Two-dimensional Transition Metal Dichalcogenides Research Articles

Helicity-Sensitive Terahertz Detection in Monolayer 1T'-WTe2.

Valleytronics, identified as electronic properties of the energy band extrema in momentum space, has been intensively revived following the emergence of two-dimensional transition metal dichalcogenides (TMDCs) as their valley information can be controlled and probed through the spin angular momentum of light. Previous optical investigations of valleytronics have been limited to the visible/near-infrared spectral regime through which the carriers of most TMDCs can be excited. Monolayer 1T'-WTe2 with broken time-reversal symmetry provides a fertile platform to study the long-wavelength photonic properties in different valleys. Here, we employed a circularly polarized terahertz (THz) laser to selectively excite the valley of monolayer 1T'-WTe2 and demonstrate that the helicity-dependent photoresponse is generated via the photogalvanic effect (PGE). We also observed that the photocurrent is controlled by circular polarization and the external electric field. Because of the tunable Berry curvature dipole derived from the nontrivial wave functions near the inverted gap edge in monolayer WTe2, the bandgap can be tuned efficiently. Our results provide a versatile venue for controlling, detecting, and processing valleytronics and applications in on-chip THz imaging and quantum information processing.

Magnetic proximity effect on the spin-valley coupling in two-dimensional Cr2Ge2Te6/2H-TMD van der Waals heterostructures

Two-dimensional (2D) transition metal dichalcogenides with 2H-phases, as a unique platform of valleytronics, display valley polarization and the well-known anomalous valley Hall effect when stacking with 2D magnetic substrates. In this study, we employ first-principles calculations to investigate the magnetic states, band structures, and magnetic proximity-dependent valley properties of 2D van der Waals heterostructures Cr2Ge2Te6/2H-MX2 (M = Mo, W, and X = S, Se, Te). Our findings reveal that the heterostructures possess stacking-dependent spontaneous valley polarization as well as pristine perpendicular magnetic anisotropy. Additionally, the Berry curvature and circular polarization demonstrate the presence of spin–momentum coupling characteristics, while the calculated non-zero Hall voltage indicates that the anomalous valley Hall effect can be achieved in valley-polarized systems. Furthermore, due to the strain effect and the electronic polarization at the interface, Cr2Ge2Te6/2H-MX2 heterostructures undergo the transition from semiconductors to semimetals upon substitution of early chalcogen elements. These calculations provide valuable insights for practical applications of valleytronics in 2D van der Waals heterostructure systems.

Photoluminescence Enhancement and Carrier Dynamics of Charged Biexciton in Monolayer WS2 Coupled with Plasmonic Nanocavity

Monolayer two-dimensional transition metal dichalcogenide (TMD)-based materials have become one of the ideal platforms for the study of multibody interactions due to their rich excitonic complexes. The coupling between optical nanocavity and material has become an important means for manipulating the optical properties of materials, but there are few studies on the coupling of nanocavities and the multi-body effect in materials. In this study, we investigate the optical properties of silver nanodisk (Ag ND) arrays covering a monolayer WS2. In the experimental sample, we observed a ~114.3-fold photoluminescence enhancement of charged biexciton in the heterostructure region, as compared to the monolayer WS2 region, a value which is much higher than those for exciton (~2.2-fold) and trion (~16.4-fold), a finding which is attributed to the Fano resonant coupling between monolayer WS2 and the Ag ND. By means of time-resolved spectroscopy, we studied the carrier dynamics in the hybrid system. Our findings reveal that resonant coupling promotes the formation and radiation recombination processes of the charged biexciton, significantly reducing the radiative recombination lifetime by ~15-fold, which is much higher than the measurement in exciton (~2-fold). Our results provide an opportunity to understand the multibody physics of coupling with nanocavities, which could facilitate the application of multi-body excitons in the fields of light-emitting devices and lasers, etc.

Near-field coupling of interlayer excitons in MoSe2/WSe2 heterobilayers to surface plasmon polaritons.

Two-dimensional (2D) transition metal dichalcogenides have emerged as promising quantum functional blocks benefitting from their unique combination of spin, valley, and layer degrees of freedom, particularly for the tremendous flexibility of moiré superlattices formed by van der Waals stacking. These degrees of freedom coupled with the enhanced Coulomb interaction in 2D structures allow excitons to serve as on-chip information carriers. However, excitons are spatially circumscribed due to their low mobility and limited lifetime. One way to overcome these limitations is through the coupling of excitons with surface plasmon polaritons (SPPs), which facilitates an interaction between remote quantum states. Here, we showcase the successful coupling of SPPs with interlayer excitons in molybdenum diselenide/tungsten diselenide heterobilayers. Our results indicate that the valley polarization can be efficiently transferred to SPPs, enabling preservation of polarization information even after propagating tens of micrometers.

Room-temperature quantum emission from interface excitons in mixed-dimensional heterostructures

The development of van der Waals heterostructures has introduced unconventional phenomena that emerge at atomically precise interfaces. For example, interlayer excitons in two-dimensional transition metal dichalcogenides show intriguing optical properties at low temperatures. Here we report on room-temperature observation of interface excitons in mixed-dimensional heterostructures consisting of two-dimensional tungsten diselenide and one-dimensional carbon nanotubes. Bright emission peaks originating from the interface are identified, spanning a broad energy range within the telecommunication wavelengths. The effect of band alignment is investigated by systematically varying the nanotube bandgap, and we assign the new peaks to interface excitons as they only appear in type-II heterostructures. Room-temperature localization of low-energy interface excitons is indicated by extended lifetimes as well as small excitation saturation powers, and photon correlation measurements confirm antibunching. With mixed-dimensional van der Waals heterostructures where band alignment can be engineered, new opportunities for quantum photonics are envisioned.

Environmental-Friendly Ag2S QD-Multilayer MoSe2 van Der Waals Heterostructure for High-Performance Broadband Photodetection.

Broadband photodetectors have drawn intensive attention owing to their wide application prospects in optical communication, imaging, astronomy, and so on. Two-dimensional transition-metal dichalcogenides (TMDs) are considered as highly potential candidates for photodetection applications, benefiting from their excellent photoelectric properties. However, most of the photodetectors based on TMDs suffer from low performance in the near-infrared (NIR) region due to the weak optical absorption efficiency near their absorption band edge, which severely constrains their usage for broadband optoelectronics. Here, by taking advantage of the high absorption coefficient and environment-friendly property of Ag2S quantum dots (QDs), the hybrid of multilayer MoSe2/Ag2S QDs is demonstrated with a high-performance broadband photodetection capability (532-1270 nm). The favorable energy band alignment of MoSe2/Ag2S QDs facilitates effective separation and collection of photogenerated carriers, and the heterostructure device exhibits significant enhancement of performance compared to the bare MoSe2 device. High responsivity, detectivity, and external quantum efficiency of 25.5 A/W, 1.45 × 1011 Jones, and 1070% are obtained at a low working voltage of 1 V under 980 nm illumination. The responsivity of the device can reach up to 1.2 A/W at 1270 nm wavelength, which is competitive to the commercial NIR photodetectors. Meanwhile, broadband imaging capability is demonstrated. Our work may open up a facile and eco-friendly approach to construct high-performance broadband photodetectors for next-generation compact optoelectronic applications.

High-Performance Contact-Doped WSe2 Transistors Using TaSe2 Electrodes.

Two-dimensional (2D) transitional metal dichalcogenides (TMDs) have garnered significant attention due to their potential for next-generation electronics, which require device scaling. However, the performance of TMD-based field-effect transistors (FETs) is greatly limited by the contact resistance. This study develops an effective strategy to optimize the contact resistance of WSe2 FETs by combining contact doping and 2D metallic electrode materials. The contact regions were doped using a laser, and the metallic TaSe2 flakes were stacked on doped WSe2 as electrodes. Doping the contact areas decreases the depletion width, while introducing the TaSe2 contact results in a lower Schottky barrier. This method significantly improves the electrical performance of the WSe2 FETs. The doped WSe2/TaSe2 contact exhibits an ultralow Schottky barrier height of 65 meV and a contact resistance of 11 kΩ·μm, which is a 50-fold reduction compared to the conventional Cr/Au contact. Our method offers a way on fabricating high-performance 2D FETs.

Transient Nanoscopy of Exciton Dynamics in 2D Transition Metal Dichalcogenides.

The electronic and optical properties of two-dimensional (2D) transition metal dichalcogenides are dominated by strong excitonic resonances. Exciton dynamics plays a critical role in the functionality and performance of many miniaturized 2D optoelectronic devices; however, the measurement of nanoscale excitonic responses remains challenging. Here, a near-field transient nanoscopy is reported to probe exciton dynamics beyond the diffraction limit. Exciton recombination and exciton-exciton annihilation processes in monolayer and bilayer MoS2 are studied as the proof-of-concept demonstration. Moreover, with the capability to access local sites, intriguing exciton dynamics near the monolayer-bilayer interface and at the MoS2 nano-wrinkles are resolved. Such nanoscale resolution highlights the potential of this transient nanoscopy for fundamental investigation of exciton physics and further optimization of functional devices. This article is protected by copyright. All rights reserved.

High-Performance Broadband Image Sensing Photodetector Based on MnTe/WS2 van der Waals Epitaxial Heterostructures.

Two-dimensional transition metal dichalcogenide (TMDC) heterostructure is receiving considerable attention due to its novel electronic, optoelectronic, and spintronic devices with design-oriented and functional features. However, direct design and synthesis of high-quality TMDC/MnTe heterostructures remain difficult, which severely impede further investigations of semiconductor/magnetic semiconductor devices. Herein, the synthesis of high-quality vertically stacked WS2/MnTe heterostructures is realized via a two-step chemical vapor deposition method. Raman, photoluminescence, and scanning transmission electron microscopy characterizations reveal the high-quality and atomically sharp interfaces of the WS2/MnTe heterostructure. WS2/MnTe-based van der Waals field effect transistors demonstrate high rectification behavior with rectification ratio up to 106, as well as a typical p-n electrical transport characteristic. Notably, the fabricated WS2/MnTe photodetector exhibits sensitive and broadband photoresponse ranging from UV to NIR with a maximum responsivity of 1.2 × 103 A/W, a high external quantum efficiency of 2.7 × 105%, and fast photoresponse time of ∼50 ms. Moreover, WS2/MnTe heterostructure photodetectors possess a broadband image sensing capability at room temperature, suggesting potential applications in next-generation high-performance and broadband image sensing photodetectors.

Wafer-scale synthesis of 2D PtTe2 thin films with high spin–orbit torque efficiency

Spintronic devices have become a crucial technology for overcoming the power consumption bottleneck in integrated circuits, due to their low power consumption, high-speed processing capability. Two-dimensional materials offer potential for performance enhancement and device miniaturization in spintronics because of their unique electronic and spin properties. Specifically, two-dimensional transition metal dichalcogenides (2D TMDs) are favored in the field of spintronics for their strong spin–orbit coupling effects, enabling effective control over the electron spin state. However, the preparation techniques for 2D TMDs are still in the exploratory stage. In this work, we explore novel preparation method combining magnetron sputtering and molecular beam epitaxy, leading to wafer-scale high-quality monocrystalline PtTe2 thin films. Further, Spin-Orbit Torque (SOT) efficiency is investigated in PtTe2-based heterostructures, which reveals a significant spin Hall angle of over 0.094. Our work provides a new way to fabricate the wafer-scale PtTe2 thin films and confirms a large SOT efficiency, which indicates the great promise for spintronic applications.

A comparative study on 2D materials with native high-[formula omitted] oxides for sub-10 nm transistors

Two-dimensional (2D) transition metal dichalcogenides (TMDs) with native high-κ oxides have presented a new avenue towards the development of next-generation ultra-scaled field-effect transistors (FETs). These materials have been experimentally shown to form a natively compatible oxide layer with a high dielectric constant, which can help scale down both the transistor size and the supply voltage. We present a material and device performance study into the use of several of these materials – namely HfS2, HfSe2, ZrS2, ZrSe2 – as channels in sub-10 nm FETs. All four materials exhibit isotropic transport at 10 nm channel length with ON currents over 1000 μA/μm but show anisotropic transport and degraded ON currents at 5 nm channel length. In general, the sulfide family excels in terms of subthreshold characteristics at sub-10 nm channel lengths. HfS2, in particular, surpasses all the other materials in terms of ON currents and subthreshold swing (SS), allowing it to also achieve excellent intrinsic performance. We have identified HfS2 as a superior material within this TMD family for sub-10 nm FETs.

A Molecular Coordination Strategy for Regulating the Interface of MoS2 Field Effect Transistors.

Chemically modifying monolayer two-dimensional transition metal dichalcogenides (TMDs) with organic molecules provides a wide range of possibilities to regulate the electronic and optoelectronic performance of both materials and devices. However, it remains challenging to chemically attach organic molecules to monolayer TMDs without damaging their crystal structures. Herein, we show that the Mo atoms of monolayer MoS2 (1L-MoS2) in defect states can coordinate with both catechol and 1,10-phenanthroline (Phen) groups, affording a facile route to chemically modifying 1L-MoS2. Through the design of two isomeric molecules (LA2 and LA5) comprising catechol and Phen groups, we show that attaching organic molecules to Mo atoms via coordinative bonds has no negative effect on the crystal structure of 1L-MoS2. Both theoretical calculation and experiment results indicate that the coordinative strategy is beneficial for (i) repairing sulfur vacancies and passivating defects; (ii) achieving a long-term and stable n-doping effect; and (iii) facilitating the electron transfer. Field effect transistors (FETs) based on the coordinatively modified 1L-MoS2 show high electron mobilities up to 120.3 cm2 V-1 s-1 with impressive current on/off ratios over 109. Our results indicate that coordinatively attaching catechol- or Phen-bearing molecules may be a general method for the nondestructive modification of TMDs.

Theory of interlayer exciton dynamics in two-dimensional transition metal dichalcogenide heterolayers under the influence of strain reconstruction and disorder

Theory of interlayer exciton dynamics in two-dimensional transition metal dichalcogenide heterolayers under the influence of strain reconstruction and disorder

NaCl-assisted chemical vapor deposition growth of MoSe2 and MoSe2/h-BN heterostructure

As a typical two-dimensional (2D) transition metal dichalcogenides (TMDCs), MoSe2 has attracted lots of interest due to its electronic and optical properties in recent years. The controllable synthesis of 2D MoSe2 and its heterostructure is of considerable importance for achieving diverse applications. Herein, we realized the controlled growth of MoSe2 by atmospheric pressure chemical vapor deposition (APCVD) method through using NaCl as the promoter. Raman and photoluminescence (PL) spectroscopy have been used to investigate the optical properties of MoSe2 domains with different layers. The dependence of structures on synthetic parameter is systematically investigated by tuning the growth conditions. On this basis, the monolayer MoSe2 was constructed on CVD-grown hexagonal boron nitride (h-BN) by an all-CVD approach. Detailed characterizations indicate that MoSe2 deposited on h-BN exhibits improved optical properties as compared to those on SiO2/Si. Our results could enrich the understanding for growth of TMDCs, advocating further investigation of their intrinsic properties and a variety of device applications.

Enhancing dielectric passivation on monolayer WS2 via a sacrificial graphene oxide seeding layer

The full utilization of two-dimensional transition metal dichalcogenides (2D TMDCs) faces several challenges, among which is realizing uniform material deposition on the 2D surface. Typical strategies to enable material growth lead to a poor interface quality, degrading the 2D TMDC’s properties. In this work, a sacrificial, graphene oxide-based seeding layer is used (1) as passivation layer, protecting the underlying 2D TMDC and (2) as nucleation layer, enabling uniform material growth. Graphene is transferred on monolayer WS2, establishing a high-quality van der Waals interface. After transfer, the polymeric residues on graphene are cleaned via a combination of wet- and dry treatments and functionalized via dry UV/O3 oxidation. The rate of graphene oxidation is shown to be substrate dependent, which is explained by UV light-induced ultrafast charge transfer between the graphene and WS2 monolayer. The carbon-oxygen functionalities serve as nucleation sites in a subsequent HfO2 ALD process, achieving more uniform dielectric growth and faster layer closure compared to direct deposition. The graphene-based nucleation- / passivation approach offers adaptability, allowing for tailored surface chemistry to enable any alternative material growth, while maintaining a prefect van der Waals interface.

Exciton Dynamics of TiOPc/WSe2 Heterostructure.

The van der Waals (vdW) heterostructures composed of two-dimensional (2D) transition metal dichalcogenides (TMDs) and organic semiconductors demonstrate numerous compelling optoelectronic properties. However, the influence of the vdW epitaxial effect and temperature on the optoelectronic properties and interface exciton dynamics of heterostructures remains unclear. This study systematically investigates the fluorescence properties of TiOPc/WSe2 heterostructure. Comprehensive spectral characterization elucidates that the emission behavior of the TiOPc/WSe2 heterostructure arises from charge/energy transfer at the heterostructure interfaces and the structural ordering of the organic layer on the 2D monolayer WSe2 induced by vdW epitaxy. The interface exciton dynamic features probed by ultrafast transient spectroscopy reveal that the face-to-face molecular stacking configuration of TiOPc exhibits ultrafast exciton dynamics. In particular, we observe picosecond-scale absorption of organic molecular dimer cations, providing direct evidence of interface charge transfer at room temperature. Moreover, energy transfer from the TiOPc to WSe2 may exist based on the tunability in the fluorescence emission of the TiOPc/WSe2 heterostructure as the temperature changes. This study unveils the critical role of vdW epitaxy and temperature in the exciton dynamics of organic/2D TMDs hybrid systems and provides guidance for studying interlayer charge and energy transfer in organic/inorganic heterostructures.

Metallic layered VSe2 saturable absorber based single- and dual-wavelength ultrafast fiber laser

Vanadium selenide (VSe2) is a special two-dimensional (2D) transition metal dichalcogenide (TMD) material with metallic properties similar to graphene, which has been proved to have saturable absorption properties and used in mode-locked fiber lasers. As an excellent saturable absorber (SA) material, VSe2 has advantage of ultrafast carrier recovery time and broadband optical response range. However, the potential application of VSe2 in the field of ultrafast photonics has not been fully developed so far. In this work, the as-prepared VSe2 nanosheets were deposited on tapered fiber by optical deposition to obtain VSe2 SA. By inserting VSe2 SA into an Er-doped fiber laser, the mode-locked pulses with a central wavelength of 1574.4 nm can be obtained. The pulse width of the laser is measured to be ∼680 fs which is narrowest in the reported VSe2 SA-based lasers. In addition, the unique dual-wavelength mode-locked pulse is also obtained by further adjusting intracavity dispersion and polarization. This kind of dual-wavelength pulse is valuable in high order harmonic generation enhancement, terahertz wave generation, dense wavelength division multiplexing, dual-frequency comb and other applications. Our results show that metallic VSe2 is of great potential value in ultrafast fiber laser.

Nanoscale Channel Length MoS2 Vertical Field-Effect Transistor Arrays with Side-Wall Source/Drain Electrodes.

Two-dimensional transition metal dichalcogenides (TMDCs) have natural advantages in overcoming the short-channel effect in field-effect transistors (FETs) and in fabricating three-dimensional FETs, which benefit in increasing device density. However, so far, most reported works related to MoS2 FETs with a sub-100 nm channel employ mechanically exfoliated materials and all of the works involve electron beam lithography (EBL), which may limit their application in fabricating wafer-scale device arrays as demanded in integrated circuits (ICs). In this work, MoS2 FET arrays with a side-wall source and drain electrodes vertically distributed are designed and fabricated. The channel length of the as-fabricated FET is basically determined by the thickness of an insulating layer between the source and drain electrodes. The vertically distributed source and drain electrodes enable to reduce the electrode-occupied area and increase in the device density. The as-fabricated vertical FETs exhibit on/off ratios comparable to those of mechanically exfoliated MoS2 FETs with a nanoscale channel length under identical VDS. In addition, the as-fabricated FETs can work at a VDS as low as 10 mV with a desirable on/off ratio (1.9 × 107), which benefits in developing low-power devices. Moreover, the fabrication process is free from EBL and can be applied to wafer-scale device arrays. The statistical results show that the fabricated FET arrays have a device yield of 87.5% and an average on/off ratio of about 1.7 × 106 at a VDS of 10 mV, with the lowest and highest ones to be about 1.3 × 104 and 1.9 × 107, respectively, demonstrating the good reliability of our fabrication process. Our work promises a bright future for TMDCs in realizing high-density and low-power nanoelectronic devices in ICs.

Preparation and optoelectronic performance of two-dimensional MoSe2/WSe2 lateral and vertical heterostructures

Two-dimensional materials Transition Metal Dichalcogenides (TMDs) are a novel type of semiconductor material with tunable bandgap and atomic-level thickness. Different TMDs can be flexibly combined to form heterostructures with distinct properties. In this paper, we have prepared two-dimensional MoSe2/WSe2 vertical and lateral heterostructures by using CVD and a combination of PVD and CVD, respectively. Subsequently, the structure, electronic and optoelectronic properties of these two types of heterostructures were characterized. The results indicate that field-effect transistors based on single-layer MoSe2/WSe2 lateral heterostructures, and single-layer WSe2/multi-layer MoSe2 and single-layer MoSe2/multi-layer WSe2 vertical heterostructures exhibit significant rectification effects. The in-plane monolayer MoSe2/WSe2 heterostructure devices exhibit the on/ff ratio of up to 104, and the monolayer-multilayer vertical heterostructure reaching 106, significantly outperforming most known devices of the same type. Moreover, the optical response of both in-plane and vertical heterostructures field-effect transistors reach 10 ms. Our research findings offer pathways for the flexible selective growth of in-plane and vertical heterostructures based on TMDs, and provide insights into achieving diverse performance in logic devices.

First-principles study on the electronic properties and feasibility of photocatalytic water splitting on Z-scheme GaN/MoS2 heterostructure

In recent years, van der Waals heterostructures have played a significant role in fields such as photocatalysis, quantum devices, sensors, etc., due to their excellent performance exhibited through synergistic interactions between multiple components and the highly customizable design. Two-dimensional transition metal dichalcogenides, with their highly tunable band structures and excellent electrochemical activity, are well-suited for constructing heterostructures. To investigate the specific electronic and photocatalysis properties of relative heterostructure, GaN/MoS2 heterostructure is constructed. Through the first-principles calculation, the Z-scheme GaN/MoS2 heterostructure shows a direct band gap of 0.869 eV. The excellent capability for separating the photogenerated carriers can be inferred from the conduction band offset as high as 1.915 eV and electrostatic potentials Ep of 6.361 eV. At pH = 14, oxygen evolution reaction can spontaneously occur under the photocatalytic action of the GaN/MoS2 heterostructure according to the negative Gibbs differences of −0.514 eV, −3.809 eV, −2.576 eV and −5.718 eV in the four-electron pathways. Therefore, the Z-scheme GaN/MoS2 heterostructure has great prospects in the application of optoelectronic devices and photocatalysis.