Few‐Layered PtS2 Phototransistor on h‐BN with High Gain

The very recently rediscovered group‐10 transition metal dichalcogenides (TMDs) such as PtS₂ and PtSe₂, have joined the 2D material family as potentially promising candidates for electronic and optoeletronic applications due to their theoretically high carrier mobility, widely tunable bandgap, and ultrastability. Here, the first exploration of optoelectronic application based on few‐layered PtS₂ using h‐BN as substrate is presented. The phototransistor exhibits high responsivity up to 1.56 × 10³ A W^?1 and detectivity of 2.9 × 10¹¹ Jones. Additionally, an ultrahigh photogain ≈2 × 10⁶ is obtained at a gate voltage V _g = 30 V, one of the highest gain among 2D photodetectors, which is attributed to the existence of trap states. More interestingly, the few‐layered PtS₂ phototransistor shows a back gate modulated photocurrent generation mechanism, that is, from the photoconductive effect dominant to photogating effect dominant via tuning the gate voltage from the OFF state to the ON state. Such good properties combined with gate‐controlled photoresponse of PtS₂ make it a competitive candidate for future 2D optoelectronic applications.     

Charge Photogeneration in Few‐Layer MoS2

The 2D semiconductor MoS₂ in its mono‐ and few‐layer form is expected to have a significant exciton binding energy of several 100 meV, suggesting excitons as the primary photoexcited species. Nevertheless, even single layers show a strong photovoltaic effect and work as the active material in high sensitivity photodetectors, thus indicating efficient charge carrier photogeneration. Here, modulation spectroscopy in the sub‐ps and ms time scales is used to study the photoexcitation dynamics in few‐layer MoS₂. The results suggest that the primary photoexcitations are excitons that efficiently dissociate into charges with a characteristic time of 700 fs. Based on these findings, simple suggestions for the design of efficient MoS₂ photovoltaic and photodetector devices are made.     

Photosensor Device Based on Few‐Layered WS2 Films

Few‐layered films of WS₂, synthesized by chemical vapor deposition on quartz, are successfully used as light sensors. The film samples are structurally characterized by Raman spectroscopy, atomic force microscopy, scanning electron microscopy, and high‐resolution transmission electron microscopy. The produced samples consist of few layered sheets possessing up to 10 layers. UV–visible absorbance spectra reveals absorption peaks at energies of 1.95 and 2.33 eV, consistent with the A and B excitons characteristic of WS₂. Current–voltage (I–V) and photoresponse measurements carried out at room temperature are performed by connecting the WS₂ layered material with Au/Ti contacts. The photocurrent measurements are carried out using five different laser lines ranging between 457 and 647 nm. The results indicate that the electrical response strongly depends on the photon energy from the excitation lasers. In addition, it is found that the photocurrent varies non‐linearly with the incident power, and the generated photocurrent in the WS₂ samples varies as a squared root of the incident power. The excellent response of few‐layered WS₂ to detect different photon wavelengths, over a wide range of intensities, makes it a strong candidate for constructing novel optoelectronic devices.     

Anisotropic Phonon Response of Few‐Layer PdSe2 under Uniaxial Strain

PdSe₂, an emerging 2D material with a novel anisotropic puckered pentagonal structure, has attracted growing interest due to its layer‐dependent electronic bandgap, high carrier mobility, and good air stability. Herein, a detailed Raman spectroscopic study of few‐layer PdSe₂ (two to five layers) under the in‐plane uniaxial tensile strain up to 3.33% is performed. Two of the prominent PdSe₂ Raman peaks are influenced differently depending on the direction of strain application. The $A_g^1$ mode redshifts more than the $A_g^3$ mode when the strain is applied along the a‐axis of the crystal, while the $A_g^3$ mode redshifts more than the $A_g^1$ mode when the strain is applied along the b‐axis. Such an anisotropic phonon response to strain indicates directionally dependent mechanical and thermal properties of PdSe₂ and also allows the identification of the crystal axes. The results are further supported using first‐principles density‐functional theory. Interestingly, the near‐zero Poisson’s ratios for few‐layer PdSe₂ are found, suggesting that the uniaxial tensile strain can easily be applied to few‐layer PdSe₂ without significantly altering their dimensions at the perpendicular directions, which is a major contributing factor to the observed distinct phonon behavior. The findings pave the way for further development of 2D PdSe₂‐based flexible electronics.     

Few‐Layered WS2 Nanoplates Confined in Co,N‐Doped Hollow Carbon Nanocages: Abundant WS2 Edges for Highly Sensitive Gas Sensors

Edges of 2D transition metal dichalcogenides (TMDs) are well known as highly reactive sites, thus researchers have attempted to maximize the edge site density of 2D TMDs. In this work, metal‐organic framework (MOF) templates are introduced to synthesize few‐layered WS₂ nanoplates (a lateral dimension of ≈10 nm) confined in Co, N‐doped hollow carbon nanocages (WS₂_Co‐N‐HCNCs), for highly sensitive NO₂ gas sensors. WS₂ precursors are assembled in the surface cavity of Co‐based zeolite imidazole framework (ZIF‐67) and subsequent pyrolysis produced WS₂_Co‐N‐HCNCs. During the pyrolysis, the carbonized ZIF‐67 are doped by Co and N elements, and the growth of WS₂ is effectively suppressed, creating few‐layered WS₂ nanoplates functionalized Co‐N‐HCNCs. The WS₂_Co‐N‐HCNCs exhibit outstanding NO₂ sensing characteristics at room temperature, in terms of response (48.2% to 5 ppm), selectivity, response and recovery speed, and detection limit (100 ppb). These results are attributed to the enhanced adsorption and desorption kinetics of NO₂ on abundant WS₂ edges, confined in the gas permeable HCNCs. This work opens up an efficient way for the facile synthesis of edge abundant few‐layered TMDs combined with porous carbon matrix via MOF templating route, for applications relying on highly active sites.     

Significant Exciton Brightening in Monolayer Tungsten Disulfides via Fluorination: n‐Type Gas Sensing Semiconductors

Monolayer transition‐metal dichalcogenides (TMDCs) have recently emerged as promising candidates for advanced photonic and valleytronic applications due to their unique optoelectronic properties. However, the low luminescence efficiency of monolayer TMDCs has significantly hampered their use in these fields. Here it is reported that the photoluminescence efficiency of monolayer WS₂ can be remarkably enhanced up to fourfold through the fluorination, surpassing the reported performance of molecular and/or electrical doping methods. Its degree is easily controlled by changing the fluorine plasma duration time and can also be reversibly tuned via additional hydrogen plasma treatment, allowing for its versatile tailoring for interfacial band alignment and customized engineering. The striking photoluminescence improvement occurs via a substantial transition of trions to excitons as a result of the strong electron affinity of fluorine dopants, and the fluorination enables unprecedented detection of n‐type NH₃ gas in WS₂ due to changed excitonic dynamics showing excellent sensitivity (at least down to 1.25 ppm). This work provides valuable strategies and insights into exciton physics in monolayer TMDCs, opening up avenues toward highly‐efficient 2D light emitters, photovoltaics, nanosensors, and optical interconnects.     

Efficient Photocarrier Transfer and Effective Photoluminescence Enhancement in Type I Monolayer MoTe2/WSe2 Heterostructure

Artificial van der Waals heterostructures of 2D layered materials are attractive from the viewpoint of the possible discovery of new physics together with improved functionalities. Stacking various combinations of atomically thin semiconducting transition metal dichalcogenides, MX₂ (M = Mo, W; X = S, Se, Te) with a hexagonal crystal structure, typically leads to the formation of a staggered Type II band alignment in the heterostructure, where electrons and holes are confined in different layers. Here, the comprehensive studies are performed on heterostructures prepared from monolayers of WSe₂ and MoTe₂ using differential reflectance, photoluminescence (PL), and PL excitation spectroscopy. The MoTe₂/WSe₂ heterostructure shows strong PL from the MoTe₂ layer at ≈1.1 eV, which is different from the quenched PL from the WSe₂ layer. Moreover, enhancement of PL intensity from the MoTe₂ layer is observed because of the near‐unity highly efficient photocarrier transfer from WSe₂ to MoTe₂. These experimental results suggest that the MoTe₂/WSe₂ heterostructure has a Type I band alignment where electrons and holes are confined in the MoTe₂ layer. The findings extend the diversity and usefulness of ultrathin layered heterostructures based on transition metal dichalcogenides, leading to possibilities toward future optoelectronic applications.     

Tailoring the Surface Chemical Reactivity of Transition‐Metal Dichalcogenide PtTe2 Crystals

PtTe₂ is a novel transition‐metal dichalcogenide hosting type‐II Dirac fermions that displays application capabilities in optoelectronics and hydrogen evolution reaction. Here it is shown, by combining surface science experiments and density functional theory, that the pristine surface of PtTe₂ is chemically inert toward the most common ambient gases (oxygen and water) and even in air. It is demonstrated that the creation of Te vacancies leads to the appearance of tellurium‐oxide phases upon exposing defected PtTe₂ surfaces to oxygen or ambient atmosphere, which is detrimental for the ambient stability of uncapped PtTe₂‐based devices. On the contrary, in PtTe₂ surfaces modified by the joint presence of Te vacancies and substitutional carbon atoms, the stable adsorption of hydroxyl groups is observed, an essential step for water splitting and the water–gas shift reaction. These results thus pave the way toward the exploitation of this class of Dirac materials in catalysis.     

Visualizing Energy Transfer at Buried Interfaces in Layered Materials Using Picosecond X‐Rays

Understanding the fundamentals of nanoscale heat propagation is crucial for next‐generation electronics. For instance, weak van der Waals bonds of layered materials are known to limit their thermal boundary conductance (TBC), presenting a heat dissipation bottleneck. Here, a new nondestructive method is presented to probe heat transport in nanoscale crystalline materials using time‐resolved X‐ray measurements of photoinduced thermal strain. This technique directly monitors time‐dependent temperature changes in the crystal and the subsequent relaxation across buried interfaces by measuring changes in the c‐axis lattice spacing after optical excitation. Films of five different layered transition metal dichalcogenides MoX₂ [X = S, Se, and Te] and WX₂ [X = S and Se] as well as graphite and a W‐doped alloy of MoTe₂ are investigated. TBC values in the range 10–30 MW m^?2 K^?1 are found, on c‐plane sapphire substrates at room temperature. In conjunction with molecular dynamics simulations, it is shown that the high thermal resistances are a consequence of weak interfacial van der Waals bonding and low phonon irradiance. This work paves the way for an improved understanding of thermal bottlenecks in emerging 3D heterogeneously integrated technologies.     

Photoluminescence from Liquid‐Exfoliated WS2 Monomers in Poly(Vinyl Alcohol) Polymer Composites

While liquid phase exfoliation can be used to produce nanosheets stabilized in polymer solutions, very little is known about the resultant nanosheet size, thickness, or monolayer content. The present study uses semiquantitative spectroscopic metrics based on extinction, Raman, and photoluminescence (PL) spectroscopy to investigate these parameters for WS₂ nanosheets exfoliated in aqueous poly(vinyl alcohol) (PVA) solutions. By measuring Raman and PL simultaneously, the monolayer content can be tracked via the PL/Raman intensity ratio while varying processing conditions. The PL is found to be maximized for a stabilizing polymer concentration of 2 g L^?1. In addition, the monolayer content can be controlled via the centrifugation conditions, exceeding 5% by mass in some cases. These techniques have allowed tracking the ratio of PL/Raman in a droplet of polymer‐stabilized WS₂ nanosheets as the water evaporates during composite formation. No evidence of nanosheet aggregation is found under these conditions although the PL becomes dominated by trion emission as drying proceeds and the balance of doping from PVA/water changes. Finally, bulk PVA/WS₂ composites are produced by freeze drying where >50% of the monolayers remain unaggregated, even at WS₂ volume fractions as high as 10%.     

Continuous Control and Enhancement of Excitonic Valley Polarization in Monolayer WSe2 by Electrostatic Doping

Enhancement and continuous control of the excitonic valley polarization in electrostatically doped monolayer WSe₂ are demonstrated. Under excitation with circularly polarized light, 20% valley polarization of excitons around the charge neutrality condition at 70 K is increased to 40% by modulating the electron/hole density up to 2 × 10¹² cm^?2. This increase originates from slow valley relaxation for neutral exciton between the K and ?K valleys owing to screening of long‐range e–h exchange interactions by doped carriers. The gate‐dependences of the exciton valley polarization at various temperatures are reproduced by theoretical calculations, which holds potential for next‐generation valleytronic devices continuously controlled by an applied bias voltage.     

Band‐Edge Exciton Fine Structure and Exciton Recombination Dynamics in Single Crystals of Layered Hybrid Perovskites

2D perovskite materials have recently reattracted intense research interest for applications in photovoltaics and optoelectronics. As a consequence of the dielectric and quantum confinement effect, they show strongly bound and stable excitons at room temperature. Here, the band‐edge exciton fine structure and in particular its exciton and biexciton dynamics in high quality crystals of (PEA)₂PbI₄ are investigated. A comparison of bulk and surface exciton lifetimes yields a room temperature surface recombination velocity of 2 × 10³ cm s^?1 and an intrinsic lifetime of 185 ns. Biexciton emission is evidenced at room temperature, with a binding energy of ≈45 meV and a lifetime of 80 ps. At low temperature, exciton state splitting is observed, which is caused by the electron–hole exchange interaction. Transient photoluminescence resolves the low‐lying dark exciton state, with a bright/dark splitting energy estimated to be 10 meV. This work contributes to the understanding of the complex scenario of the elementary photoexcitations in 2D perovskites.     

Self‐Aligned and Scalable Growth of Monolayer WSe2–MoS2 Lateral Heterojunctions

2D layered heterostructures have attracted intensive interests due to their unique optical, transport, and interfacial properties. The laterally stitched heterojunction based on dissimilar 2D transition metal dichalcogenides forms an intrinsic p–n junction without the necessity of applying an external voltage. However, no scalable processes are reported to construct the devices with such lateral heterostructures. Here, a scalable strategy, two‐step and location‐selective chemical vapor deposition, is reported to synthesize self‐aligned WSe₂–MoS₂ monolayer lateral heterojunction arrays and demonstrates their light‐emitting devices. The proposed fabrication process enables the growth of high‐quality interfaces and the first successful observation of electroluminescence at the WSe₂–MoS₂ lateral heterojunction. The electroluminescence study has confirmed the type‐I alignment at the interface rather than commonly believed type‐II alignment. This self‐aligned growth process paves the way for constructing various 2D lateral heterostructures in a scalable manner, practically important for integrated 2D circuit applications.     

Understanding Dopant–Host Interactions on Electronic Structures and Optical Properties in Ce-Doped WS2 Monolayers

Substitutional lanthanide doping of 2D transition metal dichalcogenides (TMDs) is expected to be a promising strategy to engineer optical, electronic, and optoelectronic properties of TMDs. Understanding the interactions between lanthanide dopants and 2D TMDs host is one of the key problems to be resolved for their profound research studies. Herein, the interactions between Ce dopants and monolayer WS₂ in a physical vapor deposition grown Ce-doped WS₂ monolayer are studied by combining scanning tunneling microscopy with optical characterizations with high spatial and temporal resolution. It is found that the highly anisotropic crystal field can effectively split the energy levels of the Ce dopants’ f orbital. The electrons in the split energy levels can bind the holes in the valence band maximum of the Ce-doped WS₂, forming optical bright excitons. These excitons collide with the free A excitons when increasing the pump fluences, reducing the A exciton's lifetime. This study may be beneficial for the design and fabrication of optical, electronic, and optoelectronic devices based on lanthanide-doped TMDs.     

Transition‐Metal Dichalcogenide NiTe2: An Ambient‐Stable Material for Catalysis and Nanoelectronics

By means of theory and experiments, the application capability of nickel ditelluride (NiTe₂) transition‐metal dichalcogenide in catalysis and nanoelectronics is assessed. The Te surface termination forms a TeO₂ skin in an oxygen environment. In ambient atmosphere, passivation is achieved in less than 30 min with the TeO₂ skin having a thickness of about 7 Å. NiTe₂ shows outstanding tolerance to CO exposure and stability in water environment, with subsequent good performance in both hydrogen and oxygen evolution reactions. NiTe₂‐based devices consistently demonstrate superb ambient stability over a timescale as long as one month. Specifically, NiTe₂ has been implemented in a device that exhibits both superior performance and environmental stability at frequencies above 40 GHz, with possible applications as a receiver beyond the cutoff frequency of a nanotransistor.     

Enhanced Reversible Sodium‐Ion Intercalation by Synergistic Coupling of Few‐Layered MoS2 and S‐Doped Graphene

Sodium‐ion batteries (SIBs) are regarded as the best alternative to lithium‐ion batteries due to their low cost and similar Na⁺ insertion chemistry. It is still challenging but greatly desired to design and develop novel electrode materials with high reversible capacity, long cycling life, and good rate capability toward high‐performance SIBs. This work demonstrates an innovative design strategy and a development of few‐layered molybdenum disulfide/sulfur‐doped graphene nanosheets (MoS₂/SG) composites as the SIB anode material providing a high specific capacity of 587 mA h g^?1 calculated based on the total composite mass and an extremely long cycling stability over 1000 cycles at a current density of 1.0 A g^?1 with a high capacity retention of ≈85%. Systematic characterizations reveal that the outstanding performance is mainly attributed to the unique and robust composite architecture where few‐layered MoS₂ and S‐doped graphene are intimately bridged at the hetero‐interface through a synergistic coupling effect via the covalently doped S atoms. The design strategy and mechanism understanding at the molecular level outlined here can be readily applied to other layered transition metal oxides for SIBs anode and play a key role in contributing to the development of high‐performance SIBs.