Versatile Crystal Structures and (Opto) Electronic Applications of The 2D Metal Mono-, Di-, and Tri-Chalcogenide Nanosheets

REVIEW
Metal Chalcogenides www.afm-journal.de
Versatile Crystal Structures and (Opto)electronic Applications

of the 2D Metal Mono-, Di-, and Tri-Chalcogenide Nanosheets
Yu Cui, Ziqi Zhou, Tao Li, Kaiyou Wang, Jingbo Li, and Zhongming Wei*
This paper is dedicated to Prof. Jian-Bai Xia for his 80th birthday
structure limits its applications, especially

Emerging 2D metal chalcogenides present excellent performance for for switching devices. Beyond graphene,
electronic and optoelectronic applications. In contrast to graphene and other semiconducting MoS2 with a natural
2D materials, 2D metal chalcogenides possess intrinsic bandgaps, versatile bandgap has been discovered to be appro-
band structures, and superior atmospheric stability. The many categories priate for electronic and optoelectronic
applications.[3] A family of 2D materials
of 2D metal chalcogenides ensure that they can be applied to various
represented by MoS2, metal chalcogenides,
practical scenarios. 2D metal monochalcogenides, dichalcogenides, and possessing the elementary composition of
trichalcogenides are the three main categories of these materials. They have metal and chalcogen has received wide-
distinct crystal structures resulting in different characteristics. Some basic spread attention from researchers.
device characteristics, such as the charge carrier characteristics, scattering MoS2 has sandwich-structure crystal
mechanisms, interfacial contacts, and band alignments of heterojunctions, stacking, with a molybdenum atom layer
sandwiched between two sulfur atom
are vital factors for practical device applications that ensure that the desired layers. Transition metal dichalcogenides
properties can be achieved. Various electronic, optoelectronic, and photonic present a similar crystal structure. They
applications based on 2D metal chalcogenides have been extensively exhibit intensely thickness-dependent
investigated. 2D metal chalcogenides are considered as competitive characteristics. MoS2, WS2, MoSe2, and
candidates for future electronic and optoelectronic applications. WSe2 exhibit a transition from indirect
to direct band structures with decreasing
thickness to the isolated monolayer.
1. Introduction Monolayered and bilayered PtSe2 is semiconducting, while
thick PtSe2 is metallic.[4] Numerous studies on electronic and
With the tendency of miniaturization, integration, and low- optoelectronic applications have focused on transition metal
energy consumption for electronic and optoelectronic applica- dichalcogenides. Recently, group IV dichalcogenides have also
tions, the progress in further improving the performance of attracted extensive attention due to their outstanding perfor-
devices based on conventional materials will be hampered. The mance and environmentally friendly characteristics.[5] GeSe2
2D materials with van der Waals layered structures that have presents a unique anisotropy, in contrast to the usual isotropy
emerged in the recent decades have been considered promising of transition metal dichalcogenides. In addition to 2D metal
candidates for future electronic and optoelectronic applications.[1] dichalcogenides, 2D metal mono- and tri-chalcogenides are
Graphene with the hexagonal structure of carbon atoms was two important types of material of this large family. They have
first investigated for its excellent electrical properties. Bilayered entirely different crystal structures than dichalcogenides and
graphene with a specific twist angle even presents superconduc- have special characteristics that can effectively expand electronic
tivity.[2] However, the semimetal characteristic of the gapless band and optoelectronic applications. GeSe has been proven to pos-
sess intense anisotropic light absorption, and the utilization
of GeSe in near-infrared polarization-sensitive photodetectors
Y. Cui, Z. Zhou, Prof. K. Wang, Prof. J. Li, Prof. Z. Wei
State Key Laboratory of Superlattices and Microstructures is promising.[6] InSe exhibits high electron mobility, which is
Institute of Semiconductors vitally important for practical device applications.[7] 2D metal
Chinese Academy of Sciences & Center of Materials Science trichalcogenides, such as TiS3, ZrS3, and In2Se3, have also been
and Optoelectronics Engineering investigated for use in electronic devices and photodetectors.[8]
University of Chinese Academy of Sciences
Beijing 100083, China
2D metal mono-, di-, and tri-chalcogenides with chalcogens
E-mail: zmwei@semi.ac.cn (S, Se, and Te) and metal elements from groups IVB-VIII, IIIA,
Prof. T. Li and IVA compose a promising 2D material system for future
Shanghai Key Laboratory of Electrical Insulation and Thermal Aging electronic and optoelectronic applications. The prime metal ele-
School of Chemistry and Chemical Engineering ments and classification for these three types of 2D metal chal-
Shanghai Jiao Tong University cogenides are marked in the presented periodic table (Figure 1).
Shanghai 200240, China
Compared to other 2D materials, 2D metal chalcogenides
The ORCID identification number(s) for the author(s) of this article
can be found under https://doi.org/10.1002/adfm.201900040.
have excellent stability, a relatively simple crystal structure,
and abundant types. Most 2D metal chalcogenides exhibit
DOI: 10.1002/adfm.201900040 stable structures under an atmospheric environment, which
Adv. Funct. Mater. 2019, 1900040 1900040 (1 of 33) © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
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is advantageous for reducing the destruction from the sur-

rounding environment during processing and storage and Yu Cui is currently a Ph.D.
can effectively prolong the practical lifetime of materials. candidate at the Institute of
2D metal chalcogenides have been extensively investigated for Semiconductors, Chinese
various applications, including electronics, optoelectronics, Academy of Sciences, under
valleytronics, spintronics, superconductivity, thermoelectricity, the supervision of Prof.
and electrochemistry.[1b,5,9] 2D metal chalcogenides possess Zhongming Wei. His current
rich band structures with various bandgaps, which are a piv- research interests include
otal issue of modern electronic and optoelectronic applications. the fabrication and physical
Some 2D metal chalcogenides with special quantum character- properties of 2D materials.
istics provide a versatile platform for investigating novel elec-
tronic and optoelectronic applications, such as the valleytronics
applications of group VIB dichalcogenides.[10] In this review,
we provide a comprehensive introduction to electronic, opto-
electronic, and photonic applications for all 2D metal chalco- Zhongming Wei received his
genides, including 2D metal mono-, di-, and tri-chalcogenides. B.S. from Wuhan University
Their different characteristics arising from the diverse crystal (China) in 2005, and
structures determine the potential applications in different Ph.D. from the Institute of
fields. Some basic device characteristics, such as the charge car- Chemistry, Chinese Academy
rier characteristics, scattering mechanisms, interfacial contacts, of Sciences in 2010 under the
and band alignments of heterojunctions, are vital factors for supervision of Prof. Daoben
optimizing the performance in practical applications. A bottom- Zhu and Prof. Wei Xu. From
to-top overview based on recent studies of 2D metal chalcoge- August 2010 to January 2015,
nides, from the crystal structures and device characteristics to he worked as a postdoctoral
applications, is provided in the following sections. fellow and then Assistant
Professor in Prof. Thomas
Bjørnholm’s group at University of Copenhagen, Denmark.
2. Crystal Structures of 2D Metal Chalcogenides Currently, he is working as a professor at the Institute
of Semiconductors, Chinese Academy of Sciences. His
The crystal structures of 2D metal chalcogenides, similar research interests include low-dimensional semiconduc-
to other 2D layered materials, present covalent bonding of tors and their (opto)electronic devices.
atoms inside the layer and van der Waals forces between
layers. Most 2D metal chalcogenides with different chemical
compositions can be divided into mono-, di-, and tri-chalcoge- stacked multilayers of 2D metal chalcogenides. The monolayers
nides. According to the different stoichiometric proportions, of hexagonal boron nitride and elemental 2D materials (such
they can be expressed as the chemical formulas MX, MX2, and as graphene and black phosphorus) are usually composed of a
MX3 (or M2X3), where M represents the metal element and X layer of atoms. However, 2D metal chalcogenides possess com-
represents the chalcogen, including S, Se, and Te. Different plex multilayered structures. The distinct structures provide
2D metal chalcogenides possessing the same stoichiometric diversity of the crystal symmetry, which is a crucial factor in
proportion usually present similar crystal structures. Figure 2 the physical characteristics of 2D systems and can influence
exhibits representative crystal structures of monolayers and the properties of 2D materials. Various crystal structures endow
Figure 1. Periodic table with symbols indicating 2D metal monochalcogenides, dichalcogenides, and trichalcogenides.
Figure 2. Representative crystal structures of 2D metal monochalcogenides, dichalcogenides, and trichalcogenides.
2D metal chalcogenides with potential for different practical can be controlled by altering the fabrication processes.[11] The
applications. Tables 1–3 introduce the characteristics and appli- crystal phases can also be transformed under different external
cations of 2D metal monochalcogenides, dichalcogenides, and conditions, such as temperature, strain, pressure, and elec-
trichalcogenides. Moreover, numerous 2D metal chalcogenides tronic doping.[12] With the use of phase engineering to control
possess several crystal phases. Multiple thermodynamically the properties of 2D metal dichalcogenides, their application
stable phases can coexist in some 2D metal chalcogenides and can be further broadened.[11]
Table 1. Characteristics and applications of 2D metal monochalcogenides.
Crystal structure Electric conductivity Band gap [eV] Fabrication method Application Ref.
GaS Hexagonal Semiconductor Indirect 2.52 Hydrogen evolution reaction [13b]
GaSe β hexagonal Semiconductor p-type 2.0 Vapor phase mass transport Photodetector, terahertz, optics [17]
ε hexagonal
γ orthorhombic
InSe β rhombohedral Semiconductor n-type (Bulk) Direct 1.25 Chemical vapor deposition, High electron mobility, broadband [7,16]
γ hexagonal (Monolayer) Direct 2.6 mechanical exfoliation photodetector
GaTe Monoclinic Semiconductor p-type Direct 1.7 Mechanical exfoliation High-sensitivity photodetector [15]
GeS Orthorhombic Semiconductor p-type (Monolayer) Indirect 2.34 Vapor deposition High electron mobility [13e,j]
SnS Orthorhombic Semiconductor p-type Indirect 1.1 Physical vapor deposition Near-infrared photodetectors, anisotropy [13d,g]
GeSe Orthorhombic Semiconductor (Bulk) Indirect 1.10 Vapor deposition, MBE, Near-infrared photodetector, anisotropic [6,13c,103a,140]
(Monolayer) Direct 1.87 mechanical exfoliation photoresponse, polarization-sensitive
photodetector
SnSe Orthorhombic Semiconductor p-type (Bulk) Indirect 0.89 Physical vapor deposition Anisotropy, thermoelectricity [13h,140]
(Monolayer) Indirect 1.63
FeSe Tetragonal MBE Superconductivity [14]
Table 2. Characteristics and applications of 2D metal dichalcogenides.
Crystal structure Electric conductivity Band gap[eV] Fabrication method Application Ref.
MoS2 2H hexagonal (2H) Semiconductor (Bulk) Indirect 1.29 Vapor deposition, mechanical Transistor, photodetector, solar cell, [3,26c,41b,127]
1T (1T) Metal (Monolayer) Direct 1.8 exfoliation, etc. photonics, supercapacitor
WS2 2H hexagonal (2H) Semiconductor n-type (Bulk) Indirect 1.3 Vapor deposition, mechanical Field-effect transistor, photodetector, [26d,e,42a,132,176]
1T (1T) Metal (Monolayer) Direct 2.1 exfoliation, et al. photonics, hydrogen evolution reaction
MoSe2 2H hexagonal (2H) Semiconductor ambipolar (Bulk) Indirect 1.4 Vapor deposition, mechanical Transistor, photovoltaic application, [20g,26e,41a,160a]
Adv. Funct. Mater. 2019, 1900040

1T (1T) Metal (Monolayer) Direct 1.58 exfoliation, MBE phototransistor, hydrogen evolution reaction
www.advancedsciencenews.com
WSe2 2H hexagonal (2H) Semiconductor ambipolar (Bulk) Indirect 1.2 Vapor deposition, Field-effect transistor, phototransistor, [26e,31,71b,78b,169b]
1T (1T) Metal (Monolayer) Direct 1.65 mechanical exfoliation, et al. solar cell, light-emitting device
MoTe2 (α) 2H hexagonal (2H) Semiconductor ambipolar (Bulk) Indirect 0.96 Chemical vapor deposition, Field-effect transistor, broadband photodetector, [12a,24c,78c,179a,198c]
(β) 1T′ monoclinic (1T′) Metal (Monolayer) Direct 1.07 mechanical exfoliation, MBE photonics, superconductivity
Td orthorhombic (Td) Metal
WTe2 Td orthorhombic Semimetal Chemical vapor transport, MBE Superconductivity, giant magnetoresistance [23,197]
ZrS2 1T rhombohedral Semiconductor n-type (Bulk) Indirect 1.7 Chemical vapor deposition High-performance photoconductivity [20i],j
(Monolayer) Indirect 1.7–1.93
ZrSe2 1T rhombohedral Semiconductor Indirect 0.57 High mobility [30]
HfS2 1T rhombohedral Semiconductor Indirect 2.0 Mechanical exfoliation Transistor, ultrasensitive phototransistor [137]
HfSe2 1T rhombohedral Semiconductor Indirect 0.45 High mobility [30]
VSe2 1T rhombohedral Metal MBE Room-temperature ferromagnetism [208]
NbS2 2H hexagonal Metal superconductivity [26d,123]
NbSe2 2H hexagonal Metal Chemical vapor transport Superconductivity, charge density wave [25b,198a]
1900040 (4 of 33)
4H hexagonal
TaS2 1T rhombohedral Metal Chemical vapor deposition Ultrabroadband photosensitivity, [25c,27]
2H hexagonal superconductivity, charge density wave
6R
ReS2 Distorted Semiconductor n-type (Bulk) Direct 1.50 Mechanical exfoliation, chemical Field-effect transistor, photodetector, [24b,144c]
1T triclinic (Monolayer) Direct 1.58 vapor deposition anisotropy
ReSe2 Distorted 1T triclinic Semiconductor ambipolar (Bulk) Direct 1.27 Mechanical exfoliation, chemical Optoelectronic application, [20b,24a,78a,144b]
(Monolayer) Indirect 1.24 vapor deposition polarization-sensitive photodetector,
anisotropy
NiTe2 1T rhombohedral Metal Chemical vapor deposition [20h]
PtSe2 1T rhombohedral (Monolayer, bilayer) Semiconductor (Monolayer) 1.20 Chemical vapor transport, chemical vapor Mid-infrared photodetector [4,32,141]
(≥Trilayer) Semimetal (Bilayer) 0.21 deposition, selenization of Pt films
PdTe2 1T rhombohedral Metal Superconductivity [198b]
SnS2 4H hexagonal Semiconductor n-type (Bulk) Indirect 2.308 Mechanical exfoliation, Field-effect transistor, photovoltaics, [25a,28,29b,135a]
(Monolayer) Indirect 2.033 chemical vapor deposition high-performance and fast photodetector
SnSe2 1T rhombohedral Semiconductor n-type (Bulk) Indirect 1.0 Mechanical exfoliation, Field-effect transistor, high-performance [20a,136,180a]
(Few-layer) Indirect 1.73 chemical vapor deposition and fast photodetector, photonic application
GeSe2 Monoclinic Semiconductor p-type (Flake) 2.74 Mechanical exfoliation, Polarization-sensitive photodetector [20k,145]
chemical vapor deposition
© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

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Table 3. Characteristics and applications of 2D metal trichalcogenides.
Crystal structure Electric conductivity Band gap[eV] Fabrication method Application Ref.
TiS3 Monoclinic Semiconductor n-type Direct 1.13 Mechanical exfoliation Ultrahigh photoresponse, polarization- [8d]
sensitive photodetector, anisotropy
ZrS3 Monoclinic Semiconductor p-type Direct 2.56 Chemical vapor transport Flexible visible-light photodetectors [8b]
HfS3 Monoclinic Semiconductor Chemical vapor transport Transistor, photodetector [35c]
TiSe3 Monoclinic Semiconductor (Bulk) Indirect 0.21 [8c]
ZrSe3 Monoclinic Semiconductor (Bulk) Indirect 0.75 Chemical vapor transport Visible light photodetector [8c,35d]
HfSe3 Monoclinic Semiconductor Chemical vapor transport Visible light photodetector [35d]
TiTe3 Monoclinic Metal [8c]
ZrTe3 Monoclinic Metal Chemical vapor transport Charge density wave [35e]
NbSe3 Monoclinic Metal Chemical vapor transport Charge density wave [36b]
TaS3 Orthorhombic Metal Charge density wave [36c]
In2S3 Tetragonal Semiconductor n-type Direct 2.02 Chemical vapor deposition Broadband photoresponse [37d]
(defective spinel)
In2Se3 α rhombohedral, Semiconductor β: (Bulk) Direct 1.3 Mechanical exfoliation High-gain phototransistor [37b,38]
β rhombohedral (Monolayer) 1.5;
α: direct 1.3
Bi2Te3 Rhombohedral Semiconductor 0.15–0.3 Chemical vapor deposition Topological insulator [37a,c]
Bi2Se3, Sb2Te3 Rhombohedral Topological insulator [37c]
2.1. 2D Metal Monochalcogenides are beneficial to applications in high-frequency devices and

quantum devices. GaSe exhibits a dramatic variation in the
MX mostly corresponds to group IIIA or IVA monochalcoge- photoresponse as its thickness changes, which is attributed
nides,[13] and FeSe[14] is an exception. Monolayer group IIIA to its unique pz-like order of Se atoms.[17] When the thickness
monochalcogenides (e.g., GaS, InS, GaSe, InSe, and GaTe) of GaSe decreases, the coupling of the pz orbit becomes weak,
possess a hexangular crystal structure with four sequential and the large interband transition energy replaces the relatively
atom planes in the order of X-M-M-X. Usually, the X and M small one induced by the pz orbit. Common X-M-M-X mono
atoms in different planes of a monolayer are severally aligned layers of group IIIA monochalcogenides present mirror-plane
along the c-axis. However, GaTe presents a distorted X-M-M-X symmetry. Various stacking configurations of multilayers can
structure in which one-third of the Ga-Ga bonds are no longer break the mirror-plane symmetry to introduce novel charac-
parallel to the c-axis.[15] For multilayers, different stacking teristics. For example, the photoluminescence (PL) spectra of
modes result in various crystal phases. For example, InSe has InSe multilayers, compared to that of the monolayer, have an
two stable crystal phases, the β-phase and γ-phase.[7,16] The additional peak.[7] Black phosphorus with a puckered crystal
c-axis periodic structure of β-InSe consists of three monolayers structure has been shown to have remarkable anisotropy.[1g,18]
with a staggered alignment, and each monolayer possesses Group IVA monochalcogenides with black phosphorus-like
the same atom sequence along the a-axis and b-axis. γ-InSe crystal structures also exhibit outstanding anisotropy.[6,13i]
has a periodic structure of two monolayers along the c-axis in Polarization-sensitive photodetectors with GeSe as the working
which all selenium atoms and indium atoms in the two layers material exhibit a remarkable dichroic ratio of 2.16 under an
are aligned with each other. Multilayer GaSe also possesses 808 nm laser.[6] Moreover, SnS and SnSe have great potential
three types of crystal phases, β-GaSe, ε-GaSe, and γ-GaSe.[17] for thermoelectric applications.[19]
The crystal structures of group IVA monochalcogenides (e.g.,
GeS, SnS, GeSe, and SnSe) are constituted by the puckered
M-X atom permutation. It is analogous to the crystal structure 2.2. 2D Metal Dichalcogenides
of black phosphorus, however, group IVA monochalcogenides
present superior stability compared to black phosphorus. MX2 (e.g., MoS2, WSe2, MoTe2, ReSe2, PtSe2, GeS2, SnS2, and
Semiconducting InSe and GeS have relatively high electron SnSe2) with various elemental compositions has been exten-
mobilities compared to other 2D metal chalcogenides. The sively investigated, and the elements from group IIIB–VIII
mobility of InSe has been experimentally proven to be over and IVA can be used to form 2D metal dichalcogenides.[20]
1000 cm2 V−1 s−1 at room temperature and 10 000 cm2 V−1 s−1 Monolayered MX2 possesses a sandwich crystal structure in
at liquid-helium temperature,[7] and theoretical calculations which one atomic layer of M atoms is located between two
for monolayered GeS has predicted an electron mobility atomic layers of X atoms. The 1H and 1T phases are two types
of 3680 cm2 V−1 s−1.[13j] The remarkable carrier mobilities of common monolayered crystal structures. The 1H phase has
trigonal prism coordination with hexagonal symmetry, and the have special distorted 1T crystal phases, and significant differ-
X atoms in different atomic layers of a 1H phase crystal are ences exist in the different orientations in the layer plane of
equivalent and mirror symmetric. The 1T phase crystal struc- their crystal structures. Hence, ReX2 and W(Mo)Te2 possess
ture has octahedral coordination with tetragonal symmetry, fascinating anisotropy in their electronic and optoelectronic
and the alignment of S atoms breaks the mirror symmetry, characteristics.[34]
in contrast to the 1H phase. For stacked multilayered MX2,
two types of common stacking configurations exist, the 2H
(including 2Ha and 2Hb) and 3R phases. The 2H phase struc- 2.3. 2D Metal Trichalcogenides
ture with hexagonal symmetry exhibits periodic layers of two
nonequivalent monolayers. For the 2Ha phase, M atoms in dif- MX3 and M2X3 are two types of 2D metal trichalcogenides with
ferent monolayers are aligned with each other. The M atoms of different stoichiometric proportions. The metal component of
the 2Hb phase crystal are aligned with the X atoms of another MX3 (e.g., TiS3, ZrSe3, HfSe3, and NbSe3) is usually from group
monolayer. Group VB dichalcogenides usually form the thermo- IVB[8b-d,35] or group VB.[36] MX3 has a quasi-1D crystal structure.
dynamically stable 2Ha phase, and group VIB dichalcogenides The MX3 crystal structures can be described as the stacking of
tend to form the 2Hb phase.[21] Specifically, 2H SnS2 and SnSe2 individual chain units with the same orientation. The parallel
constituted by the stacking of 1T monolayers have rhombo- chains formed by sequential triangular prisms where M and
hedral symmetry.[22] The rhombohedral 3R phase structure X atoms are respectively placed at the corners and centers are
possesses a periodic structure along the c-axis of three non- stacked in a plane to form a quasi-layered structure. The atomic
equivalent monolayers. Through only translation, these non- bonding between chains in the same quasi-layer is fragile.
equivalent monolayers can be moved into mutual positions and Therefore, MX3 tends to form chain-axis oriented nanorib-
replace each other. The 1T′ and Td phases possess a distorted bons. The morphology of fabricated MX3 is usually ribbonlike,
1T phase structure with different stacking configurations. 2D and the chain-axis orientation can be easily found using the
metal chalcogenides with these distorted 1T phases are usually morphology information. Quasi-1D MX3 is appropriate for
unstable. Stable crystals with this crystal structure are relatively anisotropic systems due to its unique chain-like crystal struc-
scarce. WTe2 exhibits the thermodynamically stable Td phase ture. Among the MX3 materials, TiS3 has a direct bandgap of
crystal structure.[23] Under a pressure of 8 GPa, Td phase WTe2 1.13 eV, which makes it suitable for highly efficient anisotropic
will transform into the 1T′ phase.[12d] MoTe2, ReS2 and ReSe2 photodetectors for visible and near-infrared light.[8d]
present the natural 1T′ phase crystal structure.[20b,24] The crystal Monolayered M2X3 (e.g., In2Se3, Sb2Te3, and Bi2Se3) pos-
structure of MoTe2 can be transformed from the 1T′ phase sesses a quintuple layer along the c-axis with sequential atomic
to the Td phase at a temperature of ≈270 K.[12a] In addition to planes in the order X-M-X-M-X.[37] M2X3 possesses various
the crystal phases mentioned above, some uncommon crystal crystal structures with different arrangements of atoms in a
phases have been observed for 2D metal chalcogenides, such as layer and stacking configurations. In2Se3 has been demon-
4H SnS2, 4H NbSe2, and 6R TaS2.[21,22,25] strated to have five types of crystal phases.[38] The α-phase and
The crystal structures have a decisive effect on the proper- β-phase are stable in ambient conditions. Other phases can be
ties of 2D metal chalcogenides. Same-component materials obtained under certain conditions. α-In2Se3 and β-In2Se3 are
with different crystal phases present distinct properties. 2H semiconductors possessing the bandgaps of 1.35 and 1.45 eV,
phase group VIB dichalcogenides are usually semiconducting, respectively, and α-In2Se3 exhibits better conductivity than
however, the corresponding 1T, 1T′, and Td phase crystals are β-In2Se3.[38] Moreover, Bi2Se3, Bi2Te3, and Sb2Te3 are topological
metallic.[12c,26] The 1T phase of freestanding group VIB dichal- insulators.[37c]
cogenides has been theoretically proven to be unstable.[12b]
Group V dichalcogenides with the stable 1T phase crystal struc-
ture, such as NbS2, VSe2, and NbSe2, also present metallic 3. Basic Characteristics of 2D Devices
conductivity.[21,27] Group IVA dichalcogenides, such as, SnS2,
SnSe2, and GeS2, are usually semiconductors.[5,20a,28] Semicon- 3.1. Charge Carrier Characteristics
ducting 2D metal dichalcogenides, such as MoS2 and SnS2,
have been investigated for application in field-effect transis- Intrinsic semiconductors based on 2D metal chalcogenides
tors (FETs) due to their large on/off ratio.[29] Compared to with a perfect lattice structure free from defects and impurities
other dichalcogenides, group IVB dichalcogenides possess are unattainable through state-of-the-art fabrication technolo-
high carrier mobility.[30] Semiconducting group VIB dichalco- gies. The immature fabrication processes inevitably introduce
genides present direct bandgaps for the monolayers instead defects into 2D metal chalcogenide crystals, which can act as
of the indirect bandgaps for the corresponding bulks.[31] Semi- a source of doped carriers. In general, MoS2, exhibiting n-type
conducting PtSe2 (monolayer and bilayer) can be transformed behavior, grown via mechanical exfoliation or chemical vapor
into a metallic material by increasing its thickness.[4,32] With deposition (CVD) has many sulfur vacancies.[39] Sulfur vacan-
their various types of bandgaps, these materials have potential cies as the electron donor dominate the n-type conduction.[40]
in optoelectronic applications. Specifically, by modulating the The conduction type of MoS2 can be transformed into the
components of alloys based on 2D metal dichalcogenides, such p-type when the sulfur vacancies are repaired and molybdenum
as MoxW1−xS2 and SnS2xSe2−2x, a controllable bandgap covering vacancies dominate the doped carriers.[40a] Figure 3a shows
a continuous region of the spectrum can be realized.[33] In con- the defect states introduced into the energy band of MoS2 by
trast to other 2D metal dichalcogenides, ReX2 and W(Mo)Te2 sulfur and molybdenum vacancies, and Figure 3b shows the
Figure 3. a) Additional energy levels induced by three types of typical point defects of MoS2, including the single-face sulfur defect, double-
face sulfur defect, and molybdenum defect. b) Atomic resolution STEM images of the defects listed in (a). a,b) Reproduced with permission.[39]
Copyright 2013, American Chemical Society. c) Conductivity dependence on the temperature for different carrier densities of MoS2. Reproduced with
permission.[42b] Copyright 2013, Springer Nature. d) Temperature dependence of the mobility based on different scattering mechanisms of multilayered
MoS2. Reproduced with permission.[46] Copyright 2012, Springer Nature.
corresponding STEM images of different defects. The experi- transport properties. In contrast to traditional materials, such
mental transition of the conduction type conforms to these as silicon-based semiconductors and gallium nitride, where
defect states. Moreover, the work function difference between the transport properties will sharply decrease with decreasing
contact metals and 2D metal chalcogenides and surface Fermi thickness to several nanometers due to intense scattering from
level pinning play important roles in the carrier transport the rough surface with inevitable dangling bonds,[45] 2D metal
behavior.[41] Different carrier transport behaviors have been chalcogenides are promising for future ultrathin nanodevices
demonstrated in previous reports where different metals were due to the inherent layered structures with clean surfaces. The
used as electrodes for the same material. The metal-insulator atom-thick configuration results in ambient impurities that
transition has been widely observed in 2D metal chalcogenides can obviously impact internal carriers, and numerous defects
and is attributed to the localized trap states.[40b,42] The obvious caused by immature preparation technologies cause some non-
metal-insulator transition of MoS2 is indicated in the tempera- negligible scattering. Optimizing various types of scattering is
ture dependence curves of the conductance at different carrier an important means of improving the performance of devices.
densities (Figure 3c). The temperature dependence relation of Several primary types of scattering mechanisms occur in 2D
the conductance for a low carrier density corresponds to semimetal chalcogenides, including lattice phonon scattering,
conducting behavior, and the reverse relation for a high carrier interfacial Coulomb impurity scattering, defect scattering, and
density corresponds to metallic behavior. The point defects remote interfacial phonon scattering. The final transport prop-
induce localized in-gap defect states or band tails in the band erties of 2D metal chalcogenides are ultimately determined by
structures around the defects.[39,43] When the carrier density all these scattering mechanisms, which can be expressed as
is low, the carrier transport mode is based on the hopping Mathiessen’s rule, μ−1 = μP−1 + μCI−1 + μDEF−1 + μRIP−1. Here,
between these localized defect states.[44] After the carrier den- μ represents the actual charge carrier mobility, and μP, μCI,
sity is increased, the band transport dominates the transport μDEF, and μRIP represent charge carrier mobilities under lattice
behavior. This transformation between two carrier transport phonon scattering, interfacial Coulomb impurity scattering,
mechanisms can be considered the source of the metal-insu- defect scattering and remote interfacial phonon scattering,
lator transition. respectively. Figure 3d shows the mobility variations with tem-
perature under the action of the respective as well as compre-
hensive scattering mechanisms based on typical MoS2 FETs.[46]
3.2. Scattering Mechanisms The relation between the mobility and temperature can be used
to predict the existing scattering mechanisms in devices.[47]
Scattering, which is a fundamental physical phenomenon Lattice phonon scattering, deriving from the lattice deforma-
for most practical applications, greatly determines the carrier tion potentials (acoustic phonons and optical phonons) and the
Figure 4. a) Calculated photon-limited carrier mobility variation with temperature. b) Calculated carrier mobilities with the usage of different dielectrics.
a,b) Reproduced with permission.[47] Copyright 2017, Wiley-VCH. c) Schematic diagram of interfacial impurities for a normal back-gate FET based on
2D materials. d) Thickness-dependent carrier distributions of 2D materials. c,d) Reproduced with permission.[50] Copyright 2013, American Chemical
Society. e) Histograms of different defects in MoS2 prepared by different growth methods. Reproduced with permission.[57a] Copyright 2015, Springer
Nature.
selectable Fröhlich interaction for polar 2D materials with the carriers will be restricted to the single or few atomic layers near
polarization electric field coupled to carriers, is the intrinsic the dielectric due to the gate voltage (Figure 4d).[46,50] Hence,
scattering mechanism, which greatly determines the ultimate internal carriers are very close to the interfacial Coulomb impu-
carrier transport properties of perfect 2D metal chalcogenide rities. The relation of the impurity scattering rate (PCI) and the
crystals. The intrinsic mobilities of single-layer MoS2 have been distance between carriers and interfacial impurities (d) can be
theoretically calculated, confined by only lattice phonon scat- described as PCI ∝ d−2.[50] When electrons move systematically
tering.[48] At high temperature (T > 100 K), the mobility is gov- under a driving voltage, they will be scattered by the random
erned by optical phonon scattering. The mobility is dependent static electric fields. Accordingly, the existence of Coulomb
on the temperature, following the relation μ ∝ T−γ, where γ is 1.69 impurities will significantly deteriorate the carrier transport.
at room temperature. The carrier density slightly impacts the Alleviating this type of scattering to improve the properties of
phonon-limited mobility. The interaction between electrons and 2D devices is an important research subject. Numerous efforts
acoustic phonons, instead of optical phonons, is considered the have been made, such as designing devices with suspended
primary scattering mechanism at low temperature (T < 100 K). channels, selecting high-k insulators as the dielectric,[51] using
Figure 4a exhibits the theoretical curves of the phonon-limited a high carrier density to screen the impurity scattering,[50]
carrier mobility variation with temperature and shows the two annealing to reduce contaminants generated in the preparation
regimes dominated by acoustic phonons and optical phonons. processes,[52] and constructing a clean environment to prevent
Theoretical calculations have proven that the application of adsorbates.[16] The details will be introduced in the following
strain can obviously improve the acoustic phonon-limited application sections.
mobility, providing a feasible scheme to modulate the intrinsic Another vital extrinsic scattering mechanism is remote
transport properties of 2D metal chalcogenides.[49] interfacial phonon (also called surface optical phonon) scat-
Interfacial Coulomb impurities, such as the dangling bonds tering, resulting from the remote interactions between the
of dielectric surfaces, processing contaminants, and atmos- charge carriers and polar optical phonons of dielectrics. The
pheric adsorbates, are randomly distributed on the surfaces of oscillating polarizable bonds in dielectrics, such as the metal-
2D metal chalcogenides, as shown in Figure 4c. These impuri- oxide bonds of HfO2, are the source of polar optical phonon
ties can produce random static electric fields at the interface. 2D modes and induce time-dependent electric fields at the dielec-
metal chalcogenides possess atomic-scale ultrathin structures, tric surface. This remote interaction can also limit the carrier
and even for few-layered 2D metal chalcogenides, most of the mobility.[53] The strength of the coupling of interfacial phonons
with carriers and their characteristic frequency are two deci- chalcogenides have been investigated.[61] Fang et al. achieved low
sive parameters of the interfacial phonon scattering rate, and contact resistance by doping the vicinities of electrodes through
low-frequency phonons usually have a more significant influ- the chemical adsorption of NO2 on a WSe2 surface.[61c] An
ence on carriers than other phonons.[47,54] The selection of ionic liquid is an alternative material for chemically doping 2D
appropriate insulators as the dielectric can effectively reduce the metal chalcogenides to improve the contact properties.[61b] No
impact of remote interfacial phonon scattering on the carrier feasible scheme exists for substitutional doping in designated
transport property.[55] The theoretically calculated mobilities of regions due to this doping usually being implemented together
MoS2 on different dielectrics are exhibited in Figure 4b. Espe- with the crystal growth process. Chuang et al. presented an
cially in high electric fields, serious consideration of remote advanced strategy for realizing low-resistance ohmic contacts
interfacial phonon scattering is necessary.[55,56] When a high with substitutionally doped 2D metal chalcogenides.[61d] After a
field is applied through the gate voltage in a device with the piece of highly p-substitutionally doped WSe2 (Nb0.005W0.995Se2)
metal-oxide-semiconductor structure, carriers close to the gate is inserted between a metal electrode and pristine WSe2
dielectric are highly localized, which enhances the coupling of (Figure 5a), this contact exhibits a low contact resistance of
carriers with interfacial optical phonons. The remote interfacial 300 Ω µm, which is significantly lower than that of WSe2-gra-
phonon scattering thus becomes more crucial to the carrier phene contacts (≈2000 Ω µm). Phase engineering can also be
transport than the interfacial Coulomb impurity scattering. utilized to improve the performance of contacts.[26a,b] Kappera
Various types of defects exist in 2D metal chalcogenides, et al. have indicated that in contrast to only 2H phase (semi-
such as vacancies, dislocations and grain boundaries, and these conducting) MoS2, the device with 1T phase (metallic) MoS2
defects can be effectively observed via aberration-corrected scan- in contact with metal electrodes possesses the superior con-
ning transmission electron microscopy.[39,57] The amounts and tact resistance (200–300 Ω µm) with an approximately fivefold
categories of defects existing in 2D metal chalcogenides have decrease.[26b] This strategy has also been utilized for MoTe2,
been shown to be related to the fabrication methods.[57a] For whose phase can be controllably transformed from the semicon-
example, the statistical data of several vacancies in MoS2 fabri- ducting phase to the metallic phase under laser illumination.[26a]
cated through three different methods (mechanical exfoliation, The work functions of electrode metals can determine
physical vapor deposition and CVD) are shown in Figure 4e. the Schottky barrier height of metal-semiconductor con-
The industrial silicon crystal possesses an ultralow defect den- tacts, which influences the injection of charge carriers. The
sity, thus satisfying the necessary properties. However, the use of the appropriate metal as the electrode is an effective
defect density of state-of-the-art 2D metal chalcogenides is means to improve contacts.[62] Das et al. investigated different
very high, reaching orders of magnitude of ≈1012–1013 cm−2, metal electrodes, such as scandium, titanium, nickel, and
thus making the consideration of the impact of defects neces- platinum, and the scandium electrodes demonstrated the
sary. Wu et al. found that the increasing defect density of WSe2 lowest Schottky barrier height (30 meV) compared with the
revealed by low-temperature PL spectra leads to degradation of other electrodes (Figure 5b).[62b] However, the Schottky barrier
the electrical properties.[58] Another work in which an obvious height of the 2D metal chalcogenide-metal contact does not
improvement of the mobility was realized by repairing sulfur strictly conform to the Schottky-Mott model due to the Fermi
vacancies in MoS2 also powerfully supports this point.[40b] Other level pinning induced by imperfections of the interface.[63] In
scattering mechanisms also impact the application of 2D metal addition, due to the low-density interfacial states, the Fermi
chalcogenides. Brief introductions to several primary scattering level has been demonstrated to be partially pinned.[64] Con-
mechanisms in 2D metal chalcogenides were presented above, ventional metal evaporation can introduce numerous imper-
and some literatures focusing on scattering can provide exhaus- fections into the contact regions of 2D metal chalcogenides
tive content.[47,59] (Figure 5c). A perfect contact interface was achieved via a well-
designed electrode integration process based on transfer tech-
nology (Figure 5d).[41b] The Schottky contact free from Fermi
3.3. Interfacial Contacts level pinning has been proven to conform to the Schottky-
Mott model nearly ideally, and both electrons and holes can be
Contacts are a pivotal factor in regulating the performance of injected by assembling metal electrodes with different work
2D metal chalcogenides.[1e,60] For conventional semiconductors, functions. The use of a metallic 2D material as the electrode
the interfacial contact between heterogeneous constituents is also an effective approach to weaken the Fermi level pin-
with defective lattices can introduce additional charge traps ning.[65] Figure 5e exhibits the work functions of different
and carrier scattering. Usually, a buffer layer is used to release metals corresponding to the bandgaps of semiconducting
strains between lattice-mismatched constituents. 2D metal 2D metal chalcogenides. Graphene has been comprehensively
chalcogenides are free from lattice-mismatch-induced damage considered as a superior electrode material due to its excel-
to the interfacial contacts due to their van der Waals contact lent electrical properties.[13a,f,66] Doped graphene and glassy
without dangling bonds. However, this weak contact leads to a graphene hold promise for ohmic contact.[65a,66c] The h-BN
relatively high contact resistance. intercalation between the 2D metal chalcogenide and metal as
Heavy doping to realize advantageous ohmic contacts is used the tunneling barrier can also be used to optimize the con-
to optimize contacts. Rough doping of conventional semicon- tact to extract the intrinsic characteristics.[67] A layer of thiol
ductors, such as ion implantation doping, is detrimental to molecules inserted in the contact region can contribute to
2D metal chalcogenides due to their few-atomic-layer thick- an additional tunneling regime, which improves the contact
ness. Some special doping technologies aimed at 2D metal property.[68]
Figure 5. a) Diagrammatic device drawing of an FET with a doped transition layer between WSe2 and the electrodes. Reproduced with permission.[61d]
Copyright 2016, American Chemical Society. b) Experimental metal Fermi levels of different metals in contact with MoS2, which are determined by
both the work functions and interfacial environments. Reproduced with permission.[62b] Copyright 2013, American Chemical Society. c,d) Two cross-
sectional TEM images of the interfaces between MoS2 and Au electrodes fabricated using conventional evaporation technology and the modified
transfer method, respectively. c–d) Reproduced with permission.[41b] Copyright 2018, Springer Nature. e) Conduction band edges and valence band
edges of various semiconducting 2D metal chalcogenides and corresponding work functions of different metals and metallic 2D metal chalcogenides.
Reproduced with permission.[65a] Copyright 2016, American Association for the Advancement of Science. f) Schematic diagrams of type-I, II, and III
band alignment heterojunctions.
3.4. Band Alignments of Heterojunctions electrons from one side to the other side.[72] This alignment has
a stronger ability to separate electrons and holes than type-II
Heterojunctions based on 2D metal chalcogenides can be easily band alignment. The effective separation of electrons and holes
constructed and present superior electric and photoelectric is advantageous to reducing their interactive scattering.[29a]
properties compared with single-component 2D metal chalco- Moreover, the interfacial Coulomb scattering can also be weak-
genides. 2D heterojunctions can be classified into three typical ened due to the enhanced screening effect of the increased
band alignments (Figure 5f), i.e., type I with a straddling gap, carrier density in heterojunctions.[73] In addition, p–n hetero-
type II with a staggered gap, and type III with a broken gap. junctions usually present type-II or type-III band alignment
Type-I band alignment results in both electrons and holes accu- due to the special position of their Fermi levels in the bandgap.
mulating on the same side, with a relatively narrow bandgap.[69] The intrinsic band alignment of heterojunctions can be trans-
This characteristic can be used to build quantum wells and formed by applying an electric field or strain.[74]
applied in light-emitting devices and semiconducting lasers.
Enhanced PL of MoTe2 has been observed in the MoTe2/WSe2
heterojunction with type-I band alignment due to the con- 4. Versatile Device Applications
tribution of extraneous carriers from WSe2.[70] Type-II-band-
alignment heterojunctions of 2D metal chalcogenides are the 4.1. Electronic Devices
most widely investigated. The separation of electrons and holes
into different layers is beneficial and holds promise for various Electronic devices using the charge of electrons to process or
applications, such as rectifiers, photodetectors, solar cells and store information are a vitally important part of modern infor-
light-emitting diodes.[71] Type-III band alignment is particu- mation technology. They also serve as the basis for other appli-
larly appropriate for tunneling applications due to the overlap cations. The strategy of continuous miniaturization of devices
of the conduction band and the valence band, which belong has been developed in recent decades to enhance the proper-
to two components, and to the feasible tunneling transport of ties of traditional semiconductors, such as silica-based devices.
However, this strategy will be terminated when the size of high on/off ratio.[51b] In contrast with the relatively low mobili-
devices approaches the atomic dimension. 2D materials are ties (approximately a few hundred cm2 V−1 s−1) of usual 2D
considered promising candidates for future electronics devices, metal chalcogenides, InSe, a group III metal monochalcoge-
and their various band structures can be utilized in different nide, exhibits an ultrahigh mobility exceeding 1000 cm2 V−1 s−1
applications.[75] In this section, different types of basic elec- at room temperature, which is comparable to those of silicon
tronic devices and applications for 2D metal chalcogenides, thin films and black phosphorus.[7] Furthermore, InSe is more
such as FETs, p–n junctions, tunneling devices, and Schottky stable than black phosphorus. Some 2D metal chalcogenides
junctions, will be discussed. with anisotropic crystal structures, such as ReS2 and ReSe2,
present anisotropic electronic properties.[83]
The selection of the appropriate 2D metal chalcogenides as
4.1.1. Field-Effect Transistors the channel materials of FETs can satisfy the basic require-
ments of current switching. Designing FETs with high carrier
FETs, possessing the advantages of a simple structure and mobility is also necessary for practical electronic applications.
low power consumption, are basic cells of modern integrated Carrier mobilities of some 2D metal chalcogenides are exhib-
circuits. The scale of FETs has been continuously shrunk to ited in Table 4. The carrier mobility of 2D metal chalcogenides
achieve miniaturization and improved performance.[76] How- is usually limited by the electrode contact or various scattering
ever, traditional silica-based materials as channels are restricted mechanisms, such as internal defect scattering, external Cou-
by short channel effects when the feature size approaches lomb impurity scattering and remote interfacial phonon scat-
several nanometers.[77] 2D materials are promising candidates tering from the dielectric.[55,58,59c] For example, the theoretically
due to their unique atomic structures, which are beneficial for calculated electron mobility under the phonon limit for mono
relieving the limitation of short channel effects and efficiently layer MoS2 is reported to be ≈410 cm2 V−1 s−1.[48a] However,
controlling channel electrons. Moreover, the super clean sur- experimental FETs based on monolayered or even multilayered
face without dangling bonds of 2D materials can reduce the MoS2 usually cannot reach this high mobility.[41b,42b,62b,73] Many
carrier scattering from surface defects for atom-thick electronic attempts have been made to reach their intrinsic mobility.
devices. FETs have two crucial parameters: the carrier mobility The use of high-κ materials, such as HfO2, Al2O3 and AlN,
determining the feasible operation frequency and the on/ with large dielectric constants as the dielectric layers of 2D
off ratio as the cornerstone to realize reliable switching char- metal chalcogenide FETs can effectively increase the car-
acteristics. Ultrahigh electron and hole mobilities have been rier mobilities due to their screening effects for Coulomb
discovered in graphene and black phosphorus. However, the impurity scattering.[42a,51,55,84] Cui et al. observed this remark-
gapless band of graphene resulting in a low on/off ratio limits able enhancement by comparing the pristine device with a
its performance in FETs, and black phosphorus is unstable in processed device covered by 10 nm Al2O3 on SiO2, and the
an atmospheric environment. Numerous 2D metal chalcoge- metal-insulator transition phenomenon also appeared in the
nides with a natural bandgap and preferable stability have been device with an Al2O3 dielectric (Figure 6c,d).[42a] In addition to
proven to be appropriate for FETs. 2D metal chalcogenides Coulomb impurity scattering, remote phonon scattering from
expand the electronic applications of FETs. However, their dielectrics should also be considered when different insulators
unique atomic structures pose some challenges in terms of are utilized as dielectrics. The experimental and theoretical car-
the appropriate device structure and processing technology. To rier mobilities for different dielectric materials are shown in
date, diverse strategies to design the channels, dielectrics, and Figure 6e,f, respectively, and AlN has the highest mobility in the
electrodes of FETs based on 2D metal chalcogenides have been low-field region.[55] Polymethyl methacrylate (PMMA) can also
widely investigated to improve the performance. be applied as the dielectric (Figure 6g), which can suppress the
Figure 6a shows a typical structure schematic of 2D metal scattering from interfacial impurities and is more convenient
chalcogenide FETs. 2D metal chalcogenides as channel mate- than depositing dielectric layers.[16,41b,85] Insulating h-BN is an
rials are usually placed on insulating silicon oxide, with a ideal dielectric material for 2D metal chalcogenides due to its
heavily doped silicon substrate as the bottom gate, and con- good compatibility, lack of surface dangling bonds and effective
nected with two pieces of metallic materials as the source and screening of the scattering of substrate phonons and impuri-
drain electrodes on both lateral sides. For top-gate devices, the ties. Moreover, it induces fewer trap states than oxide dielec-
top gate should be assembled over the channel with separation trics, which benefits the device reliability. With the surrounding
by an appropriate dielectric layer. The source-drain current can h-BN encapsulation, the channel materials can be protected
be tuned by the bottom-gate (top-gate) voltage. Figure 6b shows from ambient interference and corrosion.[7,20c,73,86] Figure 6h,i
the transfer characteristics for both n-type and p-type channel show the diagram of the device with h-BN as the dielectric and
FETs, where electrons or holes flow past the channel under its STEM image, respectively, where the interfaces of different
positive or negative bias, respectively.[60a] Ambipolar FETs can layers can be clearly distinguished. The selection of different
even exhibit both types of transfer characteristics.[41a,78] Var- electrodes will impact the transfer properties and carrier type
ious 2D metal chalcogenides have been used for FETs, such due to the Schottky barrier and interfacial states, which have
as MoS2,[51b] WS2,[78e,79] MoSe2,[41a] MoTe2,[78c,80] WSe2,[20d,78b,81] been introduced above.[41b,62b,73]
ReSe2,[20b,78a] ReS2,[24b] SnS2,[29b] SnSe2,[20a] and InSe.[7,16,82] Some attempts have been made to realize practical applica-
Among all 2D metal chalcogenides, MoS2 is a representative tions based on FETs, such as super-short channel devices,[87]
2D metal chalcogenide first utilized as a channel material due logic circuits,[29b,66a,78c,88] amplifiers[89] and memory.[90] The gate
to its band gap of 1.8 eV for the monolayer,[3a] which enables a length, a vital characteristic parameter, is a few nanometers for
Figure 6. a) Structure diagram of a typical FET based on 2D materials. Reproduced with permission.[51b] Copyright 2011, Springer Nature. b) Transfer
characteristics and schematics for n-type and p-type conductivities. Reproduced with permission.[60a] Copyright 2018, Royal Society of Chemistry.
c,d) Curves of the conductance dependence on the gate voltage at different temperatures based on the only SiO2 dielectric and Al2O3 added dielectric,
respectively. c,d) Reproduced with permission.[42a] Copyright 2015, Wiley-VCH. e) Experimental field effect mobilities as functions of the electric field
intensity for different dielectrics. f) Theoretical field effect mobilities for different dielectrics. e,f) Reproduced with permission.[55] Copyright 2016,
Wiley-VCH. g) The FET structure diagram with PMMA as the dielectric. Reproduced with permission.[16] Copyright 2014, Wiley-VCH. h,i) Structure
diagram and cross-sectional STEM image of a MoS2 device with the hBN dielectric and graphene electrodes. h,i) Reproduced with permission.[73]
Copyright 2015, Springer Nature.
modern integrated circuits. Carriers in 2D metal chalcogenides (Figure 7h), static random access memory (Figure 7i) and an
can be better controlled by the gate voltage than those in tra- oscillator (Figure 7j), have been investigated.[66a,88b] The analog
ditional bulk materials due to the atom-scale thickness. Desai circuit is another vitally important part of modern electronics.
et al. assembled a MoS2 device possessing a super-short gate Using a structure similar to that of the NOR logic unit, a
composed of single-walled carbon nanotubes with excellent small-signal amplifier with a gain of ≈1 at 2 kHz (Figure 7k)
subthreshold swing (65 mV·dec−1) and on/off current ratio can be built.[89] In particular, 2D metal chalcogenide FETs with
(106).[87a] The schematic structure and an optical microscope ambipolar properties provide flexible strategies for analog
image are shown in Figure 7a,b, respectively. Another work circuits.[78c] Referring to nonvolatile memory applications, the
realized a channel length of 4 nm for MoS2 FETs by laying memory cell based on the traditional flash memory structure in
monolayer MoS2 on etched graphene with an ultranarrow which monolayered MoS2 and few-layered graphene are used
gap (Figure 7c).[87b] Song et al. used SnS2 to realize a NOR as the channel material and floating gate, respectively, exhibits
logic unit, which possesses excellent output swing (>90%) strong charge-storage ability (maintaining 30% charge after ten
and voltage gain (3.5).[29b] This NOR logic unit was assembled years), and the structure schematic is shown in Figure 7l.[90a]
according to the structure shown in Figure 7d. Figure 7e,f pre- Some researchers have also investigated novel nonvolatile
sents an optical microscope image and the circuit diagram, memory combining 2D metal chalcogenides with ferroelectric
respectively. The unit transfer characteristic (Figure 7g) dem- materials.[90b,c] Ko et al. designed a nonvolatile memory with
onstrates the feasible logic operation. In addition to simple 2D metal chalcogenides as channels and Pb[Zr0.2Ti0.8]O3 as the
logic circuits, complex logic circuits, such as a NAND logic gate ferroelectric material.[90b] This 2D ferroelectric FET memory
Table 4. Carrier mobilities of 2D metal chalcogenides usually used for channel materials.
Thickness Contact materials Device structure/dielectric Electron mobility [cm2 V−1 s−1] Hole mobility [cm2 V−1 s−1] Ref.
InSe 6L Graphene Top gate/hBN 1000 [7]
12 700 (below 50 K)
InSe 35 nm Au/Cr Back gate/Al2O3 and PMMA 1055 [16]
GeS 1L 3680 (calculated) [13j]
MoS2 1L Ti/Pd Back gate/SiO2 (285 nm) and HfO2 (10 nm) 150 [51a]
MoS2 4–20 nm Transferred Ag (n type) Back gate/SiO2 (300 nm) 260 175 [41b]
Transferred Pt (p type) and PMMA (170 nm)
MoSe2 7 nm Au/Ti Back gate/SiO2 (270 nm) 200 150 [41a]
250 (Hall) 250 (Hall)
MoTe2 3L Au/Ti Back gate/SiO2 (270 nm) 20 (2L) [80]
7L 27 (7L)
WS2 1L Ti/Pd Back gate/SiO2 (300 nm) 83 [42a]
and Al2O3 (10 nm) 337 (low temperature)
WSe2 1L Au/Ni Top gate/ion gels 7 90 [81]
SnS2 1L Au/Ti Top gate/Al2O3 (35 nm) 50 [29b]
SnSe2 8.6 nm Au/Ti Back gate/SiO2 (300 nm) 85 [20a]
233 (78 K)
ReS2 2L Au/Cr Back gate/SiO2 (285 nm) 12 [24b]
26 (77 K)
ReSe2 7.7 nm Au Back gate/SiO2 (300 nm) 0.36 0.22 [78a]
Metal contacts are usually built via deposition methods. Carrier mobilities without marks are field-effect mobilities at room temperature.
possesses data retention time over 10 d and a switching voltage been proven to exhibit n-type and p-type behaviors, respec-
less than 2.5 V. Moreover, Liu et al. constructed quasi-nonvola- tively.[92] Stable p–n homojunctions based on these two types
tile memory with a nanosecond write time and a longer charge of doped MoS2 were built by Svatek et al..[93] Hole doping can
hold time than that of dynamic random access memory.[91] also be induced through plasma treatment. Combining plasma-
This memory possesses a semi-floating gate structure obtained assisted p-MoS2 with intrinsic n-MoS2 is another approach.[94]
via stacking of WSe2, MoS2, HfS2, and hBN. WSe2 and MoS2 However, the above methods will destroy the atomic structures,
constitute the p–n junction to control the charge injection and and the few-atomic-layer thickness of 2D materials makes their
discharge, and HfS2 as the floating gate maintains the charge. properties susceptible. Surface engineering is a facile approach
to modulate the carrier type. Spin-coating AuCl3 on the sur-
face of MoS2 has been demonstrated to effectively realize
4.1.2. p–n Junctions p-type doping.[95] In contrast to AuCl3-induced p-type doping,
hydrazine can serve as the electron donor, which has been
The p–n junction constituted by both n-type and p-type semi- confirmed with WSe2-based p–n homojunctions.[96] Moreover,
conducting materials is another important type of electronic both lateral (Figure 8a) and vertical (Figure 8b) homojunctions
device. The band alignment of p–n junctions can modulate are easily realized through surface engineering doping. The
internal carriers and bring about new electronic applications. ingenious approach of inserting a foreign atom layer into the
The intrinsic carrier types of different 2D metal chalcoge- interlayer of a bilayered 2D metal chalcogenide can effectively
nides derive from vacancies and defects.[40a] In addition, the modulate the conducting behavior.[97] Intrinsic SnS2 exhibits
electrode material and ambient environment also influence the an n-type behavior, which is attributed to the sulfur vacan-
carrier type.[41b,61b,62b] Hence, by selecting appropriate 2D metal cies. With copper or cobalt intercalation, SnS2 will behave as
chalcogenides and device structures, various p–n junctions can a p-type semiconductor or metal, respectively. Figure 8c shows
be built. Moreover, due to the super smooth surfaces without an optical microscope image of a p–n homojunction composed
dangling bonds of 2D metal chalcogenides, p–n heterojunc- of intrinsic n-SnS2 and Cu-intercalated p-SnS2. In addition to
tions with relatively large lattice mismatch are realizable. p–n homojunctions, homojunctions with different doping den-
The p–n junction of 2D metal chalcogenides is mentioned sities or band structures in different regions are noteworthy.
here, including both the p–n homojunction and heterojunction. An n+–n homojunction can be realized by repairing the sulfur
p–n homojunctions can be realized by modulating the carrier vacancies of MoS2, and its band structure diagram is shown
type. Impurity doping is an important method used to build in Figure 8d.[98] Homojunctions of 2D metal chalcogenides
p–n junctions for silicon-based integrated circuits, and it can with different thicknesses possess band alignments similar
also be utilized in the processing of 2D metal chalcogenides. to those of conventional heterojunctions.[99] Figure 8e shows
With the substitutional doping of iron and niobium, MoS2 has the scanning tunneling spectra for the band alignment of the
Figure 7. a,b) Structure schematic and optical microscope image of a MoS2 FET with a special gate electrode constituted by single-walled carbon
nanotubes. a,b) Reproduced with permission.[87a] Copyright 2016, American Association for the Advancement of Science. c) Diagram of an ultra-
short-channel FET realized by etching graphene to two pieces of graphene electrodes. Reproduced with permission.[87b] Copyright 2017, Wiley-VCH.
d–g) Device diagram, optical image, circuit diagram, and output characteristic of a NOR logic unit based on SnS2. d-g) Reproduced with permission.[29b]
Copyright 2013, Royal Society of Chemistry. h) NAND logic unit based on MoS2. i) Static random-access memory unit based on MoS2. j) Oscillator
based on MoS2. h–j) Reproduced with permission.[88b] Copyright 2012, American Chemical Society. k) Frequency-dependent gain of a small-signal ampli-
fier based on monolayered MoS2. Reproduced with permission.[89] Copyright 2012, AIP Publishing. l) Structure diagram of a nonvolatile flash memory
unit based on MoS2 and graphene. Reproduced with permission.[90a] Copyright 2013, American Chemical Society.
homojunction with bilayered and monolayered WSe2 in dif- organics,[105] and perovskite,[106] can also be combined with
ferent regions.[100] 2D metal chalcogenides to form p–n junctions.
For p–n heterojunctions, two types of heterojunctions exist: Vertical p–n junctions have two main configurations for
vertical and lateral heterojunctions. Stacking of 2D metal chal- (Figure 9a): the partially overlapped mode, where there is at
cogenides with different conducting types can easily constitute least one electrode connecting to only one component, and the
a vertical p–n heterojunction (Figure 8f),[101] even when the entirely overlapped mode, where two components parallelly
components possess a large lattice mismatch.[29a] Lateral p–n exist between the source and drain electrodes. For the entirely
heterojunctions (Figure 8g), however, can only be obtained overlapped mode, the electrons or holes of the noncontact
through bottom-up growth methods, such as CVD and physical layer can easily transfer into the electrode through tunneling
vapor deposition (PVD), rather than by mechanical stacking.[102] due to the ultrathin structure.[95b] The p–n junctions for each
Other materials, such as silicon,[103] GaN,[104] phosphorene,[13f ] mode present different I–V characteristics.[107] Usually, an
Figure 8. a) Cross-sectional diagram of the lateral p–n junction fabricated through AuCl3 surface doping. Reproduced with permission.[95c] Copyright 2014,
American Chemical Society. b) Cross-sectional diagram of the vertical p–n junction fabricated through AuCl3 surface doping. Reproduced with
permission.[95b] Copyright 2015, Springer Nature. c) Optical image of the p–n junction constituted by intrinsic n-type SnS2 and Cu-intercalated p-type
SnS2. Reproduced with permission.[97] Copyright 2018, Springer Nature. d) Band alignment of an n+–n MoS2 homojunction fabricated by repairing sulfur
vacancies. Reproduced with permission.[98] Copyright 2017, Springer Nature. e) Scanning tunneling spectra for the band alignment of the homojunction
with bilayered and monolayered WSe2. Reproduced with permission.[100] Copyright 2016, Springer Nature. f) Optical image of a p–n junction device
obtained via stacking of MoS2 and WSe2. Reproduced with permission.[101] Copyright 2015, John Wiley and Sons. g) Optical image of a CVD-grown
lateral MoS2/WSe2 heterojunction. Reproduced with permission.[102b] Copyright 2015, American Association for the Advancement of Science.
obvious current-rectification characteristic similar to that of Under the modulation of the gate bias, ambipolar char-
bulk p–n diodes can be observed for the partially overlapped acteristics can be realized in entirely overlapped devices due
mode.[71c,d,f,95c,101,107,108] Li et al. found rectification in the to the existence of both electron and hole transport channels
entirely overlapped device (Figure 9b).[95b] We attribute this (Figure 9f).[95b,107] The special device shown in Figure 9g
result to the thick channel (≈11 nm here) of this device. Lee et al. also exhibits ambipolar behavior, which is attributed to the
have investigated the current-rectification characteristic of the tunneling of minority carriers from the bottom noncontact
p–n junction built via stacking one layer of MoS2 on another channel.[101] For partially overlapped devices, an additional
layer of WSe2 (Figure 9b).[108b] The individual transfer character- current peak called the antiambipolar peak appears in the
istics can be measured through their respective electrodes, and common current window of n-type and p-type channels, as
MoS2 and WSe2 show n-type and p-type behaviors, respectively, shown in Figure 9h.[71c,101,108a,111] This antiambipolar behavior
as shown in the inset of Figure 9c. The integral p–n junction provides a new option for electronic device design. In addition,
exhibits the current-rectification characteristic (Figure 9d). This Cheng et al. designed a novel van der Waals device (Figure 9i)
p–n junction has a different physical mechanism compared possessing the programmable rectification characteristic shown
with conventional p–n diodes. No depletion region exists in the in Figure 9j, which holds promise for memory applications.[112]
2D p–n junction due to its atom-thick structure. When a posi-
tive bias is applied, electrons and holes congregated in n-MoS2
and p-WSe2 will recombine with the assistance of tunneling in 4.1.3. Tunneling Devices
the overlapped region to induce a corresponding drain-source
current, as shown in Figure 9d. However, since both electrons Reducing the operation voltages is an effective strategy to opti-
and holes are depleted at a negative bias, the drain source will mize the power dissipation of modern integrated circuits. A
be cut off. Moreover, Bhunia et al. have confirmed an obvious pivotal parameter, the subthreshold swing, defined as the gate
current rectification of p–n junctions in the vertical direction operation voltage needed to decrease the source-drain current
via scanning tunneling microscopy.[109] The lateral p–n junc- by one order magnitude, reveals the potential of FETs for low-
tions with the current-rectification characteristic possess carrier power dissipation. However, the thermionic injection mecha-
transport similar to that in conventional p–n diodes.[95c,102b,110] nism of carriers in conventional FETs limits the pursuit of a
The rectification ratios of p–n junctions are altered following very low subthreshold swing. Tunneling devices, realizing a
the variation of the gate voltage, in general reaching the max- fast on/off switching based on interband tunneling by bending
imum at a nonvanishing gate voltage, which is clearly demon- the band using a gate bias, are presented as promising can-
strated in Figure 9e.[71f,107] didates for low-power FETs with a lower subthreshold swing
Figure 9. a) Two configurations for vertical p–n junctions, including the partially overlapped mode and entirely overlapped mode. b) Optical image of a
stacked heterojunction, where the D1 and D2 electrodes connect with WSe2 and the S1 and S2 electrodes connect with MoS2. c) Output characteristics
between D1 and S1 exhibited in (a) at various gate biases. d) Band alignment along the lateral direction for the D1–S1 configuration. b–d) Reproduced
with permission.[108b] Copyright 2014, Springer Nature. e) Gate-voltage-dependent rectification ratios of p–n junctions. Reproduced with permission.[71f ]
Copyright 2018, Wiley-VCH. f) Drain-source current map as a function of the drain-source and gate voltages, which reveals different conduction
characteristics. Reproduced with permission.[95b] Copyright 2015, Springer Nature. g) Ambipolar carrier transport of a special heterojunction device.
Reproduced with permission.[101] Copyright 2015, Wiley-VCH. h) Antiambipolar carrier transport characteristic. Reproduced with permission.[111] Copy-
right 2016, American Chemical Society. i,j) Device diagram and output curves of a programmable rectification device based on MoS2 and MoTe2. i,j)
Reproduced with permission.[112] Copyright 2018, Springer Nature.
than conventional FETs. Various tunneling FETs based on con- stacking different 2D materials together and is extensively used
ventional bulk semiconductors, including silicon and indium for tunneling devices. Heterojunctions with intrinsic type-III
arsenide, have been investigated.[113] 2D metal chalcogenides band alignment as the channel of tunneling devices have been
with ultrathin bodies and operable band structures can also be presented.[72,116] Yan et al. first investigated the heterojunc-
applied in tunneling FETs. In addition, the tunneling current tion constituted by n-type SnSe2 and p-type black phosphorus
plays an important role in the charge carrier transport of 2D (Figure 10b) and proved its type-III band alignment as an Esaki
systems. diode.[72] The obvious negative differential resistance (NDR)
In 2012, a tunneling FET with the structure of graphene/ effect at room temperature, a representative characteristic of
barrier/graphene (Figure 10a) was built to realize a good off Esaki diodes, can be observed in the I–V curve (Figure 10c).
state for graphene devices.[114] MoS2 as the barrier provides Figure 10d presents the band alignments at different biases as
an on/off ratio (≈104) two hundred times larger than that of a suitable explanation of the I–V characteristic. The variation
hBN. Tunneling devices with similar structures based on other of the band alignment is similar to that of conventional Esaki
2D metal chalcogenides were also investigated in subsequent diodes. Furthermore, when a gate voltage is applied, the peak
studies.[115] Type-III band alignment is easily implemented by value of the I–V curve with the NDR effect will be changed
Figure 10. a) Cross-sectional diagram of a graphene/barrier/graphene tunneling FET. Reproduced with permission.[114] Copyright 2012, American
Association for the Advancement of Science. b) Optical image of an Esaki diode constituted by a stacked n-SnSe2/p-black phosphorus heterojunc-
tion possessing type-III band alignment. c) Output characteristics at 80 and 300 K of the Esaki diode in (b). d) Band alignments corresponding to
different regions at the different biases shown in (c). b–d) Reproduced with permission.[72] Copyright 2015, American Chemical Society. e) I–V curves
with the NDR effect under various gate voltages. Reproduced with permission.[116] Copyright 2016, Springer Nature. f,g) Cross-sectional diagram and
I–V characteristics of a special MoS2/WSe2 device with two regulating gates. f,g) Reproduced with permission.[117] Copyright 2015, American Chemical
Society. h) Diagram of a tunneling junction obtained via heavy doping. Reproduced with permission.[120] Copyright 2017, American Physical Society.
i) Cross-sectional diagram, optical image, and truth table of a ternary logic circuit based on 2D metal chalcogenides. Reproduced with permission.[118]
Copyright 2016, American Chemical Society.
due to the accumulation or depletion of carriers, as shown in semiconductors, can be used to regulate the carrier motion.[122]
Figure 10e.[116] Roy et al. assembled a special device based on The asymmetric I–V characteristic caused by the Schottky bar-
the MoS2/WSe2 heterojunction with two gates (Figure 10f).[117] rier is observed in the MoS2 FETs with Pd and Cr/Au depos-
This heterojunction possesses intrinsic type-II band alignment ited as electrodes (Figure 11a,b).[95c] Das et al. achieved bipolar
that can be transformed into type-III band alignment under behavior instead of the usual n-type behavior in MoS2 devices,
appropriate gate biases, and the two gates enable the modulated in which the hole injection occurred by means of Schottky bar-
device to work as an Esaki diode. Figure 10g shows the I–V rier tunneling.[122d] The Schottky barrier is formed due to the
curves of this device in the tunneling mode. This result con- strong Fermi level pinning in this device (Figure 11c) with Pd/Ti
firmed in the following work of Norbakhsh,[118] and it is also electrodes and a channel length of 4 µm. Figure 11e–g shows
applicable to the WSe2/SnSe2 system.[74a,119] Mukherjee et al. band alignments at different gate biases corresponding to three
realized a tunneling junction (Figure 10h) via heavy doping, regions of the transfer curve (Figure 11d). In region I with a
where Re and Nb were doped into WSe2 as the electron donor larger Vg than Vfb (the flat band voltage), the curve is dominated
and acceptor, respectively.[120] For practical applications, tun- by both thermionic emission and tunneling. When Vg decreases
neling devices based on 2D metal chalcogenides are promising to below Vfb, the tunneling current disappears. Referring to the
for ternary logic circuits.[116,118,121] Figure 10i demonstrates an negative gate bias, a sufficient bias induces the reduction of
example of this application. the metal Fermi level to below the valence band edge of MoS2,
and hole tunneling through the Schottky barrier can lead to
successful injection into MoS2. NbS2 is a metallic 2D metal
4.1.4. Schottky Junctions chalcogenides that can be used to build complete 2D Schottky
junctions.[123] The NbS2/MoS2 junction with a Schottky bar-
In addition to three types of electronic devices mentioned rier of 0.5 eV has been investigated.[122e] An optical microscope
above, Schottky junctions, possessing the Schottky bar- image of this device with four electrodes, where NbS2 is stacked
rier formed due to the mismatch of the working function above MoS2, is shown in Figure 11h. When electron-1 or elec-
or Fermi level pinning of the interface between metals and tron-2 serve as one termination and electron-3 and electron-4
Figure 11. a,b) Optical image and I–V curves at various gate voltages of a Schottky junction. a,b) Reproduced with permission.[95c] Copyright 2014,
American Chemical Society. c) Optical image of a MoS2 device with bipolar behavior. d) Transfer curve of the device in (c). e–g) Band alignments of
the Schottky junction in regions I, II, and II. c–g) Reproduced with permission.[122d] Copyright 2014, American Chemical Society. h–j) Optical image,
output curve, and transfer curve of a stacked NbS2/MoS2 Schottky heterojunction. k) Working schematics of the device in (h) at forward and reverse
gate biases. h–k) Reproduced with permission.[122e] Copyright 2018, American Chemical Society.
serve as another termination, this device works in the Schottky provides the possibility to extend the optoelectronic applica-
diode mode. Furthermore, the use of NbS2 as the gate can con- tions. Some remarkable optoelectronic applications, including
vert this device to the FET mode where MoS2 is the channel. photodetectors, solar cells, and light-emitting devices, will be
This Schottky device in the diode mode demonstrates the discussed below.
obvious rectification characteristic, as shown in Figure 11i. In
the FET mode, this device possesses a subthreshold swing of
67 mV·dec−1 and an on/off ratio of 106, obtained from the transfer 4.2.1. Photodetectors
curve (Figure 11j). Figure 11k shows schematics of the device in
different working states. The channel is conductive at forward Photodetectors are important optoelectronic devices for con-
bias, whereas it will be switched off at reverse bias because elec- verting an optical signal into an electric signal. Electron-hole
trons in the channel below the NbS2 gate are depleted. pairs in semiconductors are generated and separated by the
gap under light illumination. Generated electrons and holes
can act as carriers and impact the conductivity of semiconduc-
4.2. Optoelectronic Devices tors. Based on this process, an optical signal can be effectively
detected, and it is manifested by the variations in the electric-
In contrast to gapless graphene, the abundant band struc- transport characteristics. Beyond conventional photodetectors
tures of 2D metal chalcogenides provide a reliable foundation composed of bulk materials, 2D materials provide emerging
for optoelectronic applications. Their spatial restriction to an opportunities for photodetectors with remarkable transparency,
ultrathin atomic-scale plane provides optoelectronic properties excellent flexibility, and ultrathin thickness. Graphene has been
distinct from those of conventional bulk materials. Moreover, investigated for photodetectors, but it is limited by its gapless
the outstanding ability to form van der Waals heterojunctions band structure.[124] 2D metal chalcogenides possess diverse
Figure 12. a,b) Device diagram and photocurrent map of a MoS2 phototransistor. c) Corresponding photoresponsivity spectrum from 400 to 800 nm.
d) Transfer curves under illumination and dark environments. e) Diagrams of band alignments and carrier motion under illumination at different gate
voltages. a–e) Reproduced with permission.[126] Copyright 2013, Springer Nature. f) Band gaps for MoS2 with different thicknesses. Reproduced with
permission.[131] Copyright 2012, American Chemical Society. g–i) Device diagram, anisotropic light absorption spectra, and photocurrent map of a
polarization-sensitive photodetector based on GeSe. g–i) Reproduced with permission.[6] Copyright 2017, American Chemical Society. j–l) Structure
diagram, optical image, and frequency-dependent radio frequency signal response curve of a MoTe2 waveguide photodetector. j–l) Reproduced with
permission.[150] Copyright 2018, American Chemical Society.
band structures and can be assembled into different van der of electron-hole pairs excited by photons and their movement
Waals junctions, which can realize the universal detection of driven by the drain-source voltage. The thermionic transport
light with different wavelengths ranging from the infrared to and tunneling transport together dominate the extraction of
ultraviolet regions. generated electrons and holes. The absorption of ambient air on
Compared with the indirect bandgap of the bulk form, mono the surface of 2D metal chalcogenides has been proven to influ-
layered MoS2 becomes a direct bandgap material, which is bene- ence the photodetector properties.[127] The adsorbed air will reduce
ficial for light absorption.[3] Monolayered MoS2 has been utilized the p-type doping and introduce Coulomb traps. Traps can
to build phototransistors (Figure 12a) and exhibits reliable accelerate the recombination of generated electron-hole pairs.
optical switching properties.[125] Lopez-Sanchez et al. realized Fast recombination leading to a short photocurrent relaxation
an ultrasensitive phototransistor based on monolayered MoS2 time is conducive to realizing a high-frequency photoresponse.
with a remarkable photoresponsivity of 880 A W−1 under laser However, the reduced carrier mobility caused by the additional
illumination (561 nm).[126] The photocurrent map is exhibited carrier scattering decreases the photocurrent gain and photore-
in Figure 12b. The photoresponsivity decreases with increasing sponsivity. The encapsulation and control of trap states in 2D
illumination wavelength, and an obvious demarcation exists at metal chalcogenides can be considered useful means to opti-
≈680 nm, corresponding to the bandgap of MoS2, as shown in mize photodetector properties. The electrode contact is also an
Figure 12c. The photocurrent gain can be observed for both the important factor in the photodetector properties.[66c,128] Xu et al.
on and off states (Figure 12d). Figure 12e shows the genera- used glassy graphene as electrodes to realize a photodetector
tion of a photocurrent, which can be attributed to the existence with a high detectivity (1.8 × 1010 Jones), in which an ohmic
contact replaces the usual Schottky contact.[66c] Inserting a TiO2 photoelectronic memory based on 2D metal chalcogenide with
interlayer between metal electrodes and 2D metal chalcogenides the designed devices structures has been investigated. Roy et al.
has been proven to be effective in enhancing the properties of investigated the persistent photoconductivity of MoS2/graphene
photodetectors.[129] The distance between electrodes can also hybrid structures, which possessed a sustained decrease lasting
influence the photo-responsivity, which has been investigated close to 100 s.[151] Lee et al. designed multibit MoS2 photo-
toward the realization of GaSe photodetectors.[130] In addition to electronic memories, which can realize the 3 bit data storage
monolayered devices, detectors working in different wavelength retaining over 104 s and possess stable writing-erasing cycles of
regions can be designed by changing the number of layers of 200 times.[152] MoS2 was used as the photoresponse channels,
2D metal chalcogenides due to the dependence of their band- and Au nanoparticles separated by a tunneling gate dielectric
gaps on the thickness (Figure 12f).[131] layer was used as the charge-trapping layer. Under the control
Numerous 2D metal chalcogenides with natural bandgaps, of illumination and gate electric fields, photonic signal can be
such as WS2,[132] MoSe2,[133] ReS2,[134] SnS2,[135] SnSe2,[136] stored in this memory. Xiang et al. have also realized a simple
HfS2,[137] InSe,[138] GaTe,[15] TiS3,[35b] and In2Se3,[8a] have been photoelectronic memory based on WSe2/hBN heterojunctions
investigated for their excellent photodetector properties. InSe with retention time ≈4.5 × 104 s.[153]
and SnS2 have been experimentally proven to easily realize
faster photoresponses (87 µs for InSe and 5 µs for SnS2) than
other 2D metal chalcogenides.[28,139] 2D metal chalcogenides 4.2.2. Solar Cells
with different bandgaps can be used to detect different wave-
length light, such as visible-light detectors based on SnSe The photovoltaic effect is an important physical phenomenon
or GeSe[140] and broadband mid-infrared detectors based on in which the illumination can induce the formation of a sponta-
PtSe2.[141] Moreover, alloys, such as GaS1−xSex, can be adapted neous voltage in devices. Applications based on the photovoltaic
to different wavelength light by altering the constituents.[142] In effect are an important direction for clean energy technology.
addition, semimetallic 2D metal chalcogenides exhibits superior The photovoltaic effect was primarily used to convert solar
performance for broadband (especially for mid-infrared) energy into electric energy based on silicon p–n junctions in
photodetectors. Photodetectors based on type-II Weyl semimetal 1954.[154] The silicon-based device is still the mainstream solar
Td-MoTe2 have been tested with a broadband photoresponse cells. The basis of the photovoltaic effect is the excitation of
from 532 nm to 10.6 µm.[143] electrons and holes under illumination, and another pivotal
Some 2D metal chalcogenides can exhibit anisotropic light process is the separation of electron-hole pairs to effectively
absorption due to prominent differences in their lattices in dif- form a photovoltage. The bandgaps of 2D metal chalcogenides
ferent directions.[6,144] Wang et al. built a polarization-sensitive covering the spectrum ranging from near-infrared to visible
photodetector based on GeSe (Figure 12g), which exhibits a wavelengths enable effective light absorption.[1d] 2D metal chal-
remarkable dichroic ratio and possesses the highest dichroic cogenides are supposed to have high power conversion efficien-
ratio (Ipy/Ipx of ≈2.16) for the 808 nm laser compared with other cies but are limited by large exciton binding energies.[155] The
wavelengths.[6] Figure 12h,i demonstrates the anisotropic light built-in electric fields induced by various junctions can be uti-
absorption spectra and photocurrent colormap, respectively. lized to separate excited electron-hole pairs into two terminals
GeSe2 also possesses an anisotropic crystal structure and a of a junction. p–n and Schottky junctions can be easily built
relatively wide bandgap of 2.74 eV, providing the possibility for based on 2D metal chalcogenides. The special van der Waals
short-wave polarization-sensitive photodetectors.[145] junctions free from lattice mismatch are beneficial to reducing
Using different 2D metal chalcogenides to build van der defects at interfaces that can hasten the recombination of
Waals junctions is also an important technique for realizing excited electron-hole pairs. Hence, 2D metal chalcogenides
photodetectors.[107,146] Compared with single-constituent provide an attractive option for solar cells, especially ultrathin,
photodetectors, the design of photodetectors based on van ultralight and flexible devices.
der Waals junctions is flexible, convenient and adaptable due Type-II heterojunctions possess favorable band alignment,
to the devisable band alignments and advantageous built- which can enable effective separation of electrons and holes
in electric fields.[147] Chen et al. have proven that the MoTe2/ excited by illumination. As shown in Figure 13a, electrons in
MoS2 heterojunction photodetector presents an ultralow dark a type-II heterojunction tend to accumulate at the side with the
current of ≈3 pA and a high on/off ratio.[148] Yan et al. have low conduction band edge, and holes tend to accumulate at the
realized an ultrafast photodetector based on the GaSe/InSe side with the high valence band edge. Various type-II hetero-
heterojunction, where the notable photoresponse time of junction series composed of different 2D metal chalcogenides
≈2 µs is much faster than that reported for single-constituent for solar cells have been investigated in both theoretical and
photodetectors.[17,139,146d] Heterojunction photodetectors assem- experimental studies.[71a,b,e,108b,156] The photovoltaic properties
bled with 0D or 1D materials have also been investigated.[149] of heterojunctions based on some monolayered metal dichal-
For practical applications, a waveguide photodetector based on cogenides and trichalcogenides, including MoS2/WS2, MoSe2/
MoTe2 has been investigated.[150] A schematic illustration and WSe2, TcS2/ReS2, and ZrS3/HfS3 heterojunctions, have been
an optical microscope image are shown in Figure 12j,k. This theoretically calculated.[75,156a] The ZrS3/HfS3 heterojunction
detector possesses an excellent high-frequency photoresponse exhibits the highest power conversion efficiency among these
exceeding 500 MHz (Figure 12l). metal dichalcogenide heterojunctions, which can be ascribed
The photoelectronic memory can store the optical signal and to the enhanced spin-orbit splitting and excitonic effects
possesses the capability of the multilevel storage. Recently, the induced by symmetry breaking.[157] The obvious photovoltaic
Figure 13. a) Diagram of a solar cell and its type-II band alignment. Reproduced with permission.[156a] Copyright 2018, Royal Society of Chemistry.
b) Short-circuit-photocurrent map of a MoS2/WSe2 heterojunction. c) The band alignment and hole-electron recombination processes. d) Photocurrent
density versus voltage curves. b–d) Reproduced with permission.[108b] Copyright 2014, Springer Nature. e,f) Light intensity–dependence curves of the
short-circuit current and open-circuit voltage of a MoS2/WSe2 heterojunction. e,f) Reproduced with permission.[71b] Copyright 2014, American Chemical
Society. g,h) Structure diagram and optical image of a solar cell with split gate electrodes. g,h) Reproduced with permission.[160b] Copyright 2014,
Springer Nature.
effect has been experimentally observed in MoS2/WSe2 efficiency, and an external quantum efficiency exceeding 50%
heterojunctions.[71b,108b,156c] Figure 13b shows the short-circuit was realized.[156c] Furthermore, the short (thin) active region
photocurrent map of a stacked MoS2/WSe2 heterojunction and high conductivity enable effective extraction of photogenic
(Figure 9b), indicating that the overlapping part with the type-II charge carriers from type-II heterojunctions.[156b] Tsai et al.
band alignment acts as an effective working region for photo- built an omnidirectional solar cell based on lateral heterojunc-
voltaic applications. tions, for which a power conversion efficiency of 2.56% and
The short-circuit current and open-circuit voltage are influenced a light absorption efficiency of 95% were reached.[71a] Homo-
by the light intensity and interlayer recombination.[71b,108b,158] The junctions and Schottky junctions can also be used for solar
light intensity can regulate the amount of generated charge car- cells.[41b,c,93,94,159] In particular, the designs with near-perfect
riers. The dominant recombination mechanisms for 2D hetero- Schottky junctions without Fermi level pinning have been
junctions include the SRH (Shockley Read Hall) recombination proven to possess an excellent open-circuit voltage of 1.02 V.[41b]
induced by internal defects or interfacial imperfections and the The special solar cells with lateral p–n junctions formed via
Langevin recombination induced by the Coulomb interaction of electrostatic doping controlled through split gates exhibit excel-
electrons and holes (Figure 13c), which can both be influenced lent photovoltaic properties due to their intact lattice structures
by the carrier concentration.[108b] Increasing the light intensity with high conductivities, and a typical structure schematic and
results in an increase in the carrier concentration, and the recom- an optical microscope image are shown in Figure 13g,h.[160]
bination of photogenic carriers is intensified. Finally, a dynamic The solar cells constituted by 2D metal chalcogenides and other
balance between generated carriers and recombined carriers will materials, such as perovskites[106,161] and silicon,[162] are also
be achieved. Figure 13d demonstrates the J–V characteristics meaningful for extending solar cell applications.
under illumination at different gate voltages that can modulate
the carrier concentration. Curves showing the dependence of the
short-circuit current and open-circuit voltage on the light inten- 4.2.3. Light-Emitting Devices
sity are shown in Figure 13e,f.
Wong et al. explored different device structures based on Electroluminescence based on semiconductor materials is a
the MoS2/WSe2 system to improve the photovoltaic quantum vitally important phenomenon for optoelectronic applications.
Because of the superior and efficient quantum radiation process, junctions were subsequently utilized to enhance the light-emit-
semiconducting light-emitting devices possess the advantages of ting efficiency. The electrostatic-doped p–n junctions previously
stability, controllability, low power consumption, long lifetime, mentioned can also be used as light-emitting devices with an
and good integration, and are widely used in the lighting, photo- electroluminescence efficiency of 0.01–1%.[160b,c,166] An obvious
communication, information storage, indicator light, and dis- light-emitting region located in the middle of the split gate elec-
play fields. Remarkably, research on blue-light-emitting diodes trodes is shown in Figure 14c. Four main peaks appear in the
based on GaN has greatly promoted the development of white low-temperature (60 K) electroluminescence spectrum of the
light illumination.[163] 2D metal chalcogenides are competitive WSe2 light-emitting device, corresponding to X0, X+, X−, and XI
candidates for future electroluminescence applications with (impurity-induced) excitons (Figure 14d).[166] Jo et al. built light-
prominent characteristics of ultrathin structures, excellent trans- emitting transistors with the peculiar ionic liquid gate shown in
parency and good flexibility. Light-emitting devices based on Figure 14e.[167] The usual 2D p–n heterojunctions constituted by
2D metal chalcogenides with different structures, such as the n-type MoS2 and p-type WSe2 have been investigated for light-
Schottky junction, p–n junction, and vertical tunneling hetero- emitting applications, and a light-emission image is shown in
junction, will be introduced in the following paragraphs. Figure 14f.[71d] WSe2 dominates the electroluminescence due to
For 2D metal chalcogenides, electroluminescence was first the primary nonradiative recombination induced by the indi-
observed at the contact region of MoS2 with a metal electrode rect bandgap of few-layered MoS2, and Figure 14g indicates that
(Figure 14a).[164] The large band bending around the Schottky the electroluminescence intensity is stronger in the monolayer
junction contributes to the formation of hot carriers domi- regime than in the bilayer regime. The use of p-doped silicon
nating this electroluminescence.[165] The almost identical peaks as the hole source combined with p-type 2D metal chalcoge-
of the PL and electroluminescence spectra corresponding to nides is an effective strategy to guarantee compatibility with
the A exciton of MoS2[3a] are demonstrated in Figure 14b. p–n conventional silicon integrated technologies.[162,168]
Figure 14. a) Electroluminescence intensity distribution of a MoS2 device. b) Corresponding absorption, photoluminescence, and electroluminescence
spectra. a,b) Reproduced with permission.[164] Copyright 2013, American Chemical Society. c) Electroluminescence intensity distribution of a p–n junc-
tion. d) Corresponding electroluminescence spectra under various current intensities. c,d) Reproduced with permission.[166] Copyright 2014, Springer
Nature. e) Diagram of a light-emitting transistor with an ionic liquid gate. Reproduced with permission.[167] Copyright 2014, American Chemical Society.
f) Electroluminescence image of an n-MoS2/p-WSe2 heterojunction. g) Electroluminescence intensities as a function of the current in the monolayer
and bilayer regions. f,g) Reproduced with permission.[71d] Copyright 2014, American Chemical Society. h,i) False-color STEM image and band alignment
under a high bias of a light-emitting tunneling heterojunction. h,i) Reproduced with permission.[169a] Copyright 2015, Springer Nature. j) Electrolumi-
nescence spectra of pure (red) and nanocavity-modified (blue) WSe2 tunneling heterojunctions. Reproduced with permission.[169d] Copyright 2017,
American Chemical Society. k) Thermal-light-emission device with a trench under MoS2. Reproduced with permission.[171] Copyright 2017, Wiley-VCH.
The fascinating single and multiple tunneling heterojunc- 4.3. Photonics

tions can be used as light-emitting devices.[169] A complete
2D system for tunneling heterojunctions can be formed by Semiconductors play an important role in photonic applica-
conductive graphene offering carriers, insulating hBN as a bar- tions due to their advantageous band structures. Ultrathin
rier, and semiconducting 2D metal chalcogenides as working 2D metal chalcogenides with a direct bandgap are considered
parts. Figure 14h exhibits the typical structure of a light-emit- competitive for photonic applications and can also be easily
ting tunneling heterojunction. The electrons and holes can integrated with different photonic materials and structures.[173]
be injected from two segregated graphene electrodes into the In this section, two types of photonic applications, lasing
2D metal chalcogenide through tunneling at the appropriate devices and plasmonic applications, are briefly introduced.
bias (Figure 14i), and electron-hole excitons recombine to pro-
duce photons. Withers et al. reached a remarkable electrolumi-
nescence external quantum efficiency of 8.4% use a multiple 4.3.1. Lasing Devices
tunneling heterojunction.[169a] An external quantum efficiency
of 5% at room temperature based on WSe2 was presented in Semiconductor lasers with the advantage of a low cost, a long
another of their works, and the dependence of the electrolu- lifetime and facile integration can be used for various practical
minescence on temperature was also investigated.[169b] Li et al. situations, such as optical communication, optical intercon-
observed an abnormally enhanced electroluminescence of mul- nection, and optical information processing. However, the lat-
tilayered MoS2 with an indirect bandgap, which can be attrib- tice mismatch of bulk compound semiconductor lasers with
uted to its special band structure.[169c] In addition, the WSe2 foreign substrates limits their performance. Semiconducting
tunneling heterojunction integrated with a nanocavity exhibits 2D metal chalcogenides are presented as a feasible alternative
the emergence of a new peak (Figure 14j) and possesses a mod- for lasing devices. They can be integrated into different lasing
ulation speed of 1 MHz.[169d] The light-emitting device with a systems and exhibit the capacity to act as the optical cavity, gain
metal-insulator-semiconductor structure is also promising and medium and saturable absorber. Salehzadeh et al. first discov-
has been proven to have a low threshold (few pA·µm−2) and a ered lasing at room temperature of MoS2 placed between a SiO2
quantum efficiency of 1%.[170] Dobusch et al. realized a thermal- microsphere and microdisk (Figure 15a).[174] Under continuous
light-emission device based on MoS2, where the high electron optical pumping, this lasing device presents a series of lasing
temperature reaching 1500–1600 K is ensured via the intrinsic peaks distributed from 600 to 800 nm (Figure 15a), and it pos-
high thermal resistance and isolation from the substrate.[171] sesses superior properties, with a threshold of 5 µW. Another
The unique device structure is demonstrated in Figure 14k. microdisk structure with WS2 as the gain medium embedded
Some investigations of 2D metal chalcogenides have also been in the resonator, shown in Figure 15b, can also be applied for
performed, focusing on pixels for display applications.[105,172] lasing devices.[175] The novel 2D-material-component microdisk
Figure 15. a) PL spectrum and structure diagram of a MoS2 optical cavity. Reproduced with permission.[174] Copyright 2015, American Chemical Society.
b) Diagram of a microdisk cavity with WS2. Reproduced with permission.[175] Copyright 2015, Springer Nature. c) Vertical cavity integrated with mono
layered WS2. Reproduced with permission.[178] Copyright 2017, Springer Nature. d) Schematic of a typical fiber laser with 2D metal chalcogenides.
Reproduced with permission.[180c] Copyright 2016, Royal Society of Chemistry.
cavity in which monolayered WS2 is sandwiched between two laser with the application of 2D metal chalcogenides. Yang et al.
hBN flakes has been investigated for lasing devices.[176] The have also investigated an all-optical modulator based on WS2
excellent performance of hBN in confining optical modes with a high signal-to-noise ratio and low loss, which is prom-
ensures that it is deployable in photonic devices, and the ising for on-chip optical interconnects.[181]
smooth interfaces originating from the van der Waals contacts Single photon emitters are a type of specific lasing devices,
can reduce the optical diffusion loss. Furthermore, Javerzac- which can emit individual photons. Single photon emitters
Galy et al. presented a precise measurement method for cou- based on solid-state devices hold promise for future high-
pled excitonic emission of 2D metal chalcogenides with a resolution metrology, quantum photonics and quantum
high-Q microdisk cavity where a tapered optical fiber is used for information technologies.[182] Some 2D metal chalcogenides
near field coupling with a high efficiency of 90%.[177] In addition with a direct bandgap, such as WSe2 and WS2, provide new
to the microdisk resonant cavity, the vertical cavity integrated options for integrated solid-state single photon emitters in
with monolayered WS2 has been investigated (Figure 15c).[178] the near-infrared and visible wavebands. Usually, the isolated
2D lasing with a low threshold has been realized based on this imperfections of crystals of 2D metal chalcogenides can serve
resonant cavity. Photonic crystal cavities covered by 2D metal as carrier traps and as the origination of single photon emis-
chalcogenides as the gain medium can also be considered for sion (Figure 16a) with a narrow linewidth of 100–130 µeV.[183]
low-threshold lasing devices.[179] A high Q-factor of 5603 and Localized single-photo-emitting centers have been found in
a narrow linewidth of 0.202 nm have been reported for the the interior region of monolayered WSe2 fabricated through
MoTe2 laser.[179a] For fiber lasers, especially near-infrared- and PVD (Figure 16b)[183b] and at edges where defects are easily
visible-spectrum fiber lasers, 2D metal chalcogenides, such as formed, especially for the mechanical exfoliation process
MoS2, WS2, WSe2, and SnSe2, can serve as efficient saturable (Figure 16c).[183c-e] Stable and bright single photon emis-
absorbers.[180] Figure 15d shows a schematic of a typical fiber sion with linear polarization is observed in both situations.
Figure 16. a,b) PL spectrum and PL intensity map at 1.719 eV of monolayer WSe2 with isolated imperfections. a,b) Reproduced with permission.[183b]
Copyright 2015, Springer Nature. c) PL intensity map of an exfoliated 2D material with edge defects. Reproduced with permission.[183e] Copyright 2015,
Optical Society of America. d) Single photon emission spectra under various magnetic flux densities. e) Single photon emission intensity as a function
of the gate voltage and photon energy. d,e) Reproduced with permission.[183c] Copyright 2015, Springer Nature. f,g) PL intensity map and cross-sectional
structure diagram of the corresponding device. f,g) Reproduced with permission.[185c] Copyright 2017, Springer Nature. h,i) Electroluminescence map
and spectra as a function of the excitation voltage. h,i) Reproduced with permission.[186c] Copyright 2016, American Chemical Society.
Figure 17. a) PL spectra of MoS2 modified by various plasmonic silver nanodisk arrays. Reproduced with permission.[187] Copyright 2015, American
Chemical Society. b) Schematic of optical selection rules for valleytronics applications. Reproduced with permission.[195] Copyright 2016, Springer
Nature. c) The spin transport device based on a topological insulator. Reproduced with permission.[196] Copyright 2014, Springer Nature. d) Schematic
diagram of the gas sensor based on WS2. Reproduced with permission.[203] Copyright 2014, Springer Nature. e) Photograph of a flexible MoS2 transistor
and its structure diagram. Reproduced with permission.[205] Copyright 2016, Wily-VCH.
Moreover, Tonndorfe et al. demonstrated that scratching a 4.3.2. Plasmonic Applications

crystal can also result in photon emission.[183e] Obvious Zeeman
effects can be found in these single photon emitters, as shown The relatively weak light-matter interactions of 2D metal
in Figure 16d.[183a,c,d] Figure 16e shows that the PL spectrum chalcogenides suppress their popularization in the fields of
depends on the gate voltage, which indicates the intense influ- photonic and optoelectronic applications due to their ultrathin
ence of local electric fields on the single photon emission.[183c] thickness. Plasmonic materials with strong light-matter inter-
Despite the intrinsic defects of 2D metal chalcogenides, artifi- actions have been used to improve the photonic and optoelec-
cial defects induced by thermal oxidization of WS2 have been tronic performances of 2D metal chalcogenides; moreover,
proven to enable effective realization of single photon emis- these materials exhibit fantastic compatibility. MoS2 with plas-
sion.[184] Strain-induced single photon emission is another monic silver nanodisk arrays shows an intense PL response
important avenue.[185] The strength of the strain can regu- (Figure 17a).[187] A 12-fold enhancement in the PL intensity of
late the photon emission energy, and the remarkable tuning modified MoS2 compared with pristine MoS2 can be realized
scope reaches 170 meV.[185a] Kern et al. realized strain-induced by altering the distance between silver nanodisks. Plasmonic
single photon emitters by placing WSe2 on gold nanorods with nanoparticles with different morphologies, such as nanorods
nanoscale gaps.[185b] The emission regions are located above and nanobowties, have been investigated to enhance the light-
these gaps. Interestingly, the polarization direction of emitted matter interaction of 2D metal chalcogenides.[188] With the
photons varies with the strain orientation. Based on the strain application of silver plasmonic nanotriangles to WSe2, defect
design, large-scale single-photon-emitter arrays for the visible emission is enhanced, as observed in the low-temperature PL
wavelength have been built (Figure 16f).[185c] The fabrication spectra; however, band-edge emission is quenched.[189] This
processes of these devices are demonstrated in Figure 16g. abnormal quenching is attributed to the characteristic band
Electrically pumped single photon emitters with the vertical structures of WSe2 with a dark exciton state. The investiga-
tunneling heterojunction structures mentioned above have tion of MoSe2 with nanoplasmonic waveguide paves the way
been investigated.[186] With the injection of electrons and holes for practical on-chip optical applications.[190] Lee et al. explored
from electrodes, single photon emission can occur in the the influence of plasmonic nanoparticles on the photocatalytic
defect regions (Figure 16h). The electroluminescence spectra activity of WS2.[191] Additionally, the roughness of metal films,
of single photon emitters are easily hidden in the background even when covered by dielectric films, can influence the optical
and, hence, need to be extracted by using a pinhole to select performance of adhered 2D metal chalcogenides via plasmonic
the single-photon-emitting region.[186c] Figure 16i exhibits the resonant coupling.[192] Very recently, a self-assembly method
electroluminescence spectra at different biases. to fabricate plasmonic nanoparticles on MoS2 has been
developed.[193] These self-assembled nanoparticles are attached of electronic, optoelectronic, and photonic applications has
to the point defects of MoS2. been comprehensively introduced above. 2D metal mono-,
di-, and tri-chalcogenides possess distinct crystal structures.
The quantum effect arising from the different crystal struc-
4.4. Other Applications tures results in different material characteristics, such as the
fascinating anisotropy of group IVA monochalcogenides with
In addition to the electronic, optoelectronic, and photonic appli- the black phosphorus-like crystal structure. Some basic device
cations, 2D metal chalcogenides hold promise for other applica- characteristics, i.e., the charge carrier characteristics, scattering
tions, such as spintronics, superconductivity, thermoelectricity, mechanisms, interfacial contacts, and band alignments of
and electrochemistry. The spin is another electron degree of heterojunctions, play an important role in the final perfor-
freedom that can be used for future information technologies, mance of 2D metal chalcogenides for practical applications. For
and 2D metal chalcogenides are an emerging platform to realize 2D metal chalcogenides, their doped charge carriers can usu-
spintronic applications.[194] The development of 2D metal chal- ally be attributed to crystal defects, and the charge carrier type
cogenides provides the possibility and operability of the degree is related to the surface states. Scattering from ambient envi-
of freedom of the valley.[10] The 2H phase group VIB dichal- ronments, such as interfacial impurities, dielectric substrates,
cogenides are appropriate for valleytronics applications due and adsorbates, can intensively affect carrier transport due to
to their degenerate K and K′ points, with the time reversal the ultrathin structure. The interfacial contact influences the
symmetry corresponding to the band edges and large exciton carrier injection in electrode regions and the contact resistance
binding energy induced by the strong Coulomb interaction.[195] of different components. By designing appropriate heterojunc-
Figure 17b illustrates the optical selection rules, i.e., the cou- tions with desired band alignments based on the abundant
pling of light possessing left-circular polarization and right- 2D metal chalcogenides, new physical mechanisms, enhanced
circular polarization with the K and K′ valleys, respectively. properties, and expanded applications can be realized.
Topological insulators based on Bi2Se3, Bi2Te3, and Sb2Te3 have 2D metal chalcogenides hold promise for future electronic,
been demonstrated, and spin-momentum locking appears in the optoelectronic, and photonic applications. Most 2D metal chal-
metallic surface.[37c] A ferromagnetic contact has been designed cogenides naturally possess an advantageous bandgap, which
to manifest the spin-polarization direction (Figure 17c).[196] ensures an adequate on/off ratio and a carrier-modulation ability
This characteristic can be utilized in future spintronics. More- for electronic devices. Electronic devices with different structures,
over, the quantum Hall effect, anomalous quantum Hall effect, such as FETs, p–n junctions, tunneling devices, and Schottky
and quantum spin Hall effect have been observed in 2D metal junctions, have been investigated. The versatile band structures
chalcogenides.[7,14b,197] Some 2D metal chalcogenides exhibit of 2D metal chalcogenides with bandgaps corresponding to the
natural superconductivity.[23b,198] High pressure can also induce broad spectrum from the visible to near-infrared regions are
superconductivity in pristine SnSe2.[199] Moreover, charge den- beneficial to various optoelectronic device applications. Photode-
sity waves usually exist in these 2D metal chalcogenides with sup tectors, solar cells, and light-emitting devices are popular opto-
erconductivity.[25b,36c,200] SnSe with a highly anisotropic crystal electronic application directions. Some investigations have also
structure possessing a relatively high electrical conductivity and focused on photonic applications, including lasing devices and
a low thermal conductivity is considered a fascinating thermo- plasmonic applications. However, thus far, 2D metal chalcoge-
electric material.[19a,201] Additionally, 2D metal chalcogenides are nides are still in the early experimental stage, and confronted
an attractive alternative for electrochemical applications, such with numerous challenges before practical applications can be
as the hydrogen evolution reaction, gas sensors, supercapaci- realized. One challenge is that the properties of the devices are
tors, and batteries, due to their ultrathin atomic structures and far from meeting the application requirements. The low perfor-
advantageous bandgaps.[202] Figure 17d demonstrates the dia- mance can be attributed to two main causes: inevitable imper-
gram of a gas sensor based on WS2 as the sensing material.[203] fections in crystals and immature processing technologies for
Due to the ultrathin structure, 2D metal chalcogenides can also devices. 2D metal chalcogenides with an intrinsic low concentra-
be utilized for flexible applications.[204] A photograph of a typical tion of defects satisfying the semiconductor industrial standard
flexible transistor is exhibited in Figure 17e.[205] have not been achieved. The processing technologies for tradi-
tional materials are usually destructive for the ultrathin atomic
structure of 2D metal chalcogenides, and the introduction of
5. Conclusion and Perspectives contaminants into the interfaces of devices is uncontrollable.
Another challenge is that 2D devices cannot be mass produced
Three main types of 2D metal chalcogenides exist: monochalco- based on state-of-the-art technologies. The present research on
genides, dichalcogenides, and trichalcogenides. After extensive electronic and optoelectronic applications is mainly aimed at
investigations of transition metal chalcogenides for electronic investigating the properties these devices.
and optoelectronic applications, group IV dichalcogenides, To further promote the electronic and optoelectronic appli-
2D metal monochalcogenides, and 2D metal trichalcogenides cations of 2D metal chalcogenides, we can make efforts in
have very recently drawn increasing attention from researchers. the following directions: exploring appropriate 2D metal chal-
The broadened material family of 2D metal chalcogenides cogenides, improving crystal growth methods, developing
provides further reliable and plentiful operations for diverse processing technologies, and investigating compatible device
practical applications. An overview from the crystal structures structures. The exploration of 2D metal chalcogenides has not
and basic device characteristics to the preliminary exploration been completed. Recently, the high electron mobility of InSe has
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Versatile Crystal Structures and (Opto) Electronic Applications of The 2D Metal Mono-, Di-, and Tri-Chalcogenide Nanosheets

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Versatile Crystal Structures and (Opto) Electronic Applications of The 2D Metal Mono-, Di-, and Tri-Chalcogenide Nanosheets

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Metal Chalcogenides www.afm-journal.de

Versatile Crystal Structures and (Opto)electronic Applications

structure limits its applications, especially

is advantageous for reducing the destruction from the sur-

Table 1. Characteristics and applications of 2D metal monochalcogenides.

Adv. Funct. Mater. 2019, 1900040

© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Table 3. Characteristics and applications of 2D metal trichalcogenides.

2.1. 2D Metal Monochalcogenides are beneficial to applications in high-frequency devices and

The fascinating single and multiple tunneling heterojunc- 4.3. Photonics

Moreover, Tonndorfe et al. demonstrated that scratching a 4.3.2. Plasmonic Applications

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