8

PROGRESS REPORT
Transition Metal Dichalcogenides www.advmat.de
Monolayer Transition Metal Dichalcogenides as

Light Sources
Jiang Pu* and Taishi Takenobu*
layers are sandwiched at nanometer-scale

Reducing the dimensions of materials is one of the key approaches to discov- thicknesses. This quantum well fabrica-
ering novel optical phenomena. The recent emergence of 2D transition metal tion has expanded the potential of LED
dichalcogenides (TMDCs) has provided a promising platform for exploring applications, including high-brightness
new optoelectronic device applications, with their tunable electronic proper- LEDs,[3,4] high-performance optical mod-
ulators,[5,6] and laser diodes.[7,8] These
ties, structural controllability, and unique spin valley–coupled systems. This
notable advances have been primary attrib-
progress report provides an overview of recent advances in TMDC-based uted to controlling carriers (or photons) in
light-emitting devices discussed from several aspects in terms of device confined 2D systems, directly indicating
concepts, material designs, device fabrication, and their diverse functionali- that reducing the dimensions of materials
ties. First, the advantages of TMDCs used in light-emitting devices and their is a powerful approach to innovation in
optoelectronic functionalities and device
possible functionalities are presented. Second, conventional approaches for
applications. Therefore, intense research
fabricating TMDC light-emitting devices are emphasized, followed by intro- efforts have focused on exploring perfect
ducing a newly established, versatile method for generating light emission low-dimensional systems to develop LEDs
in TMDCs. Third, current growing technologies for heterostructure fabrica- with superior performance/efficiency and
tion, in which distinct TMDCs are vertically stacked or laterally stitched, are to investigate novel functionalities for
explained as a possible means for designing high-performance light-emitting next-generation optoelectronics.[9,10]
In recent years, 2D layered materials
devices. Finally, utilizing the topological features of TMDCs, the challenges
have attracted much attention as the best
for controlling circularly polarized light emission and its device applications platform for exploring new electronic,
are discussed from both theoretical and experimental points of view. optoelectronic, and photonic applications
based on the drastic evolution of their
physical properties in pure two dimen-
1. Introduction sions.[11,12] Many 2D layered materials exist in 3D bulk forms, in
which strongly bonded layers are stacked with weak interlayer
One of the greatest endeavors in human history has been the interactions. These materials are the so-called van der Waals
invention of artificial light sources, e.g., from candles, fila- layered materials, for example, graphite and molybdenum
ment lamps, fluorescent lights, light-emitting diodes (LEDs), disulfide (MoS2).[12] The layered structure allows the crystal to
and lasers. Such light sources are surely the backbone of cur- be readily cleaved along these layers, resulting in the isolation
rent lighting applications, optical communication technolo- of atomically thin layers that are pure 2D forms of materials.
gies, and sensing/monitoring devices. In the present optical In principle, these atomic layers are free from dangling bonds,
devices, one of the most fundamental components is the resulting in much higher structural stability than silicon and
light-emitting device that can directly convert electricity (cur- traditional compound semiconductors, such as gallium nitride
rent) to light (photons).[1] In past decades, tremendous efforts (GaN). The pioneering atomically thin material is graphene,[11]
have been successfully invested to realize LEDs using com- a monolayer form of a carbon atom honeycomb lattice isolated
pound semiconductors, as acknowledged by the Nobel Prize in from graphite, and it has encouraged primary research interest
Physics (2014).[2–4] Although the discovery of LEDs has boosted in 2D materials because its electronic structure differs dramat-
modern lighting and optical technologies, one significant ically from that of graphite, e.g., it has a unique linear band
breakthrough in conventional LEDs is the building of quantum dispersion with finite Berry curvature around the K (and −K)
well structures of materials, in which distinct semiconducting point.[13–15] This feature has yielded the half-integer quantum
Hall effect and the valley Hall effect in graphene,[16–19] and it
has enabled the creation of numerous graphene photonic and
Dr. J. Pu, Prof. T. Takenobu
Department of Applied Physics
optoelectronic devices, such as extremely broadband photode-
Nagoya University tectors and solar cells with high performance.[20–23] However,
Nagoya 464-8603, Japan the metallic nature (the absence of bandgaps) of graphene pre-
E-mail: jiang.pu@nagoya-u.jp; takenobu@nagoya-u.jp vents its intrinsic applicability in light-emitting devices.
The ORCID identification number(s) for the author(s) of this article In stark contrast to graphene, monolayer transition metal
can be found under https://doi.org/10.1002/adma.201707627. dichalcogenides (TMDCs), including MoS2, are direct bandgap
DOI: 10.1002/adma.201707627 semiconductors with tunable light-emitting properties ranging
Adv. Mater. 2018, 30, 1707627 1707627 (1 of 22) © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
15214095, 2018, 33, Downloaded from https://onlinelibrary.wiley.com/doi/10.1002/adma.201707627 by Delhi Technological University, Wiley Online Library on [29/05/2024]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
www.advancedsciencenews.com www.advmat.de
from visible to near-infrared wavelengths.[24–26] Analogous

with graphene, monolayer TMDCs provide naturally passi- Jiang Pu is an Assistant
vated 2D surfaces, creating light emission dominated by tightly Professor in the Department
bounded excitons (bounded states of electrons and holes) due of Applied Physics at Nagoya
to enhanced Coulomb interactions.[25,26] The large advantage of University, Japan. He received
TMDCs compared with traditional quantum wells is that they his B.E. and M.E. degrees in
enable different TMDCs to be stacked together to construct applied physics from Waseda
2D heterostructures without conventional “lattice mismatch” University, Japan. He com-
issues. Thus, the development of scalable fabrication and inte- pleted his Ph.D. degree in the
gration methods for those heterostructures will offer a simple Leading Graduate Program
way to design and modulate the optical properties of mate- in Science and Engineering
rials.[27–29] In addition, the atomically thin features of TMDCs at Waseda University in
directly translate to the mechanical flexibility of materials, pro- 2017, supported by Ministry
viding potential applicability for flexible and stretchable device of Education, Culture, Sports, Science and Technology
applications.[30,31] Moreover, monolayer TMDCs have a peculiar (MEXT). During his Ph.D. program, he was selected for
electronic structure arising from their broken spatial-inver- the Research Fellowship for Young Scientists from Japan
sion symmetry and strong spin–orbit interactions, allowing Society of Science (JSPS). His research interests include
us to control circularly polarized light emission and resulting electronic and optoelectronic properties of 2D materials
in a new optoelectronics field called “valleytronics.”[32–34] Con- and their device applications.
sidering these 2D physical and electronic virtues, monolayer
TMDCs are among the best candidates to explore in new func- Taishi Takenobu has been a
tional LED applications. Professor in the Department
In this progress report, we focus on recent advances in of Applied Physics at Nagoya
TMDC-based light-emitting devices from physical aspects: University, Japan, since 2016.
device concepts, material designs, device fabrication, and He received his Ph.D. in
functionalities. In the first section, the general properties and materials science from Japan
advantages of TMDCs are widely reviewed with experimentally Advanced Institute of Science
revealed unique optical signatures, inspiring promising func- and Technology (JAIST) in
tionalities for TMDC light-emitting devices. Second, commonly 2001. After his half-year
used approaches for fabricating TMDC LEDs based on tran- research fellowship in Sony
sistor configurations are highlighted. In particular, we intro- Corporation, he became an
duce here our newly established, simple, and versatile method Assistant Professor (2001)
for generating light emission in TMDCs, which could be ben- and an Associate Professor (2007) at the Institute of
eficial for both scalable applications and investigations of fun- Materials Research in Tohoku University, Japan. In 2010,
damental physics. Third, the notable growing technology of he was appointed as an Associate Professor at Waseda
heterostructure fabrication is presented as an efficient method University, Japan, and then promoted to a Professor in 2013.
for designing high-performance LEDs. Two typical types of His research interests include novel physical properties and
heterostructures—vertically stacked (out-of-plane) and later- devices of organic materials and low-dimensional materials.
ally stitched (in-plane) heterojunctions—are explained for each
preferable application. Importantly, we examine the differences to each other by weak van der Waals forces. Bulk TMDCs have
in LED properties between vertical and lateral heterostacks diverse physical properties, ranging from insulators, semicon-
based on recent observation of unique light emission in lateral ductors, semimetals, and metals to superconductors.[35,36] In
heterojunction LEDs. In the final section, we provide a perspec- particular, group-VI TMDCs, notably known as MoS2, are semi-
tive for realizing novel functional LEDs utilizing spin-valley conducting material series with bandgap of 1–2 eV. These prop-
coupling of TMDCs. The challenges for controlling circularly erties indicate that, by changing proper atom combinations,
polarized light emission and its device applications are dis- we can selectively choose materials for optoelectronic devices
cussed from both theoretical and experimental points of view, with the desired wavelength ranges. The rich variety of TMDCs
and possible future subjects are also discussed. is beneficial for device applications; however, TMDCs usually
exhibit indirect bandgaps in their bulk forms, and they are not
suitable for fabricating light-emitting devices. In this section,
2. Transition Metal Dichalcogenides the variations in the electronic and optical properties of TMDCs,
such as decreasing numbers of layers, are explained, and the
for Optoelectronics
emergence of remarkable optical signatures in the monolayer
TMDCs are denoted by the formula MX2 (where M is a transi- form is highlighted through recent experimental results.
tion metal atom from groups IV to VI, and X is a chalcogen
atom), and they have a hexagonal structure consisting of a metal 2.1. Evolution of Electronic Structures in Monolayers
atom (M) layer sandwiched between two chalcogen (X) layers
(Figure 1a).[24] The intralayer M–X bonds are predominantly The geometric confinement effect, by reducing the thickness
covalent, whereas the neighboring sandwich layers are coupled of layered materials, induces the drastic evolution of energy
Figure 1. a) 3D schematic illustration of a TMDC crystal structure. The chalcogen atoms are represented by X, and transition metal atoms are rep-
resented by M. Reproduced with permission.[24] Copyright 2012, Nature Publishing Group. b) The calculated band dispersions for bulk, quadrilayer,
bilayer, and monolayer MoS2, respectively. Reproduced with permission.[38] Copyright 2010, American Chemical Society. c) The comparison of PL
spectra between bilayer and monolayer MoS2. The inset indicates the layer number dependence of PL quantum efficiency. d) Normalized PL spectra for
various layer numbers of MoS2. e) The layer number dependence of the lowest PL peak energy in MoS2. The dashed line indicates the indirect bandgap
energy of bulk MoS2. Reproduced with permission.[39] Copyright 2010, American Physical Society.
dispersion in materials, known by the relationship between In general, the indirect energy transition in bulk or multilayer
graphite and graphene.[15] Similar to the initial production MoS2 requires the mediation of phonons and/or impurity scat-
method of graphene, individual TMDC monolayers with thick- tering to compensate for the momentum difference, resulting
nesses of ≈0.7 nm can be mechanically peeled off from their in poor luminescence capability because electrons tend to decay
bulk crystals using Scotch tape.[12,24,37] The change in the band with nonradiative recombination when they are excited from
structure occurs because of the quantum confinement that the valence band to the conduction band via optical excitation.
comes from decreasing the number of layers, triggering hybridi- In contrast, direct interband energy transition at the K point
zation between the pz orbital of the chalcogen atom and the d contributes to higher photoluminescence (PL) intensity in the
orbital of the transition metal atom.[38,39] For example, the layer monolayer form. As shown in Figure 1c, the PL quantum yield
number–dependent band structures for MoS2 calculated by the increases by a factor of ≈104 as the layer numbers decrease
density functional theory are shown in Figure 1b.[38] Comparing from bulk to monolayer.[39] The dependence of the layer
the sequences of band structures with different thicknesses of number on the normalized PL spectrum and its peak energy
MoS2, the gap energy for the direct transition at the Brillouin profiles are shown in Figure 1d,e. The main peak of ≈1.8 eV
zone K point is almost constant because the conduction band of monolayer MoS2 barely shifts to a lower energy as the layer
states around the K point are predominated by the localized number increases, whereas an additional peak originating from
d orbitals of the Mo atoms, which are located in the middle of the indirect bandgap transition appears in multilayer samples.
the S–Mo–S configuration. This configuration offers minimal Although both PL intensities from the direct and indirect band-
interlayer coupling and results in a relatively unaffected band gaps coexist in multilayer MoS2, most of the excited electrons
variation. In contrast, the indirect energy gap is sensitive to the relax at the bottom of the conduction band with nonradiative
number of layers and becomes the largest state in the monolayer recombination. These optical excitation measurements are con-
form. Since the states near the Γ point are composed of the anti- sistent with the band calculation indicated in Figure 1b, and
bonding pz orbitals of the S atoms and the d orbitals of the Mo they have also been confirmed by photoconductivity and optical
atoms, they are strongly affected by interlayer coupling and they absorption measurements.[39,40]
sensitively depend on the layer number. Therefore, as the layer In addition to MoS2, molybdenum diselenide (MoSe2),
number decreases to a monolayer, there is a transition from an molybdenum ditelluride (MoTe2), and tungsten-based
indirect bandgap (≈1.3 eV) to a direct bandgap (≈1.8 eV). dichalcogenides, such as tungsten disulfide (WS2) and tungsten
The unique change in the electronic band structure in the diselenide (WSe2), belong to the same family of semiconducting
monolayer form also creates advantageous optical signatures. TMDCs. These materials also show significant electronic
evolution by decreasing monolayer thickness like that of MoS2; By comparing the emission energy difference between exci-
for instance, monolayers MoSe2, MoTe2, WS2, and WSe2 show tons and trions, a large trion binding energy of 30 meV can be
direct bandgaps of ≈1.5, ≈1.1, ≈2.0, and ≈1.7 eV, respectively, extracted. Similar properties of trions and their large binding
with 103 of enhanced PL efficiency compared to those of bulk energy have also been observed in other monolayer TMDCs,
materials.[41–44] These semiconducting monolayer series cer- such as MoS2.[62] Importantly, this large binding energy ren-
tainly can be associated for use in active layers of light-emitting ders the trion formation in TMDCs stable even at room
devices with wavelengths ranging from visible to near-infrared temperature, which cannot be realized in most traditional semi-
frequencies. Furthermore, other families of 2D TMDCs, such conductors. In addition, the formation of biexciton states has
as rhenium disulfide (ReS2) and rhenium diselenide (ReSe2), been observed, and their binding energy (≈15 meV) was also
with a bandgap of ≈1.5 eV can possibly be chosen as near- remarkably large.[64–66] These observations and electrical control
infrared optoelectronic devices.[45,46] Apart from TMDCs, which of quasiparticle emissions directly reflect the many-body phe-
is another single-element layered material black phosphorus (or nomena of monolayer materials and open a door to developing
phosphorene in monolayer form), phosphorus atoms are cova- efficient strategies for manipulating excitonic effects. Moreover,
lently bonded with three adjacent phosphorus atoms to form a the tightly bound excitons could provide exciting opportunities
puckered honeycomb structure, which is also promising mate- for engineering light–matter interactions. For example, sev-
rial for optoelectronics applications.[47,48] The bandgap of phos- eral studies have reported that hybridizing monolayer TMDCs
phorene with a few layers is able to be tuned by decreasing the with metal nanostructures (or nanoparticles) achieved strong
thickness, leading to a bandgap ranging from ≈1.8 eV in mono exciton–plasmon coupling and accordingly enhanced their
layer to ≈0.3 eV in bulk.[48–50] Unlike TMDCs, few-layer phos- light absorption and emission (Figure 2d).[67–69] The signifi-
phorene retains a direct bandgap; thus, this material offers the cant enhancement of PL quantum yield, nearly 100% with the
potential ability for use in building mid-infrared light-emitting longest exciton lifetime, has also been demonstrated by chem-
devices. It should be noted that, because phosphorene is rapidly ical surface modification.[70,71] The robust mechanical structure
degraded upon exposure to air due to oxidization, the develop- of TMDCs has enabled their integration with photonic crystal
ment of encapsulating techniques for phosphorene devices is cavities and microdisk cavities, resulting in optical pumped
necessary toward practical applications.[51,52] lasing with low threshold power (Figure 2e).[72–74] These valu-
able approaches to exciton engineering via light–matter inter-
action and surface functionalization suggest new directions
2.2. Excitonic Photoluminescence for realizing highly efficient 2D light-emitting devices and
laser diodes.
The reduced layer number of TMDCs not only affects electronic The excitons in TMDCs offer further significant optical
structures but also yields interesting optical features. In the functionalities as a consequence of their peculiar crystal sym-
monolayer limit, the dielectric screening effect is sufficiently metry.[32–34] Since monolayer TMDCs consist of an M–X–M
weak, resulting in great enhancement of Coulomb interactions hexagonal structure, the spatial-inversion symmetry is explic-
between electrons and holes.[53–56] These confined carriers in itly broken (Figure 1a). In addition to their noncentrosym-
monolayer TMDCs form a quasiparticle state, exciton, which metric nature, the strong spin–orbit interaction originating
has an energy structure of a hydrogen atom.[57–60] In fact, the from the d orbitals of the transition metals splits the valence
Rydberg series of energy levels of the excitonic states have bands; for instance, for MoS2 at ≈160 meV, its value depends
been proved by PL measurements in monolayers MoS2, WS2, on the materials.[75–78] As shown in Figure 3a, because the
and WSe2.[57–60] Interestingly, the exciton binding energy in K and −K valleys are related to one another by time reversal sym-
monolayer TMDCs has been theoretically and experimentally metry, opposite spin states are charged at valence band maxima
reported in the range of 500–900 meV, which is one order of (and conduction band minima) between the K and −K valleys,
magnitude greater than that of conventional quantum wells leading to broken spin degeneracy.[77,78] Hence, the interband
consisting of III–V semiconductors.[53–60] These outstanding transition at the two valleys is coupled with optical helicity; the
excitonic effects mediated by confinement effects and strong optical transition is exclusively controlled by right (σ+) or left
Coulomb interactions provide further control of excitons in (σ–) circularly polarized light. Optically excited valley-polarized
truly 2D systems. excitons that carry the valley degree of freedom have been
Excitons can be additionally charged by binding electrons experimentally proved using polarization-resolved PL meas-
or holes to form three-body quasiparticle states, called charged urements.[79–82] Figure 3b presents the polarization-resolved
excitons (trions).[61–63] Trion formation can be electrically tai- PL spectrum (σ+ and σ− components) in monolayer WSe2,
lored by combining PL measurements and transistors, which excited by σ+ incident light.[33,82] With this optical pumping
can examine excitonic properties by controlling the carrier den- measurement, circularly polarized light can selectively excite
sity of TMDC monolayers via gating.[61,62] Figure 2a shows a an exciton in one valley. Consequently, exciton (or trion) PL is
schematic of back-gated transistors with exfoliated monolayer detected to be strongly polarized, as well as having the same
MoSe2. As the positive (negative) gate voltage changes, electron circular polarization of incident light, providing direct evidence
(hole) accumulation is induced in MoSe2.[61] In the presence of valley polarization. The control of valley populations by cir-
of doped electrons (holes), the conversion from optically trig- cularly polarized light is associated with the quantum Berry
gered excitons to negative (positive) trions occurs, as illustrated phase; the carriers in each valley experience the opposite effec-
in Figure 2b. Figure 2c directly shows the experimental results. tive magnetic field. The existence of Berry curvature generates
As gate voltage increases, all neutral excitons become trions. transverse velocity for the carriers without an external magnetic
Figure 2. Excitonic properties of monolayer TMDCs: a) optical image (top) and schematic (bottom) of a MoSe2 transistor. The scale bar is 5 µm.
b) Illustration of the gate-voltage tuning exciton (X0) and trion (X±) formations. c) 2D mapping of MoSe2 PL as a function of gate voltage. Note that
XI originates from trapped excitons. Reproduced with permission.[61] Copyright 2014, Nature Publishing Group. d) Schematic representation of exciton–
plasmon coupling to enhance the luminescence capability of TMDCs mediated by metal nanoparticles. Reproduced with permission.[67] Copyright 2016,
Wiley-VCH. e) Schematic depiction of WSe2 monolayers assembled on a photonic crystal cavity and their PL properties. The red and black lines (arrows)
correspond to the detected directions of linear polarization. Reproduced with permission.[72] Copyright 2015, Nature Publishing Group.
field, followed by induction of an anomalous Hall effect, as and valleys as information carriers. Therefore, monolayer
predicted by theory.[32,83] When the electric fields are biased TMDCs are the best candidates for using the valley degree of
to monolayer TMDCs, electrons (or holes) located at different freedom to explore new classes of electronic and optoelectronic
valleys (K or −K) experience opposite Lorentz forces and move device applications, yielding the concept of valleytronics.[88–94]
to opposite directions due to valley-dependent effective mag-
netic field, which is a phenomenon called the valley Hall effect
(Figure 3c).[84] In principle, these driven carriers compensate 3. Monolayer Light-Emitting Devices
for each other so that no net Hall voltage is generated. There-
fore, the initial valley Hall effect has been detected by irradi- The unique optical properties of monolayer TMDCs urgently
ating circularly polarized light, which could cause population inspire optoelectronic device applications. The two most impor-
imbalance between the two valleys to create finite Hall voltage. tant general optoelectronic devices are photodetectors (or solar
Another experimental method used Kerr rotation microscopy to cells) and light-emitting devices: one converts photons to current
directly observe the polarization at the edge of materials driven and the other does the opposite. Since high-performance tran-
by the valley Hall effect.[85] Although these valley-selective trans- sistors based on TMDCs have been demonstrated in an initial
port carriers utilize the valley degree of freedom as information benchmark study,[95–99] phototransistors with the capability for
flow, similar strategies have also recently been applied in the light absorption have been represented as a promising opto-
quantum transport of excitons, called the exciton Hall effect electronic device application.[99–102] In fact, ultrasensitive MoS2
(Figure 3d).[86] The consequent exciton diffusion originating phototransistors[101] and selective wavelength detection origi-
from the carrier concentration and the temperature gradient nating from a thickness-tunable bandgap have been successfully
experienced transverse motion in each valley,[87] as detected by achieved,[102] presenting possible use of TMDCs for light sensing
spatial polarization-resolved PL mapping.[86] This theoretical applications and photovoltaic cells. In contrast to phototransis-
and experimental proof of valley polarization and the anoma- tors, the formation of a p–n junction is greatly required to realize
lous Hall effect driven by the internal topological nature of efficient EL generation, and it is the primary element for fabri-
monolayer TMDCs reflect the potential ability to control spin cating LEDs. In the initial study, the fabrication of light-emitting
Figure 3. Valley polarization and valley transport phenomena. a) Schematic drawing of the band structure and valley contrasting the optical selection
rule in monolayer TMDCs. The interband transition in each K and −K valley is coupled to right-handed (σ+) and left-handed (σ−) circular polarized
light, respectively. b) Polarization-resolved PL spectra for monolayer WSe2 caused by σ+ light. Reproduced with permission.[33] Copyright 2014, Nature
Publishing Group. c) Conceptual illustration of the valley Hall effect driven by an electric field. d) Schematic depiction of the exciton Hall effect driven
by a temperature gradient. Reproduced with permission.[86] Copyright 2017, Nature Publishing Group.
devices has been limited by the observation of electrolumines- wavelengths from visible to near-infrared ranges, and they have
cence (EL) near the Schottky contact of metals in SiO2-back-gated superior transport properties, such as high electron and hole
MoS2 transistors.[103] Because MoS2 transistors have typically mobility of ≈100 cm2 V−1 s−1.[24,25,96–98] These physical proper-
shown heavy n-doped behavior, it has been difficult to create p–n ties are advantageous for use in LED applications. In general,
junctions. This obstacle has addressed the relevant approaches LEDs require the formation of a p–n junction, and conven-
to adopt advanced device structures such as split-gated and tional LED fabrication has adopted several techniques for cre-
electrolyte-gated transistors to enhance polarity control. Further- ating p–n junctions, including ion implantation,[104] atomic
more, MoSe2, WS2, and WSe2 have been chosen as suitable can- substitution,[2,105] chemical surface functionalization,[106,107]
didates for realizing TMDC LEDs because they can easily obtain and heterostructure fabrication[3–8,27–29] as will be discussed in
both hole and electron transports. In this section, we highlight Section 4. However, because these carrier doping methods are
the current progress in terms of several experimental methods not yet fully feasible in TMDC monolayers, and they have only
for the fabrication of TMDC p–n junction LEDs, and we explain been established in commonly used materials, such as III–V
their diverse EL properties. In particular, we introduce our newly semiconductors, it is difficult for emerging semiconductors to
established versatile approach to generate EL in TMDCs, which obtain EL. Therefore, relevant research on fabricating TMDC
provides a much simpler device structure and fabrication pro- LEDs has been performed with electrostatic gating, in which
cess, compared to commonly used approaches for building scal- two separate transistors (split-gate transistor configuration) are
able TMDC LEDs. Possible work in designing high-performance assembled on one TMDC film to turn the polarity to p-type and
and new functional TMDC LEDs is also discussed here. n-type transistors, respectively.[108–113]
Figure 4a provides a schematic illustration of split gate
electrodes coupled to two different regions of an exfoliated
3.1. p–i–n Light-Emitting Diodes WSe2 monolayer film.[108] Because monolayer WSe2 can easily
obtain ambipolar transport, both hole and electron transport
Monolayer TMDCs, especially for MoS2, MoSe2, WS2, and can be achieved in identical WSe2 film, enabling efficient
WSe2, are atomically thin direct bandgap semiconductors using electrostatic control for tuning the polarities of materials. By
Figure 4. WSe2 monolayer p–i–n diodes. a) Schematic of split gate transistors with exfoliated monolayer WSe2. The width of the trench (d) is 460 nm.
b) I–V characteristics of the device under light irradiation. The solid green line represents the bias condition in p–i–n junction operating mode, the
solid blue line is the n–i–p mode, and the dashed blue line shows the p–p unipolar operating condition. The inset presents electrical power (Pel) versus
voltage under illumination. c) EL spectra measured at various current injections. The inset shows the injected current dependence of the emission
amplitude of EL. Reproduced with permission.[108] Copyright 2014, Nature Publishing Group. d) EL intensity plot as a function of injected current and
the photon energy of a WSe2 monolayer p–i–n diode. The image shows the mean peak features in EL spectra, corresponding to the neutral exciton
(X0), negative and positive trions (X±), and the impurity-bound exciton (XI), respectively. e) The 2D mapping of PL spectra as a function of gate voltage
and photon energy. f) Band diagram showing recombination processes of valley excitons in a p–i–n junction. Both K and −K valleys are equally popu-
lated to generate right-handed (σ+) and left-handed (σ−) circularly polarized EL, resulting in no polarization in the total EL spectrum. Reproduced with
permission.[110] Copyright 2014, Nature Publishing Group.
applying a negative gate voltage and a positive gate voltage transistors, indicating efficient electron-hole recombination
to each gate electrode, respectively, hole and electron accu- in p–i–n diodes.[103]
mulations are induced with spatial separation in the channel Due to the similarity between EL and PL spectra, the recom-
region. The trench region in Figure 4a is not affected by elec- bination is dominated by direct-gap excitons owing to their
trostatic gating, indicating intrinsic conditions. This local large binding energy. This result indicates that we can manipu-
gate control results in a p–i–n (or n–i–p) junction in a WSe2 late unique exciton properties to use their light-emitting device
monolayer. To examine the quality of fabricated p–i–n diodes, functionalities. To gain a further understanding of the nature
Figure 4b indicates the current–voltage (I–V) characteristics of EL, Figure 4d shows intensity mapping of EL spectra as a
under optical illumination. The clear rectification behavior function of injected current at low temperatures.[110] The asym-
and the production of the open-circuit voltage and short- metric spectrum features represent mixed spectral contribu-
circuit current are obtained by recording a fill factor value tions. Figure 4e indicates the 2D mapping of PL spectra as a
of ≈0.5. The estimated power conversion efficiency reaches function of gate voltage in the same transistor configurations,
0.5%, which obviously shows that fabricated p–i–n diodes and the observed PL peaks by changing gate voltage correspond
exert efficient photovoltaic effects.[108–113] The high quality to neutral excitons, negative and positive trions, and impurity-
of p–i–n junction formation readily allows for EL genera- bounded exciton states. Comparing the EL results (Figure 4d)
tion from WSe2, as shown in the EL spectrum in Figure 4c. with the PL results (Figure 4e), the peak features in the EL
By tuning the current injections, the EL intensity is linearly spectra at each current injection can be assigned to these exci-
enhanced, and its peak energy is ≈1.6 eV, corresponding to tonic peaks, agreeing reasonably well with the results of the PL
direct bandgap energy transition of monolayer WSe2. The measurements. Finally, the schematic representation occur-
external quantum efficiency (EQE) is calculated at up to ring in this system is summarized in Figure 4f. The contribu-
0.1% at room temperature, which is several orders of mag- tion of exciton (and trion) EL implies that valley excitons could
nitude higher than the initial EL observation in n-type MoS2 play a significant role in recombination processes at intrinsic
or doped regions, but no polarized EL was observed here top). In contrast, when the gate voltage is much smaller than
because of cancelation at each (K and −K) valley recombination the drain voltage, the effective gate voltage contribution near
(Figure 4f).[110] Nevertheless, these experimental investigations the drain electrode is inverted, which addresses the accumula-
of EL properties in monolayer TMDCs provide viable possi- tion of the opposite type of carrier and induces both the hole
bilities for controlling circularly polarized EL only by breaking and electron accumulations inside TMDCs (Figure 5a, bottom).
populations between K and −K valleys, for instance, using fer- Figure 5b indicates the transfer characteristics of MoS2 EDLTs,
romagnetic contacts for spin-polarized current injection and/ and clear ambipolar transport with high on/off ratios of >105
or inducing intense electric field, possibly creating novel func- is obtained. In this ambipolar condition, although the p–i–n
tional LEDs arising from valley degrees of freedom of TMDCs junction is simultaneously induced during application of bal-
(as discussed in Section 5). anced gate and drain voltage, it is necessary for realizing p–i–n
diodes to fix the doped regions. Therefore, to fix the electrostati-
cally induced p–i–n junction, the device is cooled to 180 K after
3.2. Ambipolar Light-Emitting Transistors applying a voltage sufficiently lower than the glass transition
temperature of the ionic liquids to freeze the movements of the
The successful demonstrations of the fabrication of monolayer ions (ion rearrangements). This step allows for the stable for-
p–i–n diodes using split-gate transistors emphasize that the mation of p–i–n junctions, as shown in the rectification curves
electrical controllability of device structure is important to real- of Figure 5c, so that we have directly demonstrated the photo-
izing high-quality p–i–n junctions. However, there are limits to detecting ability of this frozen p–i–n junction, and it has exhib-
carrier density control in conventional transistors with oxide ited one of the most sensitive photodetection and low-power
gate dielectrics such as SiO2, resulting in limited applicability consumption properties among TMDC p–i–n diodes.[137] This
of materials that can obtain ambipolar transport. In most cases, p–i–n diode fabrication has been applied to several TMDCs,
the performance of monolayer TMDC transistors is easily and the EL spectrum has been measured.[138–142] For example,
affected by naturally implanted impurities and/or defects.[114,115] Figure 5d,e shows the direct observation of EL images from
For example, the vacancies of sulfur atoms serve as uninten- monolayer WS2 EDLTs and its EL spectrum.[141] Although the
tional electron doping sites in MoS2, resulting in crucial trap luminescence image is unclear, mainly because of the use of
states and the pinning effect of the Fermi level in MoS2 tran- a droplet of ionic liquids and the tiny sample size, the consist-
sistors.[114,115] In addition, these effects degrade polarity con- ency between the PL and EL spectrum proves the generation of
trol and have caused typically (heavy-doped) n-type behavior in WS2 direct-gap exciton EL. Importantly, in addition to group VI
reported MoS2 transistors.[24,95–99] Introducing high-k materials semiconducting TMDCs, that EL spectra are observed in bulk
as gate dielectrics, such as HfO2, can reduce the adverse effects ReS2 EDLTs is one significant advance for expanding possibili-
due to their efficient carrier density control and wide-range ties toward near-infrared to mid-infrared light-emitting device
band filling, and in fact, almost all high-performance TMDC applications (Figure 5e).[130] Bulk and few-layer ReS2 is gener-
transistors have been fabricated using high-k dielectric mate- ally an indirect bandgap material, so it is commonly difficult
rials.[116–119] Therefore, a device configuration with high capaci- to obtain EL. Since the high capacitance of EDLTs can induce
tance is necessary to increase the variety of TMDCs for use in high carrier density and high current density in materials and
light-emitting device applications. devices, it would facilitate carrier recombination to generate EL
In this regard, a transistor configuration using electrolytes in ReS2, directly reflecting the efficient combination of electro-
such as ionic liquid as a gate dielectric material, so-called lytes and TMDCs for investigating EL properties in emerging
electric double layer transistor (EDLT), is one of the desir- 2D semiconductors, such as black phosphorus, as a future
able candidates.[120,121] Owing to the high specific capacitance subject.
(≈10 µF cm−2) of EDLTs, they can achieve several times larger
electric fields and one order of magnitude higher carrier den-
sity accumulation, compared to typical SiO2-back-gated transis- 3.3. New Approaches for Light-Emitting Devices
tors.[122,123] These properties have allowed for some beneficial
transport properties that are difficult to realize in conventional Although either split-gated or electrolyte-gated transistors have
TMDC transistors, such as ambipolar transports with low enabled the formation of p–i–n junctions, these methods inevi-
operating voltages (<4 V) and high mobility (>100 cm2 V−1 s−1) tably apply a constant gate voltage. Regarding device applica-
in MoS2, MoSe2, WS2, WSe2, ReS2, and black phosphorus.[124–130] tions, polarity control using an external gate electrode is a
Furthermore, electric field–induced insulators to metal and disadvantage due to its limited structural applicability. Consid-
to superconductor transition have been realized, directly visu- ering this drawback, efforts should be made to discover a new,
alizing the effectiveness of the electrostatic controllability of versatile and simple approach for fabricating light-emitting
EDLTs for tuning material transport properties.[131–135] There- devices without local gate control. In 1995, one of the simplest
fore, the combination of EDLTs and TMDCs could expand the methods to generate light emission was reported by Pei et al.
applicable materials for building light-emitting devices. based on electrochemistry.[143,144] These devices were named
Figure 5a presents the schematics of MoS2 EDLTs based on light-emitting electrochemical cells (LECs), made by a mixture
ionic liquid gating as an example to explain the operation mech- of electrolytes and organic polymers with two electrodes. In
anisms.[136] The device structure replaces oxide dielectrics only LECs, both the electrochemical oxidization and reduction are
with ionic liquids. When the gate voltage is applied, one type caused by the voltage application, leading to the formation of a
of carrier is accumulated in the transistor channel (Figure 5a, p–n junction.[145–148] To increase the simplicity of LEC concept,
Figure 5. Ambipolar TMDC light-emitting transistors using ionic liquids. a) Schematics of unipolar and ambipolar operations in MoS2 EDLTs. Top:
Unipolar accumulation occurred when the drain voltage (VDS) is smaller than the gate voltage (VGS). Bottom: Ambipolar accumulation is induced when
VDS is sufficiently larger than VGS. b) Ambipolar transfer characteristics measured at 220 K. c) The I–V curves are shown for both 220 and 180 K. The
device is cooled from 220 to 180 K to form stable p–i–n junctions. The inset shows a logarithmic plot of an I–V curve obtained at 180 K. Reproduced
with permission.[136] Copyright 2013, American Chemical Society. d) EL image recorded in a WS2 monolayer ambipolar EDLT. e) The comparison of
PL and EL spectra for a WS2 EDLT. Reproduced with permission.[141] Copyright 2014, American Chemical Society. f) EL spectra obtained from a ReS2
ambipolar EDLT under various bias conditions. The blue and dashed gray lines are the PL spectra measured for thin (<30 nm) and thick (>150 nm)
flakes, respectively. Reproduced with permission.[130] Copyright 2016, IOP Publishing.
we placed an electrolyte on TMDCs with two electrochemically with polymer. Because the thickness of ion-gel films is 100 nm,
stable electrodes, as shown in the schematic of Figure 6a, called it is sufficiently flat and transparent to perform spectroscopic
electric double layer light-emitting diodes (EDLEDs).[149] In the measurements, compared to a droplet of ionic liquid, as a com-
initial condition, ions are uniformly distributed in the electro- parison between Figure 5d (ionic liquids) and Figure 7a (ion
lytes. By applying a voltage between two electrodes, anions and gels).[149,150] Figure 7b illustrates schematic depictions of the I–V
cations drift in the opposite direction, and they form EDLs on and light-emission measurements; a photodiode was set on top
each electrode surfaces (Figure 6b). The intense electric field of of EDLEDs and recorded their photocurrents (Iph). As shown in
EDLs is partially applied to the metal/semiconductor interface, Figure 7c, both I–V and Iph–V characteristics showed a nonlinear
contributing to the injection of charge carriers into the semi- enhancement with increasing voltage. In addition, the loga-
conductor through the Schottky barrier narrowing and the tun- rithmic plot displayed in the inset of Figure 7c indicates that Iph
neling effect. These tunneling carriers are captured by ions so was linearly enhanced with a slope of 1, indicating constant EQE
that EDLs are formed on the electrolyte/semiconductor inter- due to p–i–n junction formations. We also performed EL imaging
face. When large voltage is applied, both holes and electrons are and spectroscopy, and observed clear light emission from a WSe2
injected, followed by occurring transient electrostatic doping to EDLED (Figure 7d). Figure 7d shows the comparison between
form n-doped and p-doped regions (Figure 6c). Finally, in the PL and EL, and their perfect consistency revealed that EL was
equilibrium condition, the dynamic p–i–n junction is induced; generated from the direct-gap exciton recombination.
thus, the recombination of holes and electrons is expected in EDLEDs feature significant advantages compared with pre-
the intrinsic region (Figure 6d). viously reported TMDC LEDs in terms of easy fabrication,
To prove this device concept, Figure 7a shows an optical image durability, and applicability to emerging materials. Compared
of a fabricated WSe2 monolayer EDLED. Two gold electrodes with transistor configurations,[108–113] EDLEDs only require
were patterned on the chemical vapor deposition (CVD)-grown two electrodes and putting electrolyte without any local gate
centimeter-scale monolayers on sapphire substrates, followed control, offering a much simpler structure and easier fabrica-
by spin-coating ion-gel films and gelation of ionic liquids mixed tion. The simplicity of EDLEDs evolves its device applicability.
Figure 6. Conceptual diagram of EDLEDs. a) Schematics of a two-terminal light-emitting structure with an electrolyte. b) When a small voltage is applied
between two electrodes, the ion replacement is induced, and anions and cations distribute to opposite side of the electrode. c) When a large voltage is
applied, electrons and holes are injected from the electrodes, followed by the inducing of p- and n-doped regions originating from the electric double
layers formed at the electrolyte/semiconductor interfaces. d) In the equilibrium condition, the p–i–n junction is dynamically formed. As the bias further
increases, the recombination of holes and electrons occurs in the intrinsic region to generate EL. Reproduced with permission.[149] Copyright 2017,
Wiley- VCH.
In particular, monolayer TMDCs are inherently flexible, so device lifetime, for instance, we continuously applied pulsed
the combination of EDLEDs and CVD-grown monolayers voltage into devices with high current density of 7.5 kA cm−2
inspires large-area, flexible, and stretchable light-emitting for more than 500 cycles. The device showed stable operation
devices as a reasonable target. Indeed, the transfer technique without degradation, representing excellent reproducibility and
of CVD-grown monolayers has been already established, and device stability. We expect that this robust light-emitting struc-
highly flexible and fully stretchable device applications have ture increases the ability of TMDCs for electrical-driven laser
also been realized.[151,152] Moreover, we also investigated the diodes. To reach this goal, the combined EDLEDs with cavities
Figure 7. Large-area TMDC monolayer EDLEDs. a) Optical microscope image of a CVD-grown WSe2 monolayer EDLED. The top panels show the
channel region with/without spin-coated ion-gel films. b) Schematic depiction of the light-emitting measurement setup, in which a Si photodiode is
placed atop the devices to collect emitted photons as photocurrent (Iph). c) The I–V (gray) and Iph–V (red) characteristics of a WSe2 device, respectively.
The inset shows the logarithmic plot of I and Iph. The gray triangle represents the slope of 1. d) The comparison of PL (gray) and EL (blue) spectra for
a WSe2 device. The inset exhibits an EL image obtained from a WSe2 device under bias condition. Reproduced with permission.[149] Copyright 2017,
Wiley- VCH.
and/or distributed feedback/Bragg reflectors should be a desir- above section, another key approach to realize LEDs is het-
able device structure,[72–74] and performing high current pulsed erostructure fabrication. Semiconductor heterostructures that
measurements could be a possible future work. Finally, we also enable the building of quantum wells have been among the
realized EDLEDs with ZnO, GaN, and organic single crystals. most fundamental platforms to yield many important optoelec-
Although ZnO and GaN are naturally doped semiconductors, tronic device applications, such as highly bright LEDs, high-per-
these results emphasize that EDLEDs are applicable to highly formance laser diodes, and so on.[3–8] Analogous to traditional
doped unipolar materials and are not only an efficient approach heterostructures, mainly based on III–V semiconductors, 2D
to the TMDC family, but they are also available to other inor- materials, including graphene, hexagonal boron nitride (hBN),
ganic materials. In ordinary cases, although chemical doping TMDCs, and black phosphorus, promise perfectly matched het-
is regarded as one of the most promising methods for creating erostructures, in which dissimilar or similar 2D materials are
LEDs, it inevitably requires a long time to establish reliable stacked layer by layer. The intrinsically passivated surfaces of
doping techniques in new materials. The chemical modifica- these materials, indicating the absence of dangling bonds, can
tion methods of TMDC monolayers is still under develop- be vertically stacked together (van der Waals heterostructure) or
ment.[153,154] Therefore, we believe that EDLEDs provide a laterally stitched together in atomic precision without strict lat-
versatile platform for discovering light-emitting devices using tice mismatches.[27–29] In principle, heterostructures made from
emerging materials. 2D materials eventually yield atomically regulated and sharp
interfaces, allowing us to explore unusual electrical and optical
phenomena and to make outstanding improvements to device
4. Heterostructure Light-Emitting Devices performance.[155–157] In this section, we focus on recent progress
in heterostructure fabrications to apply TMDC LEDs from both
In addition to several techniques adopted for p–i–n junction geometries: vertical van der Waals heterostructure and lateral
formation in an identical TMDC monolayer described in the heterojunctions. Important findings in terms of unique optical
properties, device applications, and future assembly techniques respectively. This type of heterostructure has been demonstrated
are highlighted, followed by a discussion of the different situ- as a tunneling diode with negative differential resistance,[158]
ations between vertical and lateral heterostructures for light- tunneling transistors,[159] and photovoltaic devices.[160,161] Ren-
emitting device applications, based on recent experimental dering these metal–insulator–semiconductor (MIS) band struc-
observations. tures with tunneling barriers, both electrons and holes can be
injected into the active layer of TMDCs from two graphene
electrodes, and the recombination of electrons and holes leads
4.1. Van Der Waals Heterostructure LEDs to light emission from an operational LED. Comparing an
optical image of a fabricated device (Figure 8c) and its EL image
The most commonly adopted technique for assembling verti- (Figure 8d), the whole area of the device shows bright EL, and
cally stacked van der Waals heterostructures remains mechan- the maximum EQE in this MIS type of heterostacked LED has
ical exfoliation due to its commendable quality control of each been recorded at up to 10% both at low temperatures and at
monolayer. The idea of stacking different 2D materials requires room temperature.[162,163] The significant enhancement of light-
a powerful method for band structure engineering with atomic emitting performance supports the effectiveness of 2D multiple
precision, allowing us to design high-quality tunneling bar- heterostructures for LED applications in many aspects, such as
riers and quantum wells.[158–162] Figure 8a schematically shows the selectivity of active materials, reduced contact resistance,
the architecture of quantum well structures comprising single low threshold current density, and the manipulation of radia-
and multilayers of TMDCs, graphene and hBN.[162] The atomi- tive recombination by geometrical confinement.[164] Since this
cally sharp interfaces of layers without interlayer contamina- MIS-type heterostacked LED can generate light emission from
tion can be clarified using cross-sectional bright-field scanning the whole area of the device, it has enabled the examination
transmission electron microscope (STEM) images, as shown of spatially localized EL in materials and has determined the
in Figure 8b. In these structures, graphene, hBN, and TMDCs generation of single photon emission, which has elevated a
(WS2 in Figure 8a) serve as a transparent conducting layer, an new class of quantum emitters toward hybrid, broadband atomi
insulating layer for tunneling barriers, and an active material, cally thin quantum photonic devices.[165,166] Moreover, this
Figure 8. Vertical van der Waals heterostacked TMDC LEDs. a, b) Schematic illustration of the quantum well LEDs constructed by heterostructures of
graphene, hBN, and WS2, and its cross-sectional bright-field TEM image. The scale bar is 5 nm. c,d) Optical image and EL image of the heterostacked
LEDs. The scale bar is 10 µm. Reproduced with permission.[162] Copyright 2015, Nature Publishing Group. e,f) Schematic depiction and band diagram
of the WSe2/ MoS2 van der Waals structure p–n diode. g) The EL spectra of a WSe2/ MoS2 p–n diode obtained at different current injections. The
marked EL peaks of A, B, A′, and B′ originate from the excitonic features of WSe2, and the EL peaks of I come from the indirect-gap transition of MoS2.
Reproduced with permission.[171] Copyright 2014, American Chemical Society.
architecture can also be assembled on photonic crystal nano- approach, and this approach remains as a popular method for
cavities.[167] The integrated heterostacked 2D LEDs have gained studying fundamental properties and for performing device
a cavity-enhanced mode of EL with a high degree of linear tests, the low throughput and the lack of scalability of the
polarization and a high-speed modulation ability of 1 MHz. The mechanical exfoliation technique have hampered their prac-
integration of nanocavities with atomically thin light emitters is tical device utility. In this regard, direct growth methods, such
an essential step toward on-chip nanoscale photonics and could as physical vapor transport, CVD, and molecular beam epitaxy,
possibly lead to the realizing of electrically pumped laser. are suitable for the scalable and reproducible manufacturing
Although MIS-type tunneling diodes have important abili- of van der Waal heterostructures.[181–183] To date, many suc-
ties for high-performance LED applications, their heterostruc- cessful reports have detailed the growth of various combina-
ture, consisting of different members of TMDCs, has inspired tions of vertical heterostructures based on 2D materials, such
a variety of material and device designs. When the family of as MoS2/graphene, MoS2/hBN, MoS2/WS2, WS2/WSe2, WSe2/
semiconducting TMDCs is stacked together, it provides various MoSe2, and MoSe2/Bi2Se3.[27–29] These robust formations of van
band offsets, categorized by type I (straddling gap), type II (stag- der Waals structures have also been linked to the fabrication
gered gap), and type III (broken gap), which have been theo- of p–n diodes and examinations of their photodetection and
retically and experimentally examined across different TMDC photovoltaic properties, providing a viable route for easier and
heterostructures.[27–29,168] These band offsets are inherently larger-scale production.[157,183] Despite these advances in chem-
crucial parameters for designing device functionalities, and ical synthesis and van der Waals epitaxy approaches, the fab-
the type II heterostructure is particularly exciting for managing rication throughput, scalability, layer thickness controllability,
light harvesting.[169–171] One typical type II heterostructure can and patterning ability of such vertical heterostructures remain
be formed by stacking monolayers WSe2 and MoS2, as shown severely limited, and it is inevitably difficult to develop large-
in Figure 8e,f.[171] In type II band alignment, the atomically area integration of heterostacked devices.
flat interface of the TMDC heterostructure facilitates charge Recently, another important strategy for fabricating 2D heter-
transfer and enhances the interaction between adjacent layers, ostructures has been explored, namely, lateral heterojunctions,
resulting in photoexcited electrons and holes accumulating in in which different types of TMDCs are artificially stitched along
different layers—called interlayer excitons.[172–174] These inter- in-plane directions. Compared with manual transfer or selec-
layer excitons have been observed in several combinations of tive growth of vertically stacked heterostructures, lateral het-
heterostructures (e.g., MoSe2/WSe2).[172–174] Interestingly, such erojunctions can be ideally adopted for the scalable approach
interlayer excitons typically have long lifetimes and show spin- to CVD methods for a growing variety of TMDCs, which are
valley polarization with long valley lifetimes; thus, these unique able to create various high-quality TMDC heterojunctions with
emerging optical properties could lead to new optoelectronic scalable size, controllable thickness, reproducible device fabri-
applications for TMDC heterostructures.[174,175] As shown in cations, and lithographic patterning processes. In addition to
Figure 8f, when WSe2 is used as a p-type material, and MoS2 these virtues for the application side, lateral heterojunctions
serves as an n-type material, they naturally provide the oppor- are easier to tune for band offset and design electronic prop-
tunity to create atomically sharp p–n junctions. These TMDC- erties at junction interfaces because of their spatial separation.
based heterostacked p–n junctions have shown efficient charge Thereby, the direct CVD growth of TMDC lateral heterojunc-
separation and photocurrent generation so that the recorded tions with atomically sharp interfaces is a key challenge. In the
EQE exceeded 10%. In addition, Figure 8g shows the measured initial study of the growth of lateral heterojunctions, a one-step
EL spectrum from a WSe2/MoS2 p–n junction with increasing CVD process was used to yield in-plane connections, such as
current injections. The EL spectrum indicates multiple exci- MoS2-MoSe2, WS2–MoS2, and WS2-WSe2, which exhibited
tonic peaks and hot electron luminescence peaks arising from typical p–n junction properties.[184–186] These demonstrations
WSe2, as well as the indirect-gap emission peak of MoS2, which provide a simple method for lateral heterojunction formations;
reasonably closely agrees with the band offset of the WSe2/ however, their junction interfaces were thermodynamically pre-
MoS2 heterostructure.[168] Furthermore, the van der Waals ferred alloy structures due to the coexistence of precursors in
heterostructure, based on p-type black phosphorus and n-type the vapor phase during the synthetic process. To obtain lateral
monolayer MoS2, has enabled the creation of p–n photodiodes heterojunctions with atomically sharp interfaces, a controlled
with high photodetection sensitivity.[176] Therefore, TMDC- two-step CVD process to synthesize WSe2–MoS2 lateral junc-
based heterostructure fabrications could provide a new pathway tion was developed.[187] As shown in the schematic flow of
for designing atomically thin p–n diodes for creating high-per- Figure 9a, WSe2 is first grown via van der Waals epitaxy with
formance photovoltaic and light-emitting devices, and they offer a high growth temperature (925 °C). Then, to avoid the alloy
an attractive platform for exploring new classes of excitonic reaction, the edge epitaxy of MoS2 is secondarily grown along
device applications. The recent advent of mixed-dimensional the W growth front in a separate furnace at a lower tempera-
van der Waals heterostructure geometries, for instance, 2D ture (755 °C). The two steps involve a large difference in the
materials stacked with 3D and/or 1D materials, also provides a growth of temperature, and the careful retention of precur-
feasible way to develop novel optoelectronic devices.[177–180] sors allows for precise control to yield the atomically sharp
transition in compositions at the junctions. The high-quality
4.2. Lateral Heterojunction LEDs WSe2–MoS2 lateral junction interface can be revealed by optical
images (Figure 9b) and STEM images (Figure 9c), with ≈90%
Although numerous experimental demonstrations of van der of W atoms implanted at the junction interface to bridge two
Waals heterostructures have been realized using the Scotch-tape pairs of Se atoms and one pair of S atoms. A similar strategy
Figure 9. Scalable growth of lateral heterojunction TMDC LEDs. a) Schematic flow of the sequential growth of the monolayer WSe2–MoS2 lateral
heterojunctions. b) Optical image of a WSe2–MoS2 laterally stitched monolayer flake. c) High-resolution STEM image obtained from a WSe2–MoS2
heterojunction interface. Reproduced with permission.[187] Copyright 2015, American Association for the Advancement of Science. d) Schematic of
the fabrication process of the two-step location-selective and self-aligned WSe2–MoS2 lateral heterojunction films. e) Photograph of the WSe2–MoS2
heterojunction light-emitting device arrays patterned on sapphire substrates. f) Optical image of a WSe2–MoS2 heterojunction interface area selected
from device arrays. The dashed white lines roughly trace the shape of the junction interface. g) EL image measured at bias condition, showing clear light
emission along the junction interface. The scale bar is 10 µm. h) The comparison of PL (gray) and EL (blue) spectra at the WSe2–MoS2 heterojunction
part. Reproduced with permission.[189] Copyright 2017, Wiley- VCH. i) Band diagram of a WSe2–MoS2 heterojunction interface acquired from the results
of scanning tunneling spectroscopy. The interface area becomes type I band alignment due to charge transfer and strain effects, consequently domi-
nating the recombination process at the lateral heterojunction interface. Reproduced with permission.[190] Copyright 2017, Nature Publishing Group.
can also be coupled with lithographic processes to pattern these revealed. Toward wafer-scale device applications and integra-
heterojunction flakes. For example, the initially grown TMDC tions, we more recently established a new CVD process for
monolayer can be patterned by lithography, such as ion beam synthesizing spatially controlled and self-aligned monolayer
etching, followed by the growth of a second TMDC monolayer WSe2–MoS2 lateral heterojunctions, and we have first demon-
to adjust the etched area seamlessly.[188] strated their light-emitting device arrays.[189] Figure 9d illus-
Although the direct growth of atomically sharp lateral het- trates the schematic flow for the synthetic process of WSe2–
erojunctions is preferred for use in p–n junction device appli- MoS2 lateral heterojunctions. In the first step, W metal layers
cations, the relevant approach still has limitations for their are lithographically patterned on a sapphire substrate for the
scalability and geometric control. Moreover, despite intense subsequent location-selective growth of WSe2 monolayers. The
investigations of photoelectric conversion in lateral heterojunc- edges of patterned W metals can act as a catalyst to facilitate
tions,[183–187] their light-emitting device application has not yet WSe2 growth. Then, a two-step CVD process is performed to
been realized, indicating that the fundamental nature of EL form WSe2–MoS2 lateral heterojunctions. Third, Mo metal
properties at lateral heterojunction interfaces has not yet been layers are deposited on MoS2 film regions to construct
W (electrode)-WSe2–MoS2–M (electrode) diode structures. In explore novel light-emitting (or photodetecting) functionali-
the final step, ion-gel films are spin-coated on the heterojunc- ties originating from their unique band structure, as shown
tion film surface to ensure carrier injection and accumulation in Figure 3a. Owing to the lack of spatial-inversion symmetry
for realizing p–n junctions. Figure 9e shows optical images of and strong spin–orbit interaction in monolayer TMDCs, their
prepared device arrays with selectively patterned interface areas. electronic properties at the band edge are associated with the
The spatial separation between monolayer WSe2 and MoS2 two inequivalent valleys of the K and −K points.[32] These val-
domains can be identified by the optical contrast (Figure 9f). leys are able to behave as opposite signs of binary pseudospins
The atomically sharp interfaces without alloy formation were in K and −K valleys, respectively, consequently leading to the
also characterized by spatial Raman and PL mapping, leading realization of valley polarization controlled by optical helicity
to scalable, location-selective, and geometry-controlled growth (Figure 3b).[79–82] These topological natures indicate that mono
approaches.[189] layer TMDCs are the best flatland to manipulate valley degrees
To realize p–n junctions for observing EL, by applying voltage of freedom as a new type of information carrier and storage,
between W and Mo electrodes, both holes and electrons are called valleytronics.[33,34] It should be noted that, although the
injected, and they formed EDLs for carrier accumulations on concept of the use of the valley index for carrying information
WSe2 and MoS2 surfaces (Figure 9f). WSe2 is then tuned to the was initially investigated in silicon and aluminum arsenide (or
p-type and MoS2 to the n-type so that a p–n junction is formed graphene more recently), the ability to manipulate for toward
by bridging the junction interface. As shown in Figure 9g, the device functionalities has been strictly limited.[18,83,192] For real-
light emission is obviously generated along the heterojunction istic device application, one could be motivated to realize the
interface, indicating that carrier recombination dominates the optoelectronic emitters and absorbers arising from valley polar-
interfacial electronic structure at junctions. Figure 9h compares ized excitons, indicating an opto-valleytronic interconnection
the measured EL and PL spectra at the junction interface. Inter- that can electrically generate circular polarized light emission
estingly, although the PL spectrum shows exciton contributions and absorption. This establishment will be one building block
from both monolayers WSe2 and MoS2, the EL only presents for the development of valley functional device applications in
excitonic features and a localized state arising from MoS2. In TMDC-based valleytronics.
principle, the heterostructure based on WSe2 and MoS2 should To realize such opto-valleytronic devices, it is required to
be type-II band offset, as shown in Figure 8f, indicating that control the populations of valley polarized carriers in each
both WSe2 and MoS2 EL and/or interband emission is pref- valley to interconvert valley polarization to emitted or absorbed
erably observed.[164–170] At the same time, the inconsistency photons. For example, the demonstration of the valley Hall
between PL and EL behavior shows that the peculiar band effect depicted in Figure 3c is direct evidence of the conver-
alignment at the WSe2–MoS2 heterojunction interface domi- sion from optically triggered valley information to electrical
nates the EL properties. On the basis of a recent scanning tun- flows.[84,85] Interestingly, valley-dependent photocurrent gen-
neling spectroscopy study, the charge transfer and a large strain eration, in which the photocurrent in a two-terminal devices
effect at the junction cause steep band bending in the valence or transistors can be modulated by the optical helicity of inci-
band minimum of MoS2 to shift it to greater than that of WSe2, dent light, is also a possible way to control valley information
resulting in a type-I alignment at the junction interface instead to electrical information.[193,194] In contrast to the valley optical
of a type-II alignment (Figure 9i).[190] Hence, holes in WSe2 selection rule using circularly polarized light, the direct conver-
domains can travel to MoS2 domains, but electrons in MoS2 sion of electrical currents to circularly polarized light, as well as
cannot pass to WSe2, so the recombination mainly occurred at the translating of electrical information to valley information, is
MoS2 domains. This situation reasonably agrees with the exper- desirable for designing light sources for future quantum infor-
imental results shown in Figure 9h. Similar band offset evolu- mation technology. However, establishing the solid manner for
tion at lateral heterojunction interfaces has also been obtained electrical control valley polarized EL remains unclear, resulting
at a WS2–MoS2 heterojunction, suggesting a common feature in the limited utility of valley light-emitting devices in aspects
for designing light-emitting device based on lateral heterostruc- of reproducible performance, polarization controllability, and
tures, unlike the predicted interfacial structure of vertical heter- operational temperature. Currently, two approaches are mainly
ostructures.[191] Our developed scalable and geometry-controlled used to realize chiral light-emitting devices using TMDCs. One
growth technique and the observation of unique EL properties is injection of a spin-polarized charge carrier directly from fer-
provide significant insights for exploring optoelectronic device romagnetic semiconductors or contacts to create circularly
applications based on lateral heterojunction films, which could polarized EL.[195,196] Because the valence band of monolayer
be a key platform for achieving wafer-scale circuit integration. TMDCs has large spin splitting, which is the opposite at the
distinct valley (K or −K), it leads to a spin-valley locking rela-
tionship and causes long valley-spin lifetime suppressed spin
5. Perspective: Spin-Valley light-Emitting devices and valley scattering by locking effects.[197,198] In this system,
as shown in Figure 10a, the vertical heterostructure p–n diode,
As discussed above, the ongoing efforts to fabricate TMDC where monolayer WS2 as an n-type semiconductor is stacked
light-emitting devices have demonstrated many advantages on a p-type ferromagnetic semiconductor (Ga,Mn)As, can
for applying next-generation optoelectronic devices with perform specific spin injection in the out-of-plane direction,
wide-range color tunability, high performances, mechanical which is the manifested direction of the spin-locking effect.[195]
deformability, scalability, and so on. In addition to these phys- Applying voltage to this heterostacked p–n diode causes unbal-
ical virtues, monolayer TMDCs offer the significant ability to anced valley populations between the K and −K valleys due to
Figure 10. Valley LEDs via spin injection using ferromagnetic materials. a) Schematic of the monolayer TMDC/(Ga,Mn)As heterostacked LED. (Ga,Mn)
As is used as a spin injection substrate via spin alignment by an external magnetic field. b) Helicity-resolved (σ+ and σ−) EL spectra obtained from
WS2/(Ga,Mn)As LED in the presence of an external magnetic field at 10 K. The polarized EL originates from spin-polarized holes. Reproduced with
permission.[195] Copyright 2016, Nature Publishing Group. c) Schematic drawing of the monolayer WSe2/MoS2 heterostacked LED with ferromagnetic
contacts attached to WSe2, as a hole spin injection electrode. d) Helicity-resolved EL spectra of a WSe2/MoS2 LED under two opposite magnetic field
conditions at 4.2 K. The helicity of EL is inversed with the changing injected spin alignment. Reproduced with permission.[196] Copyright 2016, American
Chemical Society.
injected spin-polarized holes, forming the intensity difference approach utilizing intense lateral electric fields has been pro-
between right- and left-handed circularly polarized EL posed to control circularly polarized EL in TMDCs.[138–140,203,204]
(Figure 10b). By changing the alignment of injected spins by Theoretical calculations offer the use of nonlinear valley current,
tuning the external magnetic field, the helicity of this valley polar- which simply occurs by applying lateral bias to materials.[204]
ized light emission can also be reversed. In addition to vertical Owing to the trigonal warping of the valence band due to the
spin injection geometry via magnetic substrates, a simpler device hexagonal lattice, the spin and valley currents can be generated
geometry using ferromagnetic electrodes has also been adopted by an electric field, as depicted in Figure 11a. The anisotropy of
to control circularly polarized EL. Figure 10c illustrates a sche- Fermi pockets yields a difference in the current from each valley,
matic of a van der Waals heterostructure p–n diode consisting of depending on the electric-field directions. As a result, these
monolayer MoS2 (n-type) and WSe2 (p-type).[196] A ferromagnetic spin-polarized currents could contribute to circular polarization
electrode is contacted on WSe2 to inject spin-polarized holes. in a p–n diode configuration. Figure 11b,c presents the theo-
Figure 10d shows the polarization-resolved EL spectra for oppo- retical predictions of various circularly polarized EL patterns,
site applied magnetic fields, and the relationship between σ+ and depending on the orientation of the p–n junction. When the p–n
σ− is tuned by injected spin alignments. Moreover, the degree of junction is formed along the armchair axes of TMDCs, the gen-
circularly polarized EL can be controlled by the magnetization of erated valley (spin-polarized) currents are in the same direction
the injected electrode. These results offer a beneficial approach as the applied electric field, resulting in the injection of polar-
for the electrical control and generation of valley polarized light ized electrons and holes to gain overall EL polarization at the
emission by spin injection, opening the door to the manipula- junction part (Figure 11b). In principle, changing the direction
tion of valley degrees of freedom as an information carrier for of bias also reverses the helicity of EL polarization (Figure 11b).
opto-valleytronic device applications.[199–202] In contrast, when the p–n junction is oriented in a zigzag direc-
Although the generation of circularly polarized EL using fer- tion, as shown in Figure 11c, the valley currents are perpendic-
romagnetic materials is an efficient method, the use of such ular to the charge currents; thus, the polarized carriers are accu-
substrates/electrodes and the need for an external magnetic mulated on the opposite two sides, causing spatial contrast of EL
field strictly hamper its practical utility in terms of device inte- polarization and not affecting the direction of bias (Figure 11c).
gration, operation ability/condition, and electrical controllability. In addition to this unique origin governed by nonlinear spin and
Therefore, the integrity of electrical switchable valley light-emit- valley currents, the nature of anisotropic trigonal warping pro-
ting devices is suitable for applications. In this regard, another vides an alternative scenario to control EL polarization, derived
Figure 11. Electrical control of circularly polarized EL in valley LEDs. a) Schematic depiction of the carrier distributions of a spin-up valley (red) and a
spin-down valley (blue). The Fermi pocket anisotropy creates a difference between each valley-contributed current in the presence of an electric field,
resulting in a valley (spin-polarized) current. The changing direction of the electric field causes inversed current contributions in each valley, as indicated
by the red and blue arrows. b) When the p–n junction is formed along the armchair direction, the EL shows overall polarization. Green and yellow
areas denote p-doped and n-doped regions, respectively. Red and blue arrows indicate σ+ and σ− polarization, respectively. c) Spatial patterns appear
in EL polarization when the p–n junction is formed with a zigzag orientation. Reproduced with permission.[204] Copyright 2014, American Physical
Society. d) Schematic illustrations of the electron and hole distributions shifted by an applied electric field. Orange and green areas indicate the overlap
between K and −K (K′) valleys. e) The difference in valley overlap induces the unbalanced recombination in each valley, resulting in circularly polarized EL.
Reproduced with permission.[205] Copyright 2014, Nature Publishing Group. f) Polarized-resolved EL spectra from an ionic-liquid-gated WSe2 light-
emitting transistor under different current directions. The inset shows the schematics of the contributions to EL from two valleys, representing that the
helicity of EL depends on current directions. Reproduced with permission.[138] Copyright 2014, American Association for the Advancement of Science.
from semiclassical transport theory.[138] If the in-plane electric On the basis of these theoretical predictions of the electrical
field is applied to materials, the overlap of charge distributions control of circularly polarized EL, the experimental evidence of
between K and −K valleys is unbalanced, with the hole distri- valley-dependent LED functionality has in fact been achieved
butions shifting in parallel directions to bias and the electrons in WS2, WSe2, and MoSe2.[138–140,203] Figure 11f exhibits polar-
shifting in the opposite direction (Figure 11d). This variation of ization-resolved EL spectra obtained in an ionic-liquid-gated
valley overlap in the presence of a lateral electric field provides WSe2 ambipolar light-emitting transistor.[138] The handedness
an intensity difference originating from recombination at each of the circular polarized emission is reversible by reversing
valley, leading to EL polarization (Figure 11e).[205] It is worth the direction of the applied electric field (Figure 11f). The
noting that this mechanism is sensitive to the relative angle experimental demonstrations of electrically switchable valley
between the crystal orientation and the bias direction. light-emitting devices significantly elevate a new paradigm
of opto-valleytronics that links electricity to valley degree of ability to manipulate individual monolayers with atomic preci-
freedom for next-generation quantum information processing sion, so it has introduced a new platform to construct hetero-
and computing. Finally, several desired developments have been structures for engineering the desired electronic structures.
remarked on as further expanding the applicability of TMDCs Owing to the variety of TMDC family, the fabrication of van der
for practical applications. Although current progress has ena- Waals heterostructures has revealed distinctive optical proper-
bled the control of circularly polarized light emission, one ties, such as the formation of interlayer excitons, and the het-
crucial disadvantage is its operational temperature. Since the erostacked devices can achieve high-efficiency tunneling LEDs,
valley polarization and valley-dependent transport phenomena leading to valuable methods for enhancing the brightness of
are related to spins located in K and −K valleys, they are inevi- TMDC LEDs. The lateral heterojunction films are also a feasible
tably affected by temperature-induced intervalley scattering. way to tune band structures, and the advanced CVD methods for
Therefore, the reported large valley polarizations for both PL synthesizing laterally stitched different TMDCs with atomically
and EL have mostly been observed at low temperatures of less sharp interfaces offer promising approaches for the patterning
than 80 K, except in some specific cases.[79–82,138–140,195,196,203] and integration of LEDs on the wafer scale. Finally, the topo-
To address industrial device applications, valley light-emitting logical nature of TMDCs can be used to explore a new class of
(and photodetecting) devices that can stably operate at room electronics field called valleytronics, in which the valley degree
temperature are greatly needed. Very interestingly, a recent of freedom that is an internal valley index in the momentum
report proposed a new approach to controlling valley magneti- space can be controlled and used as an information carrier. The
zation using external strain.[206] By applying uniaxial strain to excitons optically excited by circularly polarized light store its
break the threefold rotational symmetry of monolayer TMDCs, valley-spin information; hence, valley-dependent light emitters
the piezoelectric field can be interacted with charge currents to (and absorbers) can be realized. Although the electrical control
induce valley magnetization, even at room temperature. This of circularly polarized light emission in TMDC LEDs has been
result suggests that the combination of strained TMDCs and theoretically and experimentally reported, there are still several
p–n diode fabrications, such as in strained monolayer LEDs, ongoing challenges to practical device application. For example,
would be a possible way to realize room temperature valley the fully comprehensive understanding of mechanisms for elec-
polarized light-emitting devices, which would be a significant trically controlling circularly polarized light emission should be
breakthrough for future practical opto-valleytronic devices. Fur- addressed, e.g., investigating spatial EL polarization mapping,
thermore, the reproducibility of the fabrication of valley LEDs leading to reproducible valley LED fabrication and operations.
has been elusive, perhaps due to incomplete understanding One of the most significant future subjects is the development
of the detail mechanisms of polarized EL generation. Hence, of a method to control EL polarization at room temperature
more comprehensive experimental studies regarding spatial because mostly valley-dependent phenomena were observed
polarized EL mapping and spectroscopy and detailed electric only at low temperature, and they strictly limit practical utility.
field dependence and its angle-resolved spectroscopy should Therefore, achieving room temperature valley LEDs will further
be performed to identify the mechanisms of recombination accelerate the use of valley degrees of freedom in device func-
phenomena governed by valley degrees of freedom. tionalities toward the development of novel information pro-
cessing and computing methods.
6. Conclusion
Acknowledgements
In this progress report, we have focused on recent advances J.P. was supported by JSPS-KAKENHI under Grant No. JP17H06736.
in the fundamental properties, device fabrication, and optical T.T. was supported by JSPS-KAKENHI under Grant Nos. JP17H01069,
functionalities of light-emitting devices based on atomically JP16K13618, JP15K21721, JP26102012, and JP25000003. This work was
thin TMDCs. The unique physical, mechanical, and quantum supported by JST CREST Grant No. JPMJCR1715, Japan. The authors are
features derived from confined carriers in truly two dimensions grateful to Prof. L.-J. Li and Dr. M-Y. Li from King Abdullah University of
Science and Technology (KAUST) and Academia Sinica, Prof. K. Matsuda
and the explicit crystal symmetry of monolayer TMDCs offer
and Prof. Y. Miyauchi from Kyoto University, and Dr. T. Sakanoue
promising candidates for use in novel functional light-emitting from Nagoya University for their plentiful discussions and fruitful
device applications. First, the tunable electronic structure due to collaboration.
geometric confinement has enabled the stable existence of qua-
siparticle states, such as excitons and trions, with wide wave-
length ranges from the visible to near-infrared. In addition, Conflict of Interest
the mechanical stability and flexibility have allowed TMDCs The authors declare no conflict of interest.
to be easily assembled on arbitrary substrates and/or artificial
structures. These virtues have not only inspired the realization
of diverse light-emitting device applications, but they have also Keywords
endowed future possibilities for realizing large-area flexible
heterostructure, light-emitting device, optoelectronics, transition metal
and stretchable LEDs and low threshold laser diodes. Notably,
dichalcogenides, valleytronics
TMDC light sources integrated with silicon waveguides have
recently been demonstrated, so this result provides opportuni- Received: December 31, 2017
ties for building complementary integrated optical circuits.[207] Revised: February 21, 2018
Second, the naturally passivated body of TMDCs provides the Published online: June 13, 2018
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Monolayer Transition Metal Dichalcogenides as

layers are sandwiched at nanometer-scale

from visible to near-infrared wavelengths.[24–26] Analogous

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