Transition Metal Dichalcogenides Research Articles

Double Superconducting Dome of Quasi Two-Dimensional TaS2 in Non-Centrosymmetric van der Waals Heterostructure.

Two-dimensional van der Waals heterostructures (2D-vdWHs) based on transition metal dichalcogenides (TMDs) provide unparalleled control over electronic properties. However, the interlayer coupling is challenged by the interfacial misalignment and defects, which hinders a comprehensive understanding of the intertwined electronic orders, especially superconductivity and charge density wave (CDW). Here, by using pressure to regulate the interlayer coupling of non-centrosymmetric 6R-TaS2 vdWHs, we observe an unprecedented phase diagram in TMDs. This phase diagram encompasses successive suppression of the original CDW states from alternating H-layer and T-layer configurations, the emergence and disappearance of a new CDW-like state, and a double superconducting dome induced by different interlayer coupling effects. These results not only illuminate the crucial role of interlayer coupling in shaping the complex phase diagram of TMD systems but also pave a new avenue for the creation of a novel family of bulk heterostructures with customized 2D properties.

Robust Layer‐Dependent Valley Polarization and Valley Coherence in Spiral WS2 at Room Temperature

In the emerging field of valleytronics, it is aimed to coherently manipulate the valley pseudospin as an information‐bearing degree of freedom. The 2D transition‐metal dichalcogenides (TMDCs) provide a unique possibility to generate an excitonic valley pseudospin, opening the way to valley information. Although significant development of valley pseudospin in layered materials has been achieved recently, looking for new TMDCs featuring robust valley phenomenon at room temperature is still desirable for practical applications. Herein, the valley pseudospin of the spiral WS2 with different layer thicknesses at room temperature is investigated by both circular and linear polarization‐resolved photoluminescence spectroscopy. In the experimental results, it is demonstrated that the spiral WS2 emerges robust valley polarization and valley coherence, the degree of circular polarization, and linear polarization gradually increase with the lift of the layer thicknesses, reaching up to 0.91 for valley polarization and 0.94 for valley coherence, respectively. The robust layer‐dependent valley pseudospin may originate from the intrinsic broken inversion symmetry, due to the spiral structure of the multilayer WS2. The robust and near‐unity valley polarization and valley coherence at room temperature in the spiral WS2 may provide a new platform for optical manipulation of the valley pseudospin for further valleytronics applications.

Two-Step Conversion of Metal and Metal Oxide Precursor Films to 2D Transition Metal Dichalcogenides and Heterostructures.

The widely studied class of two-dimensional (2D) materialsknown as transition metal dichalcogenides (TMDs) are now well-poised to be employed in real-world applications ranging from electronic logic and memory devices to gas and biological sensors. Several scalable thin film synthesis techniques have demonstrated nanoscale control of TMD material thickness, morphology, structure, and chemistry and correlated these properties with high-performing, application-specific device metrics. In this review, the particularly versatile two-step conversion (2SC) method of TMD film synthesis is highlighted. The 2SC technique relies on deposition of a solid metal or metal oxide precursor material, followed by a reaction with a chalcogen vapor at an elevated temperature, converting the precursor film to a crystalline TMD. Herein, the variables at each step of the 2SC process including the impact of the precursor film material and deposition technique, the influence of gas composition and temperature during conversion, as well as other factors controlling high-quality 2D TMD synthesis are considered. The specific advantages of the 2SC approach including deposition on diverse substrates, low-temperature processing, orientation control, and heterostructure synthesis, among others, are featured. Finally, emergent opportunities that take advantage of the 2SC approach are discussed to include next-generation electronics, sensing, and optoelectronic devices, as well as catalysis for energy-related applications.

Understanding Substrate Effects on 2D MoS2 Growth: A Kinetic Monte Carlo Approach

AbstractControlling the morphology of 2D transition metal dichalcogenides (TMDs) plays a key role in their applications. Although chemical vapor deposition can achieve wafer‐scale growth of 2D TMDs, a comprehensive theoretical framework for effective growth optimization is lacking. Atomistic modeling methods offer a promising approach to delve into the intricate dynamics underlying the growth. In this study, kinetic Monte Carlo (kMC) simulations are employed to identify crucial parameters that govern the morphology of MoS2 flakes grown on diverse substrates. The simulations reveal that large adsorption rates significantly enhance growth speed, which however necessitates rapid edge migration to achieve compact triangles. Substrate etching can tune the adsorption–desorption process of adatoms and enable preferential growth within a specific substrate region, controlling the flake morphology. This study unravels the complex dynamics governing 2D TMD morphology, offering a theoretical framework for decision‐making in the design and optimization of TMD synthesis processes.

Photovoltaic induced self-powered gas sensor based on 2D MoS2 incorporated NbSe2 nanorods heterostructure for NH3 gas sensing at room temperature

Two-dimensional (2D) transition metal dichalcogenides (TMDs) have attracted significant attention for their optical and gas-sensing applications due to their exceptional sensitivity. Reliable selectivity and low power consumption are two major requirements for photodetector and gas sensor applications in next-generation electronic devices and the Internet of Things. Self-powered sensors (especially photovoltaic gas sensors) can solve these problems. In this study, for the first time, we report 2D TMDs (NbSe2-MoS2 hybrid) on a SiO2/Si substrate to fabricate photovoltaic self-powered gas sensors. The gas sensors are operated by the photovoltaic effect of the NbSe2-MoS2 nanostructure, which is prepared using the liquid phase exfoliation process. Initially, it was revealed that the present hybrid material exhibits photovoltaic properties under light illumination, with a circuit current of 0.25 µA and a circuit voltage of 34 mV. The NbSe2-MoS2 nanostructure characteristics were then used for NH3 gas sensing at different concentrations, and the gas sensing response was detected from low (8.8 % at 10 ppm) to high (28.8 % at 500 ppm) concentrations. The built-in electric field occurred between the NbSe2-MoS2 junction and eventually operated as a driving force for NbSe2-MoS2 gas sensing without an external bias voltage. The physisorption of gas molecules on their surface prompts a charge-transfer mechanism that improves the gas sensor response. The combined outcome of NbSe2-MoS2 heterostructures could pave way to next-generation gas sensing device fabrications.

Precision anode vacancy engineering for long-lasting and fast-charging Na-Ion batteries

In the field of energy storage materials, the unique properties of vacancies are highly significant, especially in the optimization of transition metal dichalcogenides (TMDs). However, scaling up these storage solutions remains a considerable challenge. In our study, we successfully synthesized VSe2-x via alleviating selenide content, where vacancies were introduced in situ through a straightforward physical vapor transport process. These vacancies boost the adsorption capacity for sodium ions (Na+), and create additional active sites, thereby minimizing the structural changes in VSe2-x during Na+ storage. Our VSe2-x based negative electrode demonstrates impressive sodium storage capability, offering an exceptional rate performance with a capacity of 346 mAh g−1 at 5 A g−1 and maintaining a remarkable stability of 378 mAh g−1 even after 1400 cycles at 10 A g−1. Additionally, through a combination of theoretical calculations, in situ X-ray diffraction analysis, and ex situ transmission electron microscopy, we have confirmed the creation of vanadium selenide materials containing vacancies. During continuous charging and discharging, these materials facilitate the generation of numerous sodium-containing aggregates with high electronic conductivity. This paper provides a comprehensive exploration of how vacancies in transformed materials can be an effective strategy for efficient rechargeable batteries.

Molecular Intercalation‐Induced Two‐Phase Evolution Engineering of 1T and 2H‐MS2 (M = Mo, V, W) for Interface‐Polarization‐Enhanced Electromagnetic Absorbers

AbstractPolarization at interfaces is an important loss mechanism for electromagnetic wave (EMW) attenuation, though the motion behavior of carriers in interfaces composed of different types of conductors has yet to be investigated. Tuning the phase structure of transition metal dichalcogenides (TMDs) MS2 (M = Mo, V, W) by organics small molecule intercalation to achieve the modulation of interfacial types is an effective strategy, where 1T‐MS2 exhibits metallic properties and 2H‐MS2 has semiconducting properties. To exclude the contribution of the intrinsic properties of TMDs materials, three TMDs (MoS2, VS2, and WS2), which also possess phase transitions, are investigated. Among them, the 1T‐MS2 composite exhibits excellent EMW absorption performance under the synergistic effect of interfacial polarization and conduction loss. 1T‐MoS2/MOF‐A exhibits the best EMW absorption performance with an RLmin of −61.07 dB at a thickness of 3.0 mm and an EAB of 7.2 GHz at 2.3 mm. The effectiveness of the modulation of the interfacial polarization using 1T‐phase and 2H‐phase MS2 is demonstrated, which is important for the analysis of the carrier motion behavior during the interfacial loss.

Nanophotonic route to control electron behaviors in 2D materials

Abstract Two-dimensional (2D) Dirac materials, e.g., graphene and transition metal dichalcogenides (TMDs), are one-atom-thick monolayers whose electronic behaviors are described by the Dirac equation. These materials serve not only as test beds for novel quantum physics but also as promising constituents for nanophotonic devices. This review provides a brief overview of the recent effort to control Dirac electron behaviors using nanophotonics. We introduce a principle of light-2D Dirac matter interaction to offer a design guide for 2D Dirac material–based nanophotonic devices. We also discuss opportunities for coupling nanophotonics with externally perturbed 2D materials.

Metal Doping Regulates Electrocatalysts Restructuring during Oxygen Evolution Reaction.

High-efficiency and low-cost catalysts for oxygen evolution reaction (OER) are critical for electrochemical water splitting to generate hydrogen, which is a clean fuel for sustainable energy conversion and storage. Among the emerging OER catalysts, transition metal dichalcogenides have exhibited superior activity compared to commercial standards such as RuO2, but inferior stability due to uncontrolled restructuring with OER. In this study, we create bimetallic sulfide catalysts by adapting the atomic ratio of Ni and Co in CoxNi1-xSy electrocatalysts to investigate the intricate restructuring processes. Surface-sensitive X-ray photoelectron spectroscopy and bulk-sensitive X-ray absorption spectroscopy confirmed the favorable restructuring of transition metal sulfide material following OER processes. Our results indicate that a small amount of Ni substitution can reshape the Co local electronic structure, which regulates the restructuring process to optimize the balance between OER activity and stability. This work represents a significant advancement in the development of efficient and noble metal-free OER electrocatalysts through a doping-regulated restructuring approach.

Strain engineering the spin-valley coupling of the R-stacking sliding ferroelectric bilayer 2H-VX2 (X = S, Se, Te)

The emergence of magnetic transition metal dichalcogenides has significantly advanced the development of valleytronics due to the spontaneous breaking of time-reversal symmetry and space-inversion symmetry. However, the lack of regulation methods has prevented researchers from exploring their potential applications. Herein, we propose to use strain engineering to control the spin-valley coupling in the sliding ferroelectric bilayer 2H-VX2 (X = S, Se, Te). Four multiferroic states are constructed by combining the sliding ferroelectricity and antiferromagnetism in the R-stacking bilayer VX2, where the spin and valley polarizations are coupled together from the layer-dependent spin-polarized band structures. By applying a small external strain or pressure on the out-of-plane van der Waals direction, we predicted that there is an antiferromagnetic to magnetic transition in the bilayer VX2, leading to the interesting spin-polarized and chiral circularly polarized radiation at K+ and K- valleys, similar to those found in the magnetic monolayer. To comprehend the coupling between various degrees of freedom in these multiferroic systems, we have developed an effective k·p model. This model unveils a linear relationship between the electric polarization generated by interlayer sliding and the energy difference of the valence band maximum at K+ and K- valleys. Thus, providing an alternate method to measure the electric polarization in the sliding ferroelectrics. Based on the strong coupling between the strain, spin-valley, and electric polarization, it is likely to use the strain to control the interesting emerging properties of 2H-VX2 such as the anomalous valley Hall effect.

Synthesis of flowerlike vanadium diselenide microspheres for efficient electromagnetic wave absorption

The revelation of MoS2 as an efficient electromagnetic wave (EMW) absorbing material has ratcheted up people’s attention to other transition metal dichalcogenides (TMDs). To date, extensive studies have been conducted on the semiconducting VIB-Group TMDs while research into metallic VB-Group TMDs has been relatively rare. In this work, we successfully fabricated VB-Group VSe2 microspheres through a facile one-step hydrothermal method and used them as EMW absorbers. The flowerlike VSe2 microspheres based on VSe2 nanosheets exhibited a minimum reflection loss of 46.58 dB with an effective absorption bandwidth of 4.86 GHz. The influence of material morphology, microstructure, and dielectric properties on the EMW absorption performance was systematically investigated. The hierarchically layered structure promoted dielectric loss and EMW absorption by means of multiple reflection, interfacial polarization and related relaxation, and enhanced attenuation ability. This work not only demonstrates that VSe2 is potentially a high-efficiency single component EMW absorber, but also provides fresh insights into exploration on the EMW loss mechanisms of the metallic TMD-based absorbing materials.

Strong hybridization of Nb2C with MoS2: a way to reduce contact resistance

Abstract 
The hybridization of MXene materials and transition metal dichalcogenides has a significant impact on heterojunction properties. The transport properties and electronic structure of heterojunctions of semiconducting MoS2 and metallic MXene Nb2C were studied by integrating density functional theory with non-equilibrium Green's function theory. The hybridization between Nb2C and MoS2 makes the tunneling barrier between the two layers disappear, which can enhance the electron injection efficiency from the Nb2C to the MoS2. Moreover, the Nb2C/MoS2 heterojunction exhibits a conventional n-type Schottky contact with a barrier height of 0.14 eV, which is significantly lower than the barrier height of 0.29 eV at the Ti/MoS2 junction. These factors result in a field-effect transistor with a low contact resistance of 138 Ω·μm and a higher current of 1.09 mA/μm at a bias voltage of 0.3 V applied between the left and right electrodes. Following the application of gate voltage, the Ion/Ioff ratio reaches 1266.

Modification of WS2 thin film properties using high dose gamma irradiation.

The tunability of the Transition Metal Dichalcogenide (TMD) properties has gained attention from numerous researchers due to their wide application in various fields including quantum technology. In the present work, WS2 has been deposited on fluorine doped tin oxide (FTO) substrate and its properties have been studied systematically. These samples were irradiated using gamma radiation for various doses, and the effect on structural, morphological, optical and electrical properties has been reported. The crystallinity of the material is observed to be decreased, and the results are well supported by X-ray diffraction, Raman spectroscopy techniques. The increase in grain boundaries has been supported by the agglomeration observed in the scanning electron microscopy micrographs. The XPS results of WS2 after gamma irradiation show evolution of oxygen, carbon, C=O, W-O and SO42- peaks, confirming the addition of impurities and formation of point defect. The gamma irradiation creates point defects, and their density increases considerably with increasing gamma dosage. These defects crucially altered the structural, optical and electrical properties of the material. The reduction in the optical band gap with increased gamma irradiation is evident from the absorption spectra and respective Tauc plots. The I-V graphs show a 1000-fold increase in the saturation current after 100 kGy gamma irradiation dose. This work has explored the gamma irradiation effect on the WS2 and suggests substantial modification in the material and enhancement in electrical properties. &#xD.

Observation of interlayer plasmon polaron in graphene/WS2 heterostructures

Harnessing electronic excitations involving coherent coupling to bosonic modes is essential for the design and control of emergent phenomena in quantum materials. In situations where charge carriers induce a lattice distortion due to the electron-phonon interaction, the conducting states get “dressed", which leads to the formation of polaronic quasiparticles. The exploration of polaronic effects on low-energy excitations is in its infancy in two-dimensional materials. Here, we present the discovery of an interlayer plasmon polaron in heterostructures composed of graphene on top of single-layer WS2. By using micro-focused angle-resolved photoemission spectroscopy during in situ doping of the top graphene layer, we observe a strong quasiparticle peak accompanied by several carrier density-dependent shake-off replicas around the single-layer WS2 conduction band minimum. Our results are explained by an effective many-body model in terms of a coupling between single-layer WS2 conduction electrons and an interlayer plasmon mode. It is important to take into account the presence of such interlayer collective modes, as they have profound consequences for the electronic and optical properties of heterostructures that are routinely explored in many device architectures involving 2D transition metal dichalcogenides.

Ultrafast Formation of Charge Transfer Trions at Molecular‐Functionalized 2D MoS2 Interfaces

In this work, we investigate trion dynamics occurring at the heterojunction between organometallic molecules and a monolayer transition metal dichalcogenide (TMD) with transient electronic sum frequency generation (tr‐ESFG) spectroscopy. By pumping at 2.4 eV with laser pulses, we have observed an ultrafast hole transfer, succeeded by the emergence of charge‐transfer trions. This observation is facilitated by the cancellation of ground state bleach and stimulated emission signals due to their opposite phases, making tr‐ESFG especially sensitive to the trion formation dynamics. The presence of charge‐transfer trion at molecular functionalized TMD monolayers suggests the potential for engineering the local electronic structures and dynamics of specific locations on TMDs and offers the potential for transferring unique electronic attributes of TMD to the molecular layers.

Ultrafast Formation of Charge Transfer Trions at Molecular-Functionalized 2D MoS2 Interfaces.

In this work, we investigate trion dynamics occurring at the heterojunction between organometallic molecules and a monolayer transition metal dichalcogenide (TMD) with transient electronic sum frequency generation (tr-ESFG) spectroscopy. By pumping at 2.4 eV with laser pulses, we have observed an ultrafast hole transfer, succeeded by the emergence of charge-transfer trions. This observation is facilitated by the cancellation of ground state bleach and stimulated emission signals due to their opposite phases, making tr-ESFG especially sensitive to the trion formation dynamics. The presence of charge-transfer trion at molecular functionalized TMD monolayers suggests the potential for engineering the local electronic structures and dynamics of specific locations on TMDs and offers the potential for transferring unique electronic attributes of TMD to the molecular layers.

Impact of Carrier Gas Flow Rate on the Synthesis of Monolayer WSe2 via Hydrogen-Assisted Chemical Vapor Deposition

Transition metal dichalcogenides (TMDs), particularly monolayer TMDs with direct bandgap properties, are key to advancing optoelectronic device technology. WSe2 stands out due to its adjustable carrier transport, making it a prime candidate for optoelectronic applications. This study explores monolayer WSe2 synthesis via H2-assisted CVD, focusing on how carrier gas flow rate affects WSe2 quality. A comprehensive characterization of monolayer WSe2 was conducted using OM (optical microscope), Raman spectroscopy, PL spectroscopy, AFM, SEM, XPS, HRTEM, and XRD. It was found that H2 incorporation and flow rate critically influence WSe2’s growth and structural integrity, with low flow rates favoring precursor concentration for product formation and high rates causing disintegration of existing structures. This research accentuates the significance of fine-tuning the carrier gas flow rate for optimizing monolayer WSe2 synthesis, offering insights for fabricating monolayer TMDs like WS2, MoSe2, and MoS2, and facilitating their broader integration into optoelectronic devices.

Investigation of spectro-temporal high-order sideband generation from transition metal dichalcogenides [Invited

High-order sideband generation (HSG) in semiconductors under intense terahertz fields has been extensively studied, because it provides essential information for studying ultrafast dynamics in strong-field-dressed quantum materials. In particular, transition metal dichalcogenides (TMDCs), characterized by their unique band structures, provide an exemplary semiconductor system to explore the influence of material band structure on strong-field-induced modulation of HSG. In this work, we investigate the spectro-temporally resolved HSG from different bulk TMDC materials. Our results reveal distinct temporal HSG spectra, which can be attributed to the different absorption behaviors of these materials. Simulations based on the strong-field approximation and Floquet theory can well reproduce the experimental observations. Our work also delves into the spectro-temporal interference that emerges when neighboring harmonic orders overlap in the HSG spectrum. This work enhances our understanding of high-order sideband dynamics in strong-field-dressed semiconductors, offering insights for applications in spectrum- and phase-resolved ultrafast measurements.

Enhanced photocatalytic performance of SnS2 under visible light irradiation: strategies and future perspectives.

Tin(II) sulfide (SnS2) has emerged as a promising candidate for visible light photocatalytic materials. As a member of the transition metal dichalcogenides (TMDs) family, SnS2 features a band gap of approximately 2.20 eV and a layered structure, rendering it suitable for visible light activation with a high specific surface area. However, the application of SnS2 as a visible light photocatalyst still requires improvement, particularly in addressing the high recombination of electrons and holes, as well as the poor selectivity inherent in its perfect crystal structure. Therefore, ongoing research focuses on strategies to enhance the photocatalytic performance of SnS2. In this comprehensive review, we analyze recent advances and promising strategies for improving the photocatalytic performance of SnS2. Various successful approaches have been reported, including controlling the reactive facets of SnS2, inducing defects in the crystal structure, manipulating morphologies, depositing noble metals, and forming heterostructures. We provide a detailed understanding of these phenomena and the preparation techniques involved, as well as future considerations for exploring new science in SnS2 photocatalysis and optimizing performance.

Chiral limit and origin of topological flat bands in twisted transition metal dichalcogenide homobilayers

The observation of zero field fractional quantum Hall analogs in twisted transition metal dichalcogenides (TMDs) asks for a deeper understanding of what mechanisms lead to topological flat bands in two-dimensional heterostructures, and what makes TMDs an excellent platform for topologically ordered phases, surpassing twisted bilayer graphene. To this aim, we explore the chiral limits of massive Dirac theories applicable to C3-symmetric moiré materials, and show their relevance for both bilayer graphene and TMD homobilayers. In the latter, the Berry curvature of valence bands leads to relativistic corrections of the moiré potential that promote band flattening, and permit a limit with exactly flat bands with nonzero Chern number. The relativistic corrections enter as a layer-orbit coupling, analogous to spin-orbit coupling for relativistic Dirac fermions, which we show is non-negligible on the moiré scale. The Berry curvature of the TMD monolayers therefore plays an essential role in the flattening of moiré Chern bands in these heterostructures.