon
was suppressed as well by the large electrical gating. Unfortunately, the waveguide, the modulation efficiency could be doubled with the halved
employed structure had a thick spacer layer (90 nm) between the gra- energy consumption.
phene capacitor and the silicon waveguide. The modifications of gra-
phene’s refractive index generate very weak effect over the effective C. On-chip graphene thermal modulators
refractive index of the hybrid graphene-silicon waveguide, which In silicon photonics, high-speed (>GHz) modulators fabricated
makes the device operation to require a high drive voltage. Also, since in silicon or III–V compound materials have very complicated and
the graphene layer covered over another arm was not electrically gated, high-cost fabrication processes.118,119 Contrastively, chip-integrated
its intrinsic attenuation causes a large insertion loss of the device. thermal modulators have virtues of ease-of-fabrication, high-
Sorianello et al. proposed a graphene electro-refractive modulator efficiency, and broad optical bandwidth. Unfortunately, to heat the
integrated on a silicon chip, showing figure of merits satisfying the photonic structures for realizing refractive index variation, metal elec-
requirement of real data processing.117 As shown in Fig. 9(e), an MZI trodes are required to align across the photonic structures. To avoid
fabricated on a standard silicon photonic platform was integrated by optical absorption by the metal heater, a thick silicon oxide layer (nor-
an individual graphene capacitor on each arm. Here, two graphene mally larger than 1.5 lm) would be deposited. However, such a thick
capacitors were constructed by the doped silicon waveguide and the upper-cladding layer will introduce low response speed and low heat-
top graphene layer, which were separated by a 10 nm thick silicon ing efficiency due to its poor heat conductivity. In addition, the tem-
oxide. This thin dielectric layer reduces the electrical voltage required perature in the metal heater is much higher than that in the photonic
to dope the graphene effectively. On the two arms, the graphene structures. Consequently, the temperature dynamics of the photonic
capacitors were designed with different lengths to facilitate the electri- structure is limited. While careful photonic designs to shrink the foot-
cal tuning of their phase differences. To operate the device, both gra- print or suspend the device could improve the efficiency and response
phene capacitors were applied with static voltages close to 5 V to speed to some extent, they inevitably introduce complex fabrication
eliminate graphene’s absorption. This could guarantee the low inser- and operation.
tion loss of the whole device. Figure 9(f) shows static measurements of Graphene has been well recognized as a conductive layer with
the electro-refractive modulator. With an input of 1550 nm laser, the high transparency. Its long-wavelength phonon transportation prom-
bar port of the MZI was monitored with the varied gating voltages ises the high intrinsic thermal conductivity at room temperature,
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which has been employed as spreaders in electronic and photonic large device footprint, which also gives rise to a long response time of
devices.120 With the combination of these attributes, it is possible to about 20 ls [right column of Fig. 10(a)].
directly contact a graphene heater onto a photonic structure without the To improve the modulation efficiency and speed significantly,
spacing layer by considering its moderate transparency. Compared with one of the possible routes is shrinking the device size. For example, Xu
traditional thermal modulators with thick oxide layers, heat generated et al. employed a PC nanobeam cavity to couple with a graphene
on the graphene layer could transfer to the photonic structure with fast heater [Fig. 10(b)].124 With the confinement of the total internal reflec-
speed and high efficiency. The fabrication of a graphene heater on the tion of the silicon strip with the high refractive index and photonic
photonic structure is feasible considering its semimetal property and bandgap of periodic air-holes, the nanobeam cavity has ultrasmall
mature growth and transfer techniques. Its ultrahigh thermal conductiv- mode distribution (in a wavelength scale). It is possible to shape the
ity facilitates fast transfer of thermal energy to the photonic structure, graphene heater with a width in the scale of wavelength, promising the
which also works as a fast thermal dissipation channel. Several effective interaction with the heat field and optical field. As shown in
graphene-based silicon modulators have been reported with response the middle column of Fig. 10(b), a tuning efficiency of the resonant
times smaller than 1 ls.121,122 Heated by the top graphene heater, pho- peak exceeding 1.5 nm/mW was realized. It could be considered as the
tonic structures have phase shifts due to the variation of refractive index. record high value in graphene-assisted thermal-optic modulators.
To convert it into intensity modulation, MZIs or resonators are essen- Also, the ultracompact structure of nanobeam-graphene allows the
tial, as shown in Fig. 10. Yu et al. covered the two arms of a silicon MZI fast heat conduction for operating at a high speed modulation. The
with graphene layers to maintain the high extinction ratio, and one of measured rising and falling times of the thermal-optic modulations
the graphene layer was electrically heated to change the waveguide’s are 1.11 and 1.47 ls, respectively. Microring or microdisk resonators
refractive index, as shown in the left column of Fig. 10(a).123 The middle were integrated with graphene heaters as well for thermal modula-
column of Fig. 10(a) displays the transmission spectra of the MZI by tors,121,125 while the efficiency is lower due to the larger mode volume.
applying an electrical voltage over the graphene heater. With the varied Different from resonators, slow-light waveguides have advantages of
electrical powers from 0 to 110 mW, the interfering spectral fringe has a the enhanced light–matter interaction over a broadband wavelength
red shift of 7 nm. The high power consumption was the result of the range while the device footprint is compact.
02 November 2023 14:02:46
FIG. 10. Thermal-optic modulators assisted by graphene heaters, which are integrated on (a) MZI, (b) nanobeam cavity, and (c) slow-light waveguide. From left to right col-
umns show the device images, spectra shifts with different thermal powers, and temporal response times, respectively. (a) Reproduced from Yu et al., Appl. Phys. Lett. 105,
251104 (2014), with the permission of AIP Publishing. (b) Reproduced with permission from Xu et al., Opt. Express 25, 19479 (2017). Copyright 2017 Optical Society of
America. (c) Reproduced with permission from Yan et al., Nat. Commun. 8, 14411 (2017). Copyright 2017 Author(s); licensed under a Creative Commons Attribution (CC BY)
license.
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As mentioned above, the intrinsically slow processes of heat accu- with high extinction ratios.126–128 These devices operate with the
mulation and dissipation still limit the dynamic speed of these refractive index change of the whole microfiber, ensuring a high effi-
thermal-optic modulators. The graphene thermal modulator with the ciency and low power consumption. As a consequence, featured with
highest speed was reported by Yan et al.,122 as shown in Fig. 10(c). all-in-fiber, low power requirement, and ease of fabrication, these
This device employed a PC slow-light waveguide to integrate with a graphene-microfiber devices may open the door for graphene’s realistic
graphene strip heater. Owing to the enhanced light–matter interaction applications in all-optical signal processing.
by the slow-light, it is possible to reduce the device footprint as well An alternative approach to modulating the optical signal in the
for improving the tuning efficiency and speed. In addition, the gra- graphene-microfiber is tuning graphene’s optical properties, such as
phene channel is etched into a strip line overlapping on the waveguide, absorption or refractive index. The graphene’s linearly dispersed elec-
which guarantees the effective employment of heat to control the light tronic structure around the Dirac point allows easy tuning of carrier
propagation. To accelerate the heat conduction further, the buried density all-optically, which is in the timescale of picoseconds. By
oxide layer beneath the silicon PC waveguide was etched. The charac- inputting ultrafast pulses with high energy into the graphene-
terization results showed a high tuning efficiency of 1.07 nm/mW over microfiber, the optical field coupled with graphene could saturate its
the whole telecom-band and a fast temporal response with a rising absorption via the Pauli blocking or change the refractive index via the
(falling) time of 750 (525) ns. Kerr effect. The experimental configuration for all-optical modulations
is displayed in Fig. 11(d),40,129 respectively. The saturable absorption
D. Graphene-enabled fiber-based modulators in graphene requires a simple implementation, which could be realized
Optical fibers have revolutionized the applications of light in by measuring direct transmission of the hybrid graphene-fiber. To uti-
communication, signal processing, and sensing. Unfortunately, silica’s lize the graphene’s Kerr effect, which is expected to introduce a change
intrinsic passive attributes cannot support the realizations of fiber- of the effective refractive index in the graphene-microfiber, an MZI is
based modulators, switches, phase shifters, etc. External active devices needed to convert the phase modulation into the amplitude variation.
have to be connected to the fiber lines for functional optical systems. In both working mechanisms, modulation depths exceeding 40% were
Recently, graphene’s unique electrical and optical properties have obtained, and the response times were around 2 ps relying on graphe-
attracted researchers to make fiber-based modulators, which have ne’s ultrafast carrier dynamics, as shown in Fig. 11(e). In these ultrafast
potentials to simplify the package of optical systems. To couple gra- all-optical modulators, to significantly promote the carrier density in
graphene, effective graphene-light interaction is essential. Therefore,
02 November 2023 14:02:46

phene with the optical field in optical fibers, microfibers with diame-
ters of 1–10 lm were fabricated by flame heating or acid etching, or the microfiber’s diameters were preferred to be around 1 lm for more
“D”-shaped fibers were fabricated by polishing one-side of the conven- evanescent field leaking out. At the same time, considering the scatter-
tional fibers. These fibers could provide leaky evanescent fields around ing impurity and dephasing effect of carriers in graphene, even the sat-
them to couple with the integrated graphene layer. CVD-grown or urable absorption is achieved at high pump energy, graphene’s
exfoliated graphene layers were wrapped around the microfibers. intrinsic absorption loss cannot be absolutely inhibited, i.e., it is still
Figure 11(a) displays optical microscopic images of CVD-grown gra- quite lossy in the graphene-microfiber. Hence, for the 1 lm thick
phene-wrapped microfibers, which were fabricated by flame heating microfiber, the graphene-coating length should not be very long, and
and acid etching.41,126 By simulating the guiding mode distributions of the possible optimized range is about 10–40 lm.40,129 Though ultrafast
the graphene-microfiber, the graphene–light interaction could be esti- modulations were realized, this tiny thicknesses of the microfibers
mated, as shown in Fig. 11(b).41 The lower inset plots the zoomed mount challenges for their realistic applications due to the fragile
location of the graphene layer, which indicates that the graphene layer structure during the device fabrications and operations. In contrast,
induces an abrupt change in the optical field due to its large refractive thermal-optic graphene-microfiber modulators release the require-
index. Graphene’s absorption causes propagation attenuations of ment of very thin diameter attributed to the high efficiency of
0.49and 1.84 dB/mm for the guiding modes at 980and 1540 nm, thermal-optic effect, which improve the device stability. The
respectively. Hence, microfiber’s diameter and graphene length should graphene-cladding length does not have critical demands either due to
be designed carefully to avoid large insertion loss of the modulators. the low absorption by the graphene layer coated on a much thicker
Because of graphene’s gapless Dirac-fermionic band structure, the microfiber.41,126–128
absorption of microfiber’s evanescent fields could convert into thermal It is also possible to electrically fabricate tuned graphene devices
energy with very high efficiency, which, therefore, heats the microfiber. on fibers, as shown in Fig. 11(f). Lee et al. transferred a graphene layer
Relying on the fiber’s thermo-optic effect, a considerable refractive onto a “D”-shaped fiber and made an electrolyte-gated graphene
index variation could be obtained. Similar to the above on-chip ther- capacitor.130 The fiber’s planar surface provides a flat platform to
mal modulators, all-optical fiber modulators could be implemented. deposit metal electrodes as well as leak guiding mode to couple with
Gan et al. fabricated a device by wrapping a 5 mm long graphene graphene, as indicated in Fig. 11(f). Since the leaking optical field from
around a microfiber with a diameter of 10 lm. A phase shift exceeding the “D”-shaped fiber is much weaker than those from a tapered micro-
21p with a nearly linear slope of 0.091 p/mW (0.192 p/mW) was fiber, a long graphene layer is required to achieve a considerable inter-
obtained when pumped by light at the wavelength of 980 nm action between the coated graphene and the propagating mode. As
(1540 nm). It enables all-optical switching with a modulation depth of shown in Fig. 11(g), the fabricated device has a graphene length of
20 dB and a rising (falling) time of 9.1 ms (3.2 ms)41 [Fig. 11(c)]. With 5 mm. The electrical tuning mechanism of this devices is similar to
this graphene-assisted thermo-optic effect in the microfiber, a microfi- the one reported in Ref. 108. The drop-cast ion liquid could provide
ber Bragg grating and a microfiber knotted ring were all-optically an ultrathin (1 nm) carrier layer at its interface between graphene, gen-
tuned successfully for carrying out optical bistability and switching erating a strong electric field to dope graphene into high Fermi levels.
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FIG. 11. Optical fiber-integrated graphene modulators. (a) Optical microscopic images of graphene-wrapped microfibers fabricated by flame heating (top) and acid etching (bot-
tom). (b) Guiding modes across the center of the graphene-microfiber at the wavelengths of 980 and 1540 nm, where the upper inset is the 2D distribution of the mode at
1540 nm (graphene is indicated by the white line) and the lower inset is a zoomed-in image at the fiber edge. (c) All-optical modulation result obtained from the device in (a).
(d) Two experimental architectures to realize ultrafast all-optical modulator utilizing saturable absorption (top) and Kerr effect (bottom) in the coated graphene layer. (e)
Ultrafast modulation results from a graphene-coated microfiber operating in the regimes of loss modulation and phase modulation, respectively. (f) Schematic illustration of an
electrolyte gated graphene-fiber device, where a “D”-shaped fiber was employed to provide a platform for constructing graphene field effect transistor. (g) Fabricated electrically
tunable graphene-fiber device, showing a graphene length about 5 mm. (h) Tuned transmission from the graphene-coated fiber by applying different gate voltages. (a)–(c)
Reproduced with permission from Gan et al., Optica 2, 468 (2015). Copyright 2015 Optical Society of America. (d)–(e) Reproduced with permission from Yu et al., Optica 3,
541 (2016). Copyright 2016 Optical Society of America. (f)–(h) Reproduced with permission from Hong et al., Nat. Commun. 6, 6851 (2015). Copyright 2015 Author(s); licensed
under a Creative Commons Attribution (CC BY) license.
Figure 11(h) displays the gate-varied transmission of the fabricated active controller in an ultrafast laser considering its compatibility with
device coated with the graphene monolayer. A modulation depth over all-fiber systems.130
40% was obtained with a gate voltage of 2 V. Devices with even thicker
graphene layers were fabricated and tested. A high modulation depth IV. MID-INFRARED OPTICAL MODULATORS BASED
exceeding >90% was realized from a device with the graphene quad- ON GRAPHENE AND BLACK PHOSPHORUS
layer. Considering the slow carrier mobility of the ion liquid (smaller Mid-infrared electromagnetic waves in the wavelength range from
than 100 Hz), the employment of this electro-optic modulator in fiber- 2 to 30 lm are of great utility for chemical bond spectroscopy, free-
based signal processing is limited. However, it can function as an space communications, environment/health sensing, etc. Despite the
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tremendous efforts in developing mid-infrared sources and detectors,131 device dimension, the capacitance is too large to allow the fast modula-
a viable strategy toward realizing high-performance mid-infrared modu- tion speed. Note that graphene is too lossy to exhibit strong plasmonic
lators remains elusive. For instance, solid-state mid-infrared modulators properties in the mid-infrared, especially at energies above the
based on semiconductor quantum wells require sophisticated material 200 meV optical phonon energy of graphene.139 It would limit the per-
growth and cryogenic temperatures and the modulation depth is formance and future development of mid-infrared modulators based
small.132 Liquid crystal and digital micro-mirror based spatial light on graphene plasmonics.
modulators suffer from limitations including slow response speed and Though the plasmonic structures used to hybrid with graphene
complex instrumentation.133 could be designed to realize modulators over the whole mid-infrared
The above discussed largely tunable optical conductivity in gra- spectral range, the operation wavelengths of these reported graphene
phene in the telecom-band is valid for the mid-infrared radiations as mid-infrared modulators were mainly in the wavelength range between
well, which promises high-performance mid-infrared modulators on 6 and 8 lm. For realizing modulators in even shorter mid-infrared
the basis of the easy fabrication of graphene and the simple implemen- wavelength range, layered black phosphorus (BP), another emerging 2D
tation of electrical tuning. The limited interaction between the ultra- material, has much better optical and electronic properties. In addition,
thin graphene and the single-passed mid-infrared light should be compared with the graphene based mid-infrared optical modulators
overcome to realize a high modulation depth. The graphene modula- leveraging the intraband transition, BP’s on-resonance optical transition
tors in the telecom-band could be implemented by integrating it on has stronger light-matter interactions, which is friendly for the higher
optical fibers, waveguides, or resonators to enhance light-graphene modulation depth. The insertion loss could be got around with the assis-
interactions. However, determined by the main application scope of tance of the bandgap as well, as discussed in the following.
mid-infrared modulators, they should be operated in the free-space BP was first synthesized in 1914. Bulk BP was heavily investigated
configuration. Hence, plasmonic structures/antennas were widely to reveal interesting physical properties, such as high carrier mobility
employed to integrate graphene for enhancing mid-infrared light- and superconductivity.140 Inspired by various exotic properties
graphene interactions.134–137 In the hybrid graphene-plasmonic struc- obtained from mono- and few-layer graphene and TMDCs, BP was
tures, the free-space mid-infrared illumination could be captured by mechanically exfoliated into atomically thin flakes to perform electrical
the plasmonic antennas effectively. Furthermore, the localized hot- and optical characterizations.24,141–144 These rediscoveries of BP indi-
spots in the plasmonic nanogaps could interact with the graphene cated its few-layer could well bridge the gap between graphene and
strongly. On the other hand, the plasmonic antennas are normally TMDCs for constructing 2D material-based electrical and optoelec-
02 November 2023 14:02:46

designed with resonance modes in the mid-infrared range. By tuning tronic devices. For a field effect transistor, graphene promises ultrahigh
the optical conductivity of graphene, the resonance modes of the carrier mobility while fails in the on/off current ratio due to the gap-
hybrid graphene-plasmonic structures would be shifted in the wave- less. The large bandgaps of TMDCs could provide large on/off current
length or varied in the reflection/transmission amplitude, giving rise to ratios; unfortunately, the carrier mobilities meet obstacle to surpass sil-
the expected mid-infrared modulations. For example, Zeng et al. icon’s performance. Few-layer BP has been demonstrated to support
deposited arrays of “I”-shaped Au nanoantennas on a graphene field field effect transistors with drain current modulations on the order of
effect transistor, which has slightly conducting amphorous silicon as 105 and carrier mobilities up to 1000 cm2V–1s1.141 To respond an
the back gate and 6 nm thick Al2O3 as the dielectric layer.135 With the optical radiation, BP’s direct bandgap facilitates strong light-matter
free-space illumination of a broadband mid-infrared light, the reflec- interactions, and the value could be varied from 0.3 to 2 eV by chang-
tion spectrum of the hybrid graphene-plasmonic metasurface showed ing the layer numbers.145,146 These are different from graphene’s zero-
a clear resonance dip. By applying a low gate voltage around 7 V, a res- bandgap and large bandgap in TMDCs (normally larger than 1.5 eV).
onance wavelength shift of 1 lm was observed around the central Also, TMDC experience a transition from direct to indirect bandgap
wavelength of 8 lm, resulting in a large intensity modulation with a when the layer number is increased from monolayer to few layer.31
depth up to 90%. The low operation voltage benefits from the ultrathin Varying BP flakes from tetralayer to bulk, the direct bandgaps change
dielectric layer. The modulation speed was examined as well, which between a range of 0.6 and 0.3 eV, corresponding to the mid-infrared
could exceed 1 GHz. With the virtues of low-voltage operation and wavelength range of 2–4 lm.146 Recent reliable results of electrical
fast modulation speed, a prototype mid-infrared spatial light modula- doping on few-layer BP encouraged the implementation of BP-based
tor was demonstrated to function as an electrically encoded aperture mid-infrared optical modulators.24,141,142
or mask, realizing single-pixel imaging with a high frame rate. Lin et al. first theoretically investigated the electro-optic proper-
In addition to the hybrid graphene-plasmonic structure, gra- ties of few-layer BP flakes for optical modulations in the mid-infrared
phene has intrinsic plasmonic responses in the mid-infrared range due spectral range.147 As widely demonstrated in graphene and TMDCs,
to its intermediated carrier concentrations (1012 –1013 cm2). By pat- an out-of-plane electric field could modify their electronic structures
terning graphene into nanostructures to capture the free-space illumi- remarkably due to the strong vertical confinements of wave functions.
nated mid-infrared radiations, plasmonic resonance modes in Similarly, BP thin films could be considered as a quantum well, whose
graphene could be excited. If the optical conductivity of graphene was band edge allows a reliable electrical engineering to change the optical
tuned electrically, the transmitted amplitude of the mid-infrared light responses. As schematically shown in Fig. 12(a), an out-of-plane elec-
through the graphene nanostructure could be modulated around the tric field is applied via a BP capacitor or field effect transistor to shift
plasmonic resonance modes.138 Unfortunately, because only the pat- its band edge. Because of BP’s semiconducting nature, it would have a
terned graphene is the active layer of the modulator, the coupling effi- screening length of the out-of-plane electric field on the order of
ciency with the free-space mid-infrared radiation is low, which results 10 nm, which, thereby, allows the effective modification of band struc-
in a very small modulation depth about 6%. Also, limited by the large ture over the thin BP layer. Relying on the modified band structure,
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FIG. 12. Modulations of mid-infrared radiation using BP. (a) Schematic illustration of a BP-based mid-infrared modulator in a transmission regime. (b) Schematic of energy
band diagrams and wave functions (top), and energy dispersion diagrams (bottom) of a 5 nm thick BP at different doping levels. (c) Modulations of transmission spectra from a
BP field effect transistor with a 6.5 nm thick flake by comparing with the transmission spectrum at zero bias. (b) Reproduced with permission from Lin et al., Nano Lett. 16,
1683 (2016). Copyright 2016 American Chemical Society. (c) Reproduced with permission from Whitney et al., Nano Lett. 17, 78 (2017). Copyright 2017 American Chemical
Society.
BP’s optical conductivity (optical absorption) for a mid-infrared with larger photon energy than BP’s intrinsic bandgap Eg;i . The
optical beam at a specific wavelength could be electrically controlled, absorption of photons with energy larger than Eg;i is inhibited if Vg is
giving rise to the transmission modulation of the BP flake. larger enough to reach the BMS regime. Hence, by electrically gating
02 November 2023 14:02:46

Different from the gapless graphene, there are two effects BP for mid-infrared modulations, the two opposite electro-absorption
attributed to the modifications of BP’s optical conductivity in the mid- mechanisms (QCFK and BMS effects) should be considered together.
infrared range, which leverage the variations of band structures or The prominent role of the two effects is determined by the doping
carrier densities. Figure 12(b) schematically shows the energy band level and operating wavelength.
diagrams and wave functions (top), and energy dispersion diagrams Note that BP is an anisotropic material due to different effective
(bottom) of a 5 nm thick BP with different carrier densities.147 (1) For masses along the armchair and zigzag crystalline axes. The above cal-
a BP flake without doping or doped lightly, its optical bandgap Eg is culations were considered for the light polarized along the armchair
defined as the optical transition energy between the highest filled state direction, which has a higher optical conductivity and is more favor-
in the valence band and the lowest unoccupied state in the conduction able in modulation applications. In addition, for BP films with varied
band. In the intrinsic state, its electron carrier density is estimated to be thicknesses, the QCFK and BMS effects have different layer-
1:4 1010 cm2. The intrinsic bandgap is Eg;i ¼ Ec1 Ev1 ¼ 0:62 eV, dependences of the energy shifts. The BMS effect is only determined
where Ec1 and Ev1 are the energy levels of the first conduction and by the relative position between the Fermi level and conduction/
valence subbands, respectively, as indicated by the left column of valence band. Its energy shift is not sensitive to the BP thickness.
Fig. 12(b). (2) With the application of an external electrical gate, because However, since the electric field screening across the BP layer is the
of the electric field screening across the BP quantum well, electronic origin of band-bending, the energy shift induced by the QCFK effect
bands in different layers have a relative bending [middle column of for a thicker BP film has a larger value. For BP flakes thinner than the
Fig. 12(b)]. It brings the electron and hole subbands closer, which subse- tetralayer, the optical transition bandgap is around the telecom-
quently reduce Eg. This bandgap shrinkage could be described by the band.148 The excitonic effect would contribute to the optical conduc-
quantum-confined Franz–Keldysh (QCFK) effect. It would make the BP tivity in this case. The band-bending of QCFK effect is very weak due
film respond/absorb mid-infrared light with photon energies smaller to the thin layers. Fortunately, similar to the excitonic modulation of
than BP’s intrinsic bandgap. (3) With an electrical voltage applied over visible light in TMDC monolayers, an electric field could be applied to
the gate-oxide-BP layers, besides the effective electric field across the BP tune the oscillator strengths between excitons and trions to realize a
layer, carrier density is changed as well in the gate-oxide-BP parallel promising modulation on the telecom-band light.
capacitor, corresponding to the shifted Fermi levels EF. As Vg increases, These theoretical predictions of BP’s optical responses in mid-
the Fermi level could be raised (lowered) into the conduction (valence) infrared spectral ranges were experimentally verified by different
band due to the increased carrier densities [right column of Fig. 12(b)], groups.149,150 As shown in Fig. 12(c), transmission variations of the
such as in the level of 5 1012 cm2. The strengthened degenerated optical signals with photon energies in a range between 0.3 and 0.8 eV
carrier states make the optical transitions be Pauli blocked, i.e., the (i.e., the wavelength ranging from 1.55 to 4.1 lm) were extracted from
Burstein–Moss shift (BMS) effect. Different from the QCFK regime, the a BP field effect transistor with a 6.5 nm thick BP flake. By comparing
BMS regime broadens the optical bandgap Eg, which is defined as the transmission spectra obtained at different Vgs to that at zero bias,
Eg ¼ EF Ev1 . This enables the modulation of the optical conductivity modulation depths around 2% were obtained. The oscillations of the
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modulation amplitude and sign could be attributed to the co- graphene with a thin layer of silicon oxide. By applying Vg between
contributions of the QCFK and BMS effects.149 Similar results were them, the graphene’s Fermi level will be shifted and the conductivity
reported in Ref. 150, which also experimentally studied the depen- varies correspondingly. The transmission of the terahertz wave was
dence of BP thicknesses and doping levels. While the reported modu- measured to estimate the modulation by the graphene layer. In the vis-
lation depths of the vertically illuminated BP capacitors cannot ible and infrared ranges, graphene couples with light via the interband
support the realistic applications yet, a configuration with the integra- transition of carriers, whereas, for terahertz range, it is dominated by
tion of an optical waveguide or cavity could be employed to increase intraband transitions. In this long wavelength range, graphene acts as
the light–BP interaction and the modulation depth.86,147,149,151 Finally, a conductive film and the optical conductivity can be described by a
it is worth noting that these proposed and realized modulators employ simple Drude model. With this principle, on the fabricated devices, if
the shift of BP’s absorption band edge to control optical amplitude there is no applied voltage, the graphene’s Fermi level locates at the
directly. A phase-modulation should also exist in few-layer BP because Dirac point, wherein introducing minimum insertion loss or signal
the absorption variation is accompanied by the modified refractive attenuation. When an out-of-plane electric field is applied, graphene’s
index according to the Kramers–Kronig relation. carrier density was increased to shift the Fermi level and increase the
optical conductivity, which could reduce the transmission of the tera-
V. TERAHERTZ MODULATORS BASED hertz wave. Figure 13(b) displays the measured static characteristic of
ON 2D MATERIALS
graphene’s electrical conductivity and transmission of the terahertz
A terahertz electromagnetic wave, lying between radio frequency wave at 600 GHz. As expected, the transmittance increases with the
and infrared spectral bands, is attracting research interest due to its decreased electrical conductivity of graphene. Over the range of
important applications in biochemical sensing, communication, non- 570–630 GHz, the measured transmittances showed a flat modulation
destructive imaging, etc. Similar to the active devices in the mid- depth of 16% between the applied voltages of Vg ¼ 0 and 50 V, indi-
infrared range, while terahertz sources and detectors received rapid cating its broadband operation. To evaluate the experiment results,
progress recently, the modulations of terahertz waves still lack efficient simulations with the Drude model were implemented by considering
devices. The performances, including modulation depth, broadband graphene’s DC conductivities at different Vgs, which show their excel-
operation, insertion loss, and on-chip integrability, are required to be lent agreement. The dynamic characteristic of the fabricated graphene
improved. A variety of terahertz electro-optic modulators are devel- terahertz modulator was measured as well by modulating Vg with dif-
oped based on semiconductor heterostructures containing a 2D elec- ferent speeds. The response waveform to a square modulation voltage
02 November 2023 14:02:46

tron gas, where electrons can be accumulated or depleted by an indicates a rising time of 38 ls, and the measured 3 dB bandwidth is
applied voltage. However, limited by the electronic properties of the 20 kHz. This modulation speed is mainly limited by the device’s RC
conventional semiconductor heterostructure, it is difficult to achieve a time constant, which has a large capacitance C due to the large active
tunability of electron density larger than 1 1012 cm2. Hence, these device area.
devices can only modulate the terahertz wave with a low depth, which To further improve the modulation depth of graphene-based ter-
are normally in a range of a few percent. Even with the combinations ahertz modulator, Xing et al. modified the structure displayed in Fig.
of metamaterials or plasmonic structures,152 the modulation depths 13(a).155 A metal electrode was deposited on the backside of p-silicon,
are still no more than 30%, which sacrifice their broadband operations which functioned as the gate electrode and the reflector of terahertz
though. Contrastively, the graphene’s carrier concentration could be wave. When an electrical gate was applied between metal electrode
electrically tuned to a level as high as 1 1014 cm2, which also has and graphene layer, carriers got accumulated over the graphene layer
outstanding carrier mobilities. In addition, these carrier attributes are and the interface of silicon/silicon oxide. For p-silicon, the carrier con-
available for both holes and electrons owing to graphene’s symmetric centration at the top layer will not result in the significant variation of
conical band structure. These give rise to reasonably tunable conduc- the optical conductivity. The modulation of terahertz wave is mainly
tivity ranges relative to both electrons and holes for modulating tera- achieved by the graphene active layer, which has a strong shift of con-
hertz waves, which perform better than conventional semiconductor ductivity. The terahertz wave has a zero intensity at the back metal,
heterostructures realized only by electrons. and the wave strength in the graphene layer depends on the optical
Xing et al. first theoretically proposed the graphene-based tera- thickness of the substrate and the terahertz wavelength. If the total
hertz modulator after a comprehensive analysis of limits of the 2D thickness of the silicon and silicon oxide layers is an odd-multiple of
electron gas based terahertz modulator.153 Graphene was considered the terahertz wavelength, the field intensity in graphene is at maxima.
as a “tunable metal,” which could function as the gate electrode to bias In a fabricated device, a modulation depth of 64% was obtained at the
the 2D electron gas in a conventional semiconductor with a low inser- operation frequency of 620 GHz, which is about four times higher
tion loss. In the calculations, it was indicated that a graphene mono- than that obtained in the single-passed transmission geometry.154
layer can be nearly transparent when its Fermi level was tuned at the However, for the frequency of 590 GHz, there is no any change of the
Dirac point. In contrast, the absorption on the terahertz beam could reflection with different applied voltages, which could be attributed to
be almost 100% when the Fermi level is tuned for maximum conduc- the overlap of graphene with the minimum strength of the terahertz
tivity. This geometry supports broadband, polarization-independent, wave. Hence, this graphene modulator based on reflection geometry
and chip-integratable terahertz modulators.153 can only work in a narrowband range considering the interference of
The device structure of the first experimentally demonstrated the incident and reflected waves, while the modulation depth is signifi-
graphene-based terahertz modulator is displayed in Fig. 13(a).154 To cantly improved.
tune graphene’s carrier concentration, a p-type silicon substrate is cho- Another approach to boosting the modulation depth is integrat-
sen to provide a back gate, which is electrically separated from ing graphene into a metamaterial, as shown in Fig. 13(c).156 An array
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FIG. 13. Electro-optic terahertz modulator based on graphene. (a) Schematic illustration of a graphene-based terahertz modulator. (b) Measured graphene electrical conductiv-
ity and transmission of the terahertz wave at 600 GHz at different Vgs from a device with the geometry in (a). (c) Schematic representation of compositions of an active gra-
phene metamaterial. (d) Measured transmission (T) of the terahertz wave through the graphene metamaterial at different Vgs values and the estimated changes of amplitude
[DT=TCNP ð%Þ] and phase [D/ð Þ]. (e) Monolithically integrated graphene modulator on a terahertz quantum cascade laser. (f) Terahertz spatial light modulator enabled by
dual layers of graphene ribbons, which sandwich an electrolyte layer. (g) Terahertz transmission images of the spatial light modulator in (f) with various voltage configurations
recorded at a frequency of 0.37 THz. (a) and (b) Reproduced with permission from Sensale-Rodriguez et al., Nat. Commun. 3, 780 (2012). Copyright 2012 Author(s); licensed
under a Creative Commons Attribution (CC BY) license. (c) and (d) Reproduced with permission from Lee et al., Nat. Mater. 11, 936 (2012). Copyright 2012 Nature Publishing
Group. (e) Reproduced with permission from Liang et al., ACS Photonics 2, 1559 (2015). Copyright 2015 Author(s); licensed under a Creative Commons Attribution (CC BY)
license. (f) and (g) Reproduced with permission from Kakenov et al., Opt. Lett. 40, 1984 (2015). Copyright 2015 Optical Society of America.
of meta-atoms, an atomically thin graphene layer and an array of other hand, the linewidth of the resonance become broadened with large
metallic wire gate electrodes were configured together into an ultra- Vg due to the Joule losses in the metallic graphene layer. The variation
compact, thin and flexibly polymeric substrate. The meta-atoms could of the on-resonance transmission was estimated as high as 47% (58%)
be designed into hexagonal metallic frames or asymmetric double split relative to the maximum transmission with the employment of a
rings, which generate Fano like resonances. The metal wire array sup- (multi-layer) graphene monolayer. In addition, the phase change of the

plies a quasi-plane electrode to electrically gate the graphene layer for graphene metamaterial exceeds 40 at the resonance frequency, which
shifting the Fermi level. The graphene layer couples with the near-field provides possibilities to realize advanced phase-based terahertz devices.
of the Fano resonances of the meta-atoms. Hence, variations of graphe- The ability to synthesize and transfer of large scale graphene, as
ne’s refractive index and absorption would shift and broaden the Fano well as graphene’s flexibility and integrability, provides a further basis
resonance line shape. By measuring transmission of the terahertz wave to fabricate complex active terahertz devices. Liang et al. monolithi-
through the gate-controlled active graphene metamaterial, the ampli- cally integrated a graphene modulator onto a terahertz quantum cas-
tude and phase changes at different Vgs could be calculated, as shown in cade laser directly, as shown in Fig. 13(e).157 This device not only
Fig. 13(d). When Vg was tuned away from the charge neutral point, miniaturized the terahertz modulator for improved dynamic speed but
the resonant frequency redshifts gradually, which is attributed to the also greatly enhanced the modulation depth into a level close to 100%
increased real part of the complex conductivity of graphene. On the due to the enhanced interaction between graphene and terahertz
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radiation. More importantly, the monolithic integration of graphene graphene squares was patterned onto a substrate of silicon oxide/
with the terahertz laser got rid of the optical alignment and the associ- p-silicon. A metal layer was deposited on the backside of the substrate
ated bulky mirrors or lenses. as the reflector and electrode. By applying voltage between the back
It is also possible to design graphene modulators into an array for metal and the individual graphene squares, the reflectance of the inci-
realizing a terahertz spatial light modulator. Kakenov et al. fabricated a dent terahertz wave would be reduced greatly, which gives rise to
dual graphene layer supercapacitor with an electrolyte as the isolation spatially modulated patterns.
layer.158 The top and bottom graphene layers were patterned into rib- The graphene’s Fermi level could also be shifted via a photodop-
bons along the perpendicular directions. Thence, the intersections of ing process with the illumination of an optical beam. The increased
rows and columns define individually addressable pixels, as schemati- carrier concentration supports the intraband transition for absorbing
cally shown in Fig. 13(f). By applying a voltage difference between the terahertz wave effectively, enabling a high-efficiency all-optical modu-
corresponding row and column, a certain pixel could be addressed, lator. To realize a considerable doping level of the photo-carriers, visi-
which would block the transmission of the terahertz wave due to gra- ble or infrared pump light are preferred due to the strong interband
phene’s intraband transition. Figure 13(g) displays various spatial transition, corresponding to a magnitude of the absorbance of 2.3%. A
modulation patterns with different bias configurations for the tera- prototype of the all-optical modulator of terahertz wave is schemati-
hertz wave at a frequency of 0.37 THz. The broadband operation of cally shown in Fig. 14(a).160 A graphene layer was coated onto a highly
the spatial light modulator was estimated as well, showing a flat modu- doped silicon substrate. A near-infrared pump laser at the wavelength
lation depth over the frequency range of 0.1–1.5 THz and the modula- of 780 nm was employed to populate the carriers in graphene and the
tion depth around 50%. Another similar spatial light modulator was conducting silicon layer. The probe terahertz beam was launched
reported by Xing et al. in the reflection geometry.159 An 2D array of through the device area pumped by the near-infrared beam, which
02 November 2023 14:02:46
FIG. 14. Graphene-endowed terahertz modulator leveraging all-optical and magneto-optic effects. (a) Schematic representation of an all-optically controlled terahertz modulator
by pumping the photocarriers in graphene. (b) All-optical modulation result obtained from the device in (a). (c) Schematic illustration of Faraday rotation to a terahertz radiation
when graphene is actuated by a considerable magnetic field. (d) Faraday rotation angle measured under different magnetic fields. (a) and (b) Reproduced with permission
from ACS Nano 6, 9118 (2012). Copyright 2012 American Chemical Society. (c) and (d) Reproduced with permission from Crassee et al., Nat. Phys. 7, 48 (2011). Copyright
2011 Nature Publishing Group.
Appl. Phys. Rev. 9, 021302 (2022); doi: 10.1063/5.0078416 9, 021302-21

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would be controlled by the on-off of the pump laser. Here, a doped sil- VI. SUMMARIES
icon substrate was chosen for evaluating the modulation effect by gra- In this Review, we have discussed 2D material-endowed optical
phene. Figure 14(b) displays the modulation results of terahertz beams modulators operating over a spectral range between the visible and ter-
in the frequency range of 0.2–1 THz by a bare doped silicon substrate ahertz bands, including the underlying material properties, operation
and a doped silicon integrated with a graphene layer. Without the mechanisms, and device architectures. Benefiting from the plentiful
pump laser, the transmission spectra have nearly no variations electronic and optical attributes of 2D materials, the driven effects
between the terahertz beams transmitting through the bare silicon and employed in conventional optical modulators of bulk materials are suit-
graphene-on-silicon. With the illumination of pump laser, transmis- able to them too, including electro-optic, thermo-optic, all-optical, and
sions of the terahertz beams after the bare silicon and graphene-on-sil- magneto-optic effects. Note that 2D materials have distinct properties
icon are both attenuated. However, with the assistance of the graphene from conventional bulk materials to enable their modulators with
monolayer, the modulation depth is increased by 20%, giving a advantages. The gapless band structure of graphene with linear disper-
modulation depth of 72%. Graphene’s linear electronic dispersion sion allows the optical responses over the ultraviolet to microwave
could not only ensure the modulated terahertz beams in a wide spec- range. Combining with the easy tunability of the Dirac ferimons,
tral range, but also allow the pump light to be chosen in a broadband graphene-based optical modulations could be realized in the broad spec-
optical radiations for photodoping enough carriers.161,162 Over the tral range, representing the widest one in all of the reported optical
past few years, several studies also revealed TMDCs show interesting modulators. In monolayer TMDCs, the internal quantum efficiency of
ultrafast carrier dynamics and terahertz conductivity, which promises the light–matter interaction is boosted by the tightly bound excitons,
the control of terahertz beams optically by integrating them with which cannot be realized in conventional bulk materials. Modifications
doped silicons.163–165 of the electronic states in this few atomic layer would be much easier
In conventional bulk materials, the magneto-optic effect is an than that in bulk materials, and the power consumption is even lower.
alternative concept as well for constructing optical modulators with From the view of bulk materials, the realization of mid-infrared optical
the assistance of polarizers. With the magneto-optic Faraday (Kerr) modulators remains challenging due to the requirement of material
effect, when a linearly polarized light transmits through (or reflected platforms with versatile optoelectronic properties. Remarkably, few-
by) material in the presence of a magnetic field or magnetization, its layer BP with an optical response spectral range between 0.6 and 4 l
polarization plane rotates. This phenomenon can be thought of as the could provide strongly field-effect tuned bandgap. Its interband cou-
“optical-Hall effect” if its origin comes from the conducting electrons pling also imbued it with peak-like subband absorption features. Those
02 November 2023 14:02:46

or holes. The intrinsically fast magnetization reversal in the magneto- merits promise BP advantageous in making mid-infrared modulators
optic effect can go down to a timescale of few tens of femtoseconds. with low operation voltages.
This enables ultrafast modulators if the actuated magnetic fields were In the view of integrating modulators into light wave systems, 2D
fast enough. While modulators based on conventional magneto-optic materials’ flexibility and dangling-bond-free surface facilitate their
materials were reported widely,166 remarkable electronic properties in modulators to be fabricated on photonic structures. This could get rid
2D materials also promise groundbreaking magneto-optic effects for of the requirements of complex material growths and etchings
possible optical modulators. involved in the conventional integrated optical modulators.
Graphene has the low-energy band structure with a conical dis- Leveraging the well-developed industry applications of those photonic
persion in the effective-mass approximation, which offers interesting structures in telecommunication, data communication, and sensing,
physics including half-integer quantum Hall effect. Hence, under a those integrated 2D material modulators have great potentials to find
considerable magnetic field, the quantized Hall conductivity in gra- their realistic applications. For example, in chip-integrated graphene
phene could give rise to a modulated Faraday rotation angle to a tera- modulators reported by Sorianello et al.,117 device fabrications have
hertz radiation, as schematically shown in Fig. 14(c).167,168 With a been partly included in the standard silicon photonic foundry, paving
monolayer graphene grown on the silicon carbide substrate, a Faraday the way for their low-cost and mass production. Remarkably, from the
rotation angle exceeding 0.1 rad was obtained with a magnetic field up view of power consumption, operation speed, and extinction ratio, this
to 7 T at 5 K, as shown in Fig. 14(d). The spectra of rotation angles graphene electro-refractive modulator has advantages over those fabri-
show a strongly field-dependent edge-like structure, giving rise to a cated from conventional semiconductors.64
positive rotation angle at low energies and negative angle at high ener- Here, only the widely studied 2D materials, such as graphene and
gies. In addition, the Faraday rotation is quantized as well at precisely TMDCs, have been included for reviewing the optical modulators,
the quantum Hall steps governed by the Dirac electrons, and the rota- which already showed potentials for high-quality and large scale
tion angle is defined by the fine-structure constant. While the maxi- growth and transfer.172–174 These materials have stabilities to allow the
mum Faraday rotation is only 0.1 rad, it is an exceptionally large effect device prototype to develop into industries. While BP is considered as
considering graphene’s monolayer thickness. As the rotation angle is an unstable 2D material, the developed packaging techniques could
proportional to the distance traveled by the light, even larger rotation ensure the lifetimes of these electrical and photonic devices.175,176
angles were expected from thicker graphene layers.167,168 There are some other interesting 2D materials, which also support
Alternatively, giant Faraday rotation in graphene could be remarkably possible functionalities for optical modulations. For example, it has
enhanced by constructing resonators169 or patterning graphene into been theoretically demonstrated that the silicene monolayer, a 2D allo-

metasurfaces.170,171 These unique magneto-optic effects, while are trope of silicon, could exhibit an angle of 8 for Faraday rotations in
conceptually interesting, may open avenues for constructing terahertz the terahertz regime.177
magneto-optic modulators with ultrathin materials under quantum One of another well-known 2D materials is the hexagonal BN
mechanism. that has been recognized as the ideal substrate or dielectric layer for
Appl. Phys. Rev. 9, 021302 (2022); doi: 10.1063/5.0078416 9, 021302-22

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electrical and photonic devices based on other 2D materials.178 AUTHOR DECLARATIONS

Because of its wide electronic bandgap (6 eV), strong light–matter Conflict of Interest
interactions in BN are only expected in the wavelength range of deep
The authors have no conflicts to disclose.
ultraviolet (UV).179–181 The large bandgap also makes it difficult to
modify its electronic state for controlling the optical responses in the DATA AVAILABILITY
UV range with the conventional actuation effects, including electrical, Data sharing is not applicable to this article as no new data were
magnetic, and all-optical effects. There is still an absence of BN-based created or analyzed in this study.
optical modulators. Fortunately, BN could supply high quality phonon
polariton in the mid-infrared wavelength range relying on its long
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