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Group IVB Transition Metal Trichalcogenides: A New Class of 2D Layered

Materials Beyond Graphene

Jun Dai, Department of Chemistry, University of Nebraska-Lincoln, Lincoln, NE, 68588,

USA
Ming Li, College of Chemical Engineering, North China University of Science and
Technology, Tangshan, Hebei, 063000, China and Department of Chemistry, University
of Nebraska-Lincoln, Lincoln, NE, 68588, USA
Xiao Cheng Zeng*, Department of Chemistry, University of Nebraska-Lincoln, Lincoln,
NE, 68588, USA and Collaborative Innovation Center of Chemistry for Energy
Materials, University of Science and Technology of China, Hefei, Anhui 230026, China,
Email: [email protected]

Abstract

This is the author manuscript accepted for publication and has undergone full peer review but has
not been through the copyediting, typesetting, pagination and proofreading process, which may
lead to differences between this version and the Version of Record. Please cite this article as doi:
10.1002/wcms.1243

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The discovery of graphene, a single atomic-layer of carbon in a hexagonal lattice, has invigorated
enormous research interests in two-dimensional (2D) layered materials and their one-dimensional
(1D) derivatives not only owing to their extraordinary physical and chemical properties but also their
high potential for applications in electronic and photonic devices. A weakness of the graphene
however is its lack of a bandgap – a prerequisite for building field-effect transistors (FETs). A stream
of new 2D layered materials have been developed over the past five years, including, among many
others, silicene, phosphorene, and transition metal dichalcogenides (TMDCs). Monolayers of many
of these 2D materials exhibit a bandgap, either direct or indirect. In 2015, a new class of 2D layered
materials, namely, group-IVB transition metal trichalcogenides (TMTCs), has been uncovered. A
prototypical representative of this new class of 2D materials is TiS3 whose monolayer is predicted to
possess a direct band gap of about 1 eV [close to that (1.17 eV) of bulk silicon], and relatively high
carrier mobility. Isolation of the TiS3 nanoribbons via mechanical exfoliation has been realized in the
laboratory in 2015. The modest 1-eV band gap, relatively high carrier mobility, as well as high
chemical stability in open air render TiS3 monolayer a promising 2D material for nanoelectronic and
nanophotonic applications. In this article, we give an overview of the emerging area of 2D and 1D
TMTC materials and suggest future research directions related to these novel materials.

Introduction

The successful isolation of atomic layered graphene sheets from graphite in 20041 has ignited
tremendous research interest in 2D layered materials and their 1D derivatives, due largely to their
novel electronic and optical properties and great potential in variety of applications.2-5 Despite of
graphene’s ultrahigh carrier mobility, it lacks a band gap for controllable operations. Cutting
graphene into nanoribbons can introduce band gaps, however, the carrier mobility of nanoribbons
can be three orders of magnitude lower than that of graphene sheets.6 The hexagonal boron nitride
(h-BN)7 monolayer, on the other hand, is a wide-gap semiconductor. Over the past five years,
extensive efforts have been devoted to the development of new 2D layered materials with modest
band gaps for future-generations of electronics. Indeed, many new 2D layered materials have been
brought to bear, such as group-IV element monolayers (silicene, germanene, and stanene)8-12, group-
V element monolayer (phosphorene)13, 14, and transition metal dichalcogenides (TMDCs)2-4. The
synthesis of free-standing silicene, germanene and stanene is still very challenging, in part because
Si, Ge, and Sn prefer sp3 hybridization. MoS2 and MoSe2 are two prototype TMDCs, whose
monolayers possess desired band gaps. Indeed, monolayer MoS2 based field effect transistors (FETs)
have been fabricated in the laboratory, and shown to exhibit high carrier mobility (~ 200 cm2/V/s) as
well as high on/off ratio (~ 108).15, 16 The value of the carrier mobility reported originally was later
corrected to be about 15 cm2/V/s.17, 18 Although this relatively low value of mobility of 2D MoS2 does
not invoke any concern due to the transport mechanism for the semiconducting channel of the
transistor below 10 nm is dominated by the ballistic process rather than scattering, high mobility and
high performance are still highly desired in other applications such as radio frequency transistors.
The recently rediscovered few-layer phosphorene sheets also possess layer-dependent direct band
gap, ranging from 1.5 eV for the monolayer to about 0.3 eV for the bulk19-24. Phosphorene-based

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FETs were also reported to exhibit very high mobility (~104 cm2/V/s) and high on/off ratio. However,
phosphorene suffers from its high chemical reactivity and environmental instability, thereby
requiring protection layers for long-term device applications.25

Two-dimensional layered materials can be also achieved via mechanical or liquid exfoliation of the
van der Waals (vdW) bulk materials which typically consist of stacked layers of covalently bonded
sheets with weak interlayer vdW interactions26,27. Among the vdW materials, transition metal
trichacogenides (TMTCs) represent a class of materials akin to TMDCs with novel properties.
Although growing attention has been paid to 2D TMTCs from researchers since 2015, literature on
2D TMTCs is still very scarce, and improved understanding of these 2D atomic layered materials is
yet to come. Here, we provide an overview of recent experimental and theoretical advancement in
2D and 1D TMTC fabrication and characterization studies, discuss some challenges, and suggest
possible new research directions.

Composition and Structure

Transition metal trichalcogenides (MX3) are composed of either group-IVB or group-VB transition
metal (M) and chalcogen atoms (X=S, Se or Te). Here, we focus on the group-IVB-based TMTCs with
M=Ti, Zr or Hf. In bulk form, crystalline structures of the TMTCs can exhibit one of two very similar
monoclinic structures, namely, ZrSe3-type and TiS3-type, or both. Both types belong to the P21/m
space group.28-30 ZrSe3, HfS3 and ZrTe3 are reported to adopt the ZrSe3-type structure, while TiS3 and
HfTe3 are reported to adopt the TiS3-type structure, and ZrS3 and HfSe3 can adopt both.29, 31 Very
recently, the ZrSe3-type variant of TiS3 has been reported as well.30 Schematic views of the TiS3-type
(Figure 1(a)) and ZrSe3-type (Figure 1(b)) TMTC structures are shown in Figure 1. The relationship
between the positional parameters (fractional coordinates) of the two types is suggested to be xA=1-
xB, yA=yB and zA=zB, where A and B stand for ZrSe3-type and TiS3-type, respectively. We can also see
that each single layer holds together via quasi-one dimensional structures that can be viewed as a
triangular prism in MX6 units along the b direction. It is worth to mention that the X atoms in the
triangular bases of the prism are not equivalent, one side of the triangle is shorter than the other
two because of the existence X-X bonds32. Indeed, MX3 can be viewed as M4+(X2)2-X2- with both X and
X2 units forming triangular prisms with M centers.

Synthesis of Low-Dimensional TMTCs

Methods of 2D layered material synthesis generally can be classified into two categories: top-down
methods, such as mechanical cleavage1, 33 and liquid-phase exfoliation34, 35; and bottom-up methods,
such as chemical vapor deposition (CVD) growth36-38 and hydrothermal synthesis39. Bulk TiS3 is a
layered material in which the interlayer interaction is dominated by vdW forces, rendering
mechanical exfoliation a feasible approach to produce 2D TiS3 sheets. The energy required to cleave
layered materials, i.e., the cleavage energy (CE), can be defined as the energy to separate a layered
crystal into two parts along a basal plane. Although little experimental data is available in the early
stage of low-dimensional TMTC research, a CE of about 0.20 J/m2 is theoretically predicted for TiS340,

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which is actually lower than that of graphite (0.36 J/m2 from experiment41 and 0.32 J/m2 from
calculation40). Thus, in principle, mechanical exfoliation of TiS3 is expected to be easier than that of
graphite from the energetic point of view.

Thus far, few-layer TiS3 sheets and nanoribbons have been successfully peeled off from bulk TiS3 via
mechanical cleavage, using scotch tape.42-44 Since bulk TMTCs are currently not available in the
market, and they have to be synthesized in the laboratory first before the mechanical exfoliation
experiments. It has been established that bulk TiS3 can be synthesized through direct reaction
between titanium and sulfur.28, 29, 42, 43, 45 In synthesis, for example, titanium disks are vacuum sealed
in an ampule with excess sulfur to prevent the formation of TiS2, while the system is heated to a
designated temperature. The temperature should be below 632 ˚C, the critical temperature of TiS3
decomposition to TiS2. It is also reported that the morphology of the synthesized TiS3 strongly
depends on the growth temperature. The 500 ˚C grown sample contains only belt-like nanoribbons
with different sizes (see Figure 2 (a)-(b)), while nanosheets are seen in the 400 ˚C grown sample (see
Figure 2 (c)-(d)).42 The mechanical cleavage samples are of high quality and high purity, suitable for
both fundamental characterization study and device fabrication.42-44 However, the mechanical
cleavage method is unsuitable for scalable production, only limited to use in the laboratory. Also,
mechanical cleavage method is difficult for controlling the thickness and size of the exfoliated
sample, specifically for TMTCs which entail quisi-1D structure and can easily break along the b
direction into nanoribbons.43

Liquid-phase exfoliation methods have been proven to be quite effective for producing large
quantity and large-size 2D nanosheets such as graphene, TMDCs and h-BN sheets.34, 35 Considering
similar layered structures of TMTCs as TMDCs, the liquid-phase synthesis of 2D TMTCs is likely an
effective method for producing large quantity and large-size 2D nanosheets as well. Although few
work has been reported, we noticed that Xie et al. has successfully exfoliated ultrathin 2D ZrS3
nanosheets using the liquid phase method.46 They pretreated the ZrS3 bulk with n-propylamine by
stirring for 30 min and then heated the sample to 120 ˚C for 3 days. Thereafter, the pretreated
sample was cooled to room temperature and mixed with proper amount of absolute ethanol and 1-
cyclohexyl-2-pyrrolidinone for ultrasound treatment. The exfoliated samples are shown in Figure 2
(e)-(f). Ion intercalation is another potentially viable method to exfoliate 2D TMTCs in liquid. Indeed,
lithium intercalation of TMTCs through reaction with n-butyllithium has already been reported forty
years ago.47, 48 Three lithium atoms were found to be incorporated into MX3 unit, yielding Li3MX3
compounds without destroying the structural integrity. However, it is possible that the lithium atoms
are incorporated not only into the vdW interlayer spacing but also in the area of adjacent MX3
prisms along the a direction, which may yield nanoribbons.

To enable commercial-level large-scale device production based on low-dimensional TMTCs, wafer-

scale synthesis methods such as CVD on substrates or epitaxial growth on insulating substrates are
yet be developed. Proper reagents and suitable substrates have to be experimented first for the
implementation of both direct chemical synthesis techniques.

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Facile bottom-up growth techniques is yet to be demonstrated to realize the true potential of 2D
layered TMTC materials; and future chemical synthesis techniques may draw inspiration from the
techniques already developed for TMDCs, such as CVD growth.

Electronic and Mechanical Properties of 2D and 1D TMTCs

Electronic structures

The literature on electronic structures of 2D and 1D TMTCs are rather limited compared with those
on bulk TMTCs. At present, theoretical computations are ahead of experiments. As shown in Figure
3, TiS3 is predicted, based on the first-principles computation, to undergo a transition from an
indirect band-gap semiconductor in bulk phase to a direct band-gap semiconductor in 2D monolayer
structure,40 akin to the indirect-to-direct band-gap transition in certain TMDCs. Both the conduction
band minimum (CBM) and valence band maximum (VBM) are located at the Γ point, yielding a band
gap of ~1.06 eV (at the hybrid Heyd-Scuseria-Ernzerhof (HSE06)49 level of theory) for the TiS3
monolayer. This band gap is narrower than those of typical 2D TMDCs (1.1 – 2.5 eV), but wider than
those of the semimetallic graphene and silicene, giving an ON/OFF ratio up to 104 with low
dimensional TiS3.42-44 Theoretically, the deformation potential (DP) theory can be adopted to
compute carrier mobility of the TiS3 monolayer. Note that in a perfect inorganic crystal, the coherent
wavelength of thermally activated electrons/holes at room temperature is typically much longer
than the lattice constant, and the scattering at low energy regime is dominated by the electron-
acoustic phonon coupling, which can be efficiently treated by the DP theory.50, 51 Based on the latter
theory, the in-plane carrier mobility is predicted to be highly anisotropic due to the strong structural
anisotropy of TiS3 monolayer. The computed in-plane electron mobility is about 104 cm2/V/s along
the b direction, much higher than that of MoS2 monolayer, whereas the hole mobility is about two
orders of magnitude lower than that of the electron one.40 It is noted that the measured carrier
mobility of 2D TiS3 (~70 cm2/V/s) is much lower than the theoretical one. This difference can be
attributed to a) the existence of localized defect states due to the sulfur vacancies in the samples,42,
52
as in the case of 2D MoS2 for which the carrier mobility can be significantly enhanced through
sulfur vacancy repair53; b) the multilayer samples, and (c) the substrate in the experiments. Density
functional theory computations at HSE06 level with considering the spin-orbit coupling (SOC) show
that TiS3 monolayer is the only TMTC which possesses a direct band gap among all group-IVB TMTCs.
In other words, TiTe3, ZrTe3 and HfTe3 monolayers are predicted to be metallic while TiSe3, ZrS3,
ZrSe3, HfS3 and HfSe3 monolayers are predicted to be indirect band-gap semiconductors with their
band gaps ranging from 0.57 to 1.92 eV computed at the HSE06 level.53, 54 Note that the band gap
decreases with increasing the size of chalcogen atoms. Moreover, compared with their bulk
counterparts, the indirect band gap of corresponding monolayer is smaller. These predicted band
gaps are summarized in Table 1. Another interesting feature predicted based on the effective mass

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calculations is that for TiS3 and ZrS3 monolayers, n-type is preferred along the b direction while p-
type is preferred along the a direction, but for TiSe3 and ZrSe3, p-type is preferred along the b
direction while n-type is preferred along the a direction, showing a flip of carrier polarity.53 From the
experiment, a direct band gap of about 1 eV is reported for TiS3 nanosheets and nanoribbons.42 A
more recent study shows values of 1.2 eV, 1.07 eV and 130 meV for TiS3 nanoribbons (30-130 layers
thick) based on scanning tunneling spectroscopy and photoelectrochemical measurements, and 1.15
eV, 1.05 eV and 100 meV from random phase approximation and Bethe-Salpeter equation
calculations.55 Systematic experimental measurements of the band dispersion of 2D and 1D TMTCs
are under way, for which techniques such as angle-resolved photoelectron spectroscopy are
required to offer detailed information about the band dispersions of low-dimensional TMTCs.
Among all group-IVB TMTC monolayers, the stability TiS3 monolayer has been examined theoretically
using both molecular dynamics simulation and phonon-spectrum calculation.40 The synthesis of 2D
TiS3 has also been reported.42 Phonon-spectrum calculations also show no imaginary modes in the
case of HfS3 and HfSe3 monolayers54, indicating dynamical stability of both monolayers. The stability
of 2D ZrS3 has been also confirmed experimentally since few-layer ZrS3 nanosheets have been
successfully synthesized46. For other 2D TMTCs, their dynamical stability is yet to confirmed from
either phonon-spectrum calculations or experiments.

Defects are likely to exist in synthesized low-dimensional TMTCs, as in the case of 2D TiS3. It has
been reported that sulfur vacancies exist in the nanosheets synthesized at 400 ˚C, giving a localized
defect state below the Fermi level.42 Besides sulfur vacancy, other possible vacancies such as Ti, TiS
and double S vacancies have been also investigated theoretically.52 It was found that single S vacancy
is the most probable among various vacancies considered.

As mentioned previously, the quasi-1D nature of 2D TMTCs makes the structure break into 1D
nanoribbons along the b direction very likely during the mechanical exfoliation43 or lithium
intercalation47, 48, and 1D nanoribbons may possess some distinctive properties as compared to their
2D counterparts56. Thus it is also important to gain a thorough understanding of the electronic
structures of 1D TMTCs nanoribbons. Thus far, only 1D TiS3 nanoribbons have been theoretically
investigated.57 Although in principle two type of ribbon edges can be created for theoretical
computations, i.e., one with periodicity along the a direction and another in the b direction,
hereafter, we only focus on the ribbons with periodicity in b direction because the Ti-S bond
strength is much stronger along the b direction than along the a direction. As shown in Figure 4 (a),
the computed band gaps and band edges of 1D TiS3 nanoribbons are nearly independent of the
width of the nanoribbons. Moreover, the carrier mobility of 1D nanoribbons is predicted to increase
with the width of ribbon, and the electron mobility is about one order of magnitude higher than the
hole one, retaining the n-type property of 2D TiS3.57

Although some progress has been made in our understanding of the low-dimensional TMTCs, more
studies are still needed to achieve deeper understanding of this new class of 2D materials. For
example, the layer-stacking order effect which can significantly influence the electronic properties

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of multilayers of graphene58 and phosphorene22,59 is yet to be investigated for 2D TMTCs.
Furthermore, theoretical study of electronic properties of the vdW stacking layers of different 2D
TMTCs, and heterogeneous stacking of 2D TMTCs with other 2D materials such as graphene, BN,
TMDCs, and phosphorene, will be an active area of research to complement future experimental
device design.

Mechanical Properties

Knowledge of mechanical properties of 2D TMTCs is also of great value to the assessment of

potential applications in flexible electronics and nanoelectromechanical systems. The structural
anisotropy of 2D TMTCs implies anisotropic mechanical response with respect to uniaxial loading
along the a and b directions. First-principles calculations predict that TiS3 monolayer can sustain
tensile strains up to ~20% along the b direction and ~10% along the a direction. The in-plane
stiffness of TiS3 monolayer is highly anisotropic, with Ca = 83.33 N/m, and Cb = 133.56 N/m, the
Poisson’s ratio = 0.11 along a, and 0.18 along b, while the ultimate strength is predicted to be 4.45
GPa along a and 18.32 GPa along b.60 The calculated in-plane Young’s modulus is 95.72 GPa along a,
and 153.41 GPa along b. Both are considerably lower than those of graphene (about 1T Pa61) and
MoS2 (~270 GPa62), suggesting superior flexibility of TiS3 monolayer, a feature crucial for
applications in flexible electronic devices.

The relatively high critical strain (~20% along b and ~10% along a) of the TiS3 monolayer suggests the
likelihood of strain engineering of the electronic structure of TiS3. Indeed, theoretical computations
show that tensile strain can effectively modify the band structures of 2D TMTCs. As shown in Figure
5, the MS3 monolayers show marked anisotropic response to the tensile strain. Overall the band gap
increases with the increase of strain along the b direction but decreases along the a direction. More
specifically, ZrS3 and HfS3 monolayers can undergo an indirect-to-direct band-gap transition under a
uniaxial strain along the b direction (4% and 2% for ZrS3 and HfS3) or a biaxial strain (2% for both ZrS3
and HfS3). For ZrSe3 and HfSe3 monolayers, the indirect band gap increases monotonously with the
increase of either uniaxial or biaxial strain. At the uniaxial strain of 4% and 6% along the b direction,
metallic ZrTe3 and HfTe3 monolayers transform into indirect band-gap semiconductors.54 First-
principles computations have been also performed to investigate strain engineering of electronic
structures of TiS3 nanoribbons. It is found that both band edge and band gaps are very sensitive to
the uniaxial strain. As shown in Figure 4 (b), the band gaps of TiS3 nanoribbons with widths of 4-10
all increase monotonously with the increase of strain, from ~0.3 eV at zero strain to ~0.9 eV at the
strain of 10%. Furthermore, ultra-narrow ribbon with a width of 4 is predicted to retain the direct
gap feature within the range of strain of 0 to 10%. Other ribbons with width > 4 undergo a direct-to-
indirect gap transition at certain finite strain, e.g., 10%, 6% and 4% for width of 6, 8 and 10,

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respectively. A representative example of width 8 ribbon is shown in Figure 4 (c). Indeed, both CBM
and VBM are located at the unstrained region of the ribbon (see figure 4 (d)).57

Applications

Transistors. Development of future nanoscale transistors with higher performance and lower power
consumption for digital electronics posts a great challenge to low-dimensional material science. The
predicted direct band gap of ~1 eV as well as high mobility (~104 cm2/V/s) endows 2D TiS3 sheets a
desirable candidate for FET applications.40 To date, both 1D TiS3 nanoribbon and 2D TiS3 nanosheet
based transistors have been demonstrated (see Figure 6).42-44 For the FETs based on as synthesized
TiS3 nanosheets show a polarized feature of mobility, i.e., 80 cm2/V/s along b and 40 cm2/V/s along a
with a ON/OFF ratio about 5.42 The existence of sulfur vacancies in the nanosheet samples could be a
reason for the low mobility compared to the predicted one. If so, the mobility can be further
enhanced by reducing the number of sulfur vacancies and improving the quality of the sample. For
the TiS3 nanoribbons, theoretical calculations predict the width dependent carrier mobility with
values up to several thousands of cm2/V/s, about an order of magnitude lower than that of the 2D
monolayer.57 For FETs based on synthesized TiS3 nanoribbons, the carrier mobility has been
enhanced from 1.4 - 2.6 cm2/V/s44 to 37 - 43 cm2/V/s by improving the sample quality and by
modifying the dielectric environment.43 As shown in Figure 6(c)-(e), the carrier mobility of as-
synthesized TiS3 nanoribbons is 18-23 cm2/V/s, and the ON/OFF ratio is up to 300. With atomic layer
deposition of alumia (Al2O3) on TiS3 FETs, the carrier mobility is increased up to 37-43 cm2/V/s, and
the ON/OFF ratio is increased up to 7000.43

Photodetectors and Photocatalysis. Optically active low-dimensional materials suitable for

optoelectronics are also highly desired. Low-dimensional TiS3 possesses a direct band gap about 1
eV,40, 42, 44, 57 close to the band gap of bulk silicon. So low-dimensional TiS3 may be a potential
candidate for replacing silicon in certain optoelectronic applications. The fabricated transistors
based on few-layer TiS3 nanoribbons show an ultrahigh photoresponse of 2910 A/W, several orders
of magnitude higher than the intrinsic graphene photodetectors and much higher than MoS2 based
photodetectors (up to 880 A/W).44 The device responds to wavelengths across visible spectrum and
present rise/fall time of about 4/9 ms, and a frequency up to 1000 Hz.44 Photodetector based on
ZrS3, ZrSe3 and HfSe3 nanobelts have also been reported,63-65 Flexible ZrS3 nanobelt is reported to
exhibit good response from ultraviolet (UV) to near-infrared (NIR) with a photoswitch current ratio
(PCR) of 3.563. By transferring the ZrS3 nanobelts to SiO2/Si substrates, the PCR can be further
improved to 210 under 405-nm light illumination of 5.57 mW/cm2 at a bias of 1 V.65 The
photoresponse time for ZrSe3 and HfSe3 based photodetector are reported to be less than 0.4 s, and
PCRs are of 1.97 and 2.2, respectively.64 All these devices show stability and durability.

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Collecting and utilizing solar energy in an efficient fashion is an important way to meet the increasing
societal demand for energy. TiS3 nanoribbons have been used as photoanode for hydrogen
generation.66 Energy photoconversion efficiencies up to 7% have been predicted. Moreover, ZrS3
ultrathin nanosheets have been reported to be a good photoanode material at various PH values, for
which the onset overpotentials are 610 mV, 420 mV and 280 mV, while the Tafel slopes are 102
mV/decades, 74 mV/decades and 51 mV/decades, respectively, for PH = 6.9, 9.2 and 13.46

Other Applications. The electrochemical characteristics of bulk TMTCs in rechargeable lithium

battery have been investigated for more than thirty years67. It was found that although three Li
atoms can be intercalated into TiS3, the intercalation and deintercalation (correspond to charge and
discharge) is marginally reversible.67 Theoretical calculations showed feasibility of using monolayer
TiS3 in Li- and Na-batteries. The diffusion of Li and Na ions are direction dependent, 0.44 eV and 0.35
eV along b and a direction, respectively, for Li, and 0.32 eV and 0.26 eV for Na. The bulk TiS3 is
predicted to be capable of accommodating 2 Li/Na, slightly higher than that of TiS3 monolayer of 1.5
Li/Na, corresponding to 339 and 282 mA·h·g-1 for Li and Na storage, respectively.68

Summary and Outlook

As a new member in the family of 2D layered materials, TMTCs offer similar diversity as that of
TMDCs and yet display many outstanding properties as or better than other prominent 2D materials.
For example, like phosphorene, TiS3 monolayer exhibits both a desired direct band gap and relatively
high carrier mobility for high performance electronic devices, and yet TiS3 is much more chemically
stable and free from the easy-decomposition problem in phosphorene. Applications of 2D and 1D
TMTCs in photodetectors and photocatalysis have been demonstrated. Although the realization of
few-layer TMTC 1D nanoribbons and 2D sheets occurs only very recently, these low-dimensional
materials show great potential for many applications. Compared with TMDCs, TMTCs have
chalcogen dimers on their edge surface plane, which make TMTCs more reactive and thus much
easier to be functionalized than TMDCs. The increased ease of functionalization will offer more
synthetic opportunities for engineering new functional low-dimensional TMTC materials. Moreover,
the unique edge surface structure of TMTCs may also be exploited for gas sensing or detection. The
in-plane structural, electronic, mechanical and optical anisotropic properties have yet to be utilized
for device design. The predicted relatively high electron mobility of TiS3 monolayers and ribbons may
be also utilized to build p-n junctions with other p-type 2D materials, such as phosphorene for
electric and photoelectric applications. In fundamental science aspects, the low-dimensional TMTC
materials may offer good platforms to study charge density wave. For example, nonlinear
conductivity in TiS3 has been reported, indicating possible transition to collective states for
electons69. In closing, the intrinsic novel properties of low-dimensional TMTCs create new
opportunities for device applications at nanoscale. In view of the fact that low-dimensional TMTCs
have been isolated in the laboratory, new breakthroughs in material synthesis, new discoveries in
physical and chemical properties, and new device development with higher performance are
expected in the near future.

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ACKNOWLEDGEMENTS

This work was supported by the National Science Foundation (NSF) through the Nebraska Materials
Research Science and Engineering Center (MRSEC) (grant No. DMR-1420645), grants from the UNL
Nebraska Center for Energy Science Research and USTC, and University of Nebraska Holland
Computing Center.

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Figure captions

Figure 1: Representative crystal structures of (a) TiS3-type and (b) ZrSe3-type transition metal
trichalcogenides.

Figure 2: (a)-(d) Optical images of TiS3 sheets and nanoribbons exfoliated from TiS3 films synthesized
at 400 ˚C and 500 ˚C with different thickness. (a) 13 nm nanoribbon, (b) 22 nm nanoribbon, (c) 4 nm
nanosheet, and (d) 17 nm nanosheet. (e) TEM image of an individual ZrS3 ultrathin sheet, (f) HRTEM
image of the basal surface of the ZrS3 ultrathin sheets and the corresponding FFT pattern. (a)-(d)
Reproduced from ref 42 with permission from Wiely. (e)-(f) Reproduced from ref 46with permission
from the Royal Society of Chemistry.

Figure 3: (a) Computed electronic band structure and density of states of the TiS3 monolayer at the
HSE06 level, (b) computed band structure of bulk TiS3 at the HSE06 level. Reproduced from ref 40
with permission from Wiely.

Figure 4: (a) HSE06 and PBE band gaps of TiS3 nanoribbons versus ribbon widths, (b) computed band
gap of TiS3 nanoribbons versus tensile strain, (c) computed band structure of TiS3 nanoribbon with
width 8 at tensile strain of 0%, 4% and 8%, respectively, (d) the CBM and VBM charge density of 8%
strained TiS3 nanoribbon with width4. Figure (a)-(d) adapted with permission from ref 57.
Copyrighted by the American Physical Society.

Figure 5. Computed band gaps of (a) ZrS3, (b) ZrSe3, (c) ZrTe3, (d) TiS3, (e) HfS3, (f) HfSe3 and (g) HfTe3
monolayers versus the biaxial or uniaxial tensile strain in a range of 0% - 8%. Red lines refer to
uniaxial strain along the a direction, black lines refer to uniaxial strain along the b direction, and blue
lines refer to the biaxial strain. Γ–Γ denotes the direct band gap, whereas Γ–A, Γ–B and Γ–I denote
the indirect band gap. Reproduced from ref. 54 published by The Royal Society of Chemistry.

Figure 6. (a) Scheme of a TiS3 based device on a SiO2/Si substrate. (b) SEM image of a typical TiS3 FET.
(c) Conductivity-gate voltage dependencies of four TiS3 FETs. (d)-(e) Comparison of the conductivity-
gate voltage dependencies of TiS3 FET device shown in (b) before and after ALD of Al2O3 .
Reproduced from ref. 43 published by The Royal Society of Chemistry.

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Tables

Table 1. A summary of computed band gaps of bulk and 2D monolayer group IVB TMTCs. Unlisted
bulk and 2D monolayer TiTe3, ZrTe3 and HfTe3 are metallic, where I and D in the parenthesis refer
to indirect and direct gap semiconductors, respectively.

TiS3 TiSe3 ZrS3 ZrSe3 HfS3 HfSe3

Bulk 1.02 (I)a,b 0.21 (I)b 1.83 (I)b 0.75 (I)b 0.59 (I)c 1.07 (I)c

1.87 (I)c 0.68 (I)c

ML 1.06 (D)a,b 0.57 (I)b 1.90 (I)b 1.17 (I)b 1.94 (I)c 0.80 (I)c

1.08 (D)c 1.92 (I)c 0.92 (I)c

Note: a from ref. 40, b from ref. 53, c from ref. 54

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Tuning the electronic properties of transition­
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