Current advances of transition metal dichalcogenides in electromagnetic wave absorption:A brief review

Transition metal dichalcogenides(TMDs)show great advantages in electromagnetic wave(EMW)absorption due to their unique structure and electrical properties.Tremendous research works on TMD-based EMW absorbers have been conducted in the last three years,and the comprehensive and systematical summary is still a rarity.Therefore,it is of great significance to elaborate on the interaction among the morphologies,structures,phases,components,and EMW absorption performances of TMD-based absorbers.This review is devoted to analyzing TMD-based absorbers from the following perspectives:the EMW absorption regulation strategies of TMDs and the latest progress of TMD-based hybrids as EMW absorbers.The absorption mechanisms and component-performance dependency of these achievements are also summarized.Finally,a straightforward insight into industrial revolution upgrading in this promising field is proposed.

Defect-engineered two-dimensional transition metal dichalcogenides towards electrocatalytic hydrogen evolution reaction

Recently,two-dimensional transition metal dichalcogenides(TMDs)demonstrated their great potential as cost-effective catalysts in hydrogen evolution reaction.Herein,we systematically summarize the existing defect engineering strategies,including intrinsic defects(atomic vacancy and active edges)and extrinsic defects(metal doping,nonmetal doping,and hybrid doping),which have been utilized to obtain advanced TMD-based electrocatalysts.Based on theoretical simulations and experimental results,the electronic structure,intermediate adsorption/desorption energies and possible catalytic mechanisms are thoroughly discussed.Particular emphasis is given to the intrinsic relationship between various types of defects and electrocatalytic properties.Furthermore,current opportunities and challenges for mechanical investigations and applications of defective TMD-based catalysts are presented.The aim herein is to reveal the respective properties of various defective TMD catalysts and provide valuable insights for fabricating high-efficiency TMD-based electrocatalysts.

Thermal transport properties of two-dimensional boron dichalcogenides from a first-principles and machine learning approach

The investigation of thermal transport is crucial to the thermal management of modern electronic devices.To obtain the thermal conductivity through solution of the Boltzmann transport equation,calculation of the anharmonic interatomic force constants has a high computational cost based on the current method of single-point density functional theory force calculation.The recent suggested machine learning interatomic potentials(MLIPs)method can avoid these huge computational demands.In this work,we study the thermal conductivity of two-dimensional MoS_(2)-like hexagonal boron dichalcogenides(H-B_(2)VI_(2);V I=S,Se,Te)with a combination of MLIPs and the phonon Boltzmann transport equation.The room-temperature thermal conductivity of H-B_(2)S_(2)can reach up to 336 W·m^(-1)·K^(-1),obviously larger than that of H-B_(2)Se_(2)and H-B_(2)Te_(2).This is mainly due to the difference in phonon group velocity.By substituting the different chalcogen elements in the second sublayer,H-B_(2)VIV I′have lower thermal conductivity than H-B_(2)VI_(2).The room-temperature thermal conductivity of B2STe is only 11%of that of H-B_(2)S_(2).This can be explained by comparing phonon group velocity and phonon relaxation time.The MLIP method is proved to be an efficient method for studying the thermal conductivity of materials,and H-B_(2)S_(2)-based nanodevices have excellent thermal conduction.

MoiréDirac fermions in transition metal dichalcogenides heterobilayers

Monolayer group-VIB transition metal dichalcogenides(TMDs)feature low-energy massive Dirac fermions,which have valley contrasting Berry curvature.This nontrivial local band topology gives rise to valley Hall transport and optical selection rules for interband transitions that open up new possibilities for valleytronics.However,the large bandgap in TMDs results in relatively small Berry curvature,leading to weak valley contrasting physics in practical experiments.Here,we show that Dirac fermions with tunable large Berry curvature can be engineered in moirésuperlattice of TMD heterobilayers.These moiréDirac fermions are created in a magnified honeycomb lattice with its sublattice degree of freedom formed by two local moirépotential minima.We show that applying an on-site potential can tune the moiréflat bands into helical ones.In short-period moirésuperlattice,we find that the two moirévalleys become asymmetric,which results in a net spin Hall current.More interestingly,a circularly polarized light drives these moiréDirac fermions into quantum anomalous Hall phase with chiral edge states.Our results open a new possibility to design the moiré-scale spin and valley physics using TMD moiréstructures.

Growing Biomorphic Transition Metal Dichalcogenides and Their Alloys Toward High Permeable Membranes and Efficient Electrocatalysts Applications

3D architecratured transition metal dichalcogenides constructed by atomically thin layers are appealing building blocks in various applications,such as catalysts,energy storage,conversions,sensors,and so on.However,the direct growth of 3D transition metal dichalcogenides architectures with high crystal quality and well-controlled size/thickness remains a huge challenge.Herein,we report a facile,highly-repeatable,and versatile chemical vapor deposition strategy,for the mass production of high-quality 3D-architecratured transition metal dichalcogenides(e.g.,MoS_(2),WS_(2),and ReS_(2))and their alloys(e.g.,W_(x)Mo(1–x)S_(2)and Rex Mo_((1–x))S_(2))nanosheets on naturally abundant and low-cost diatomite templates.Particularly,the purified transition metal dichalcogenides products exhibit unique and designable 3D biomorphic hierarchical microstructures,controllable layer thicknesses,tailorable chemical compositions,and good crystallinities.The weak interlayer interactions endow them with good dispersity in solutions to form stable additive-free inks for solution-processing-based applications,for example,high-permeable and high-stable separation membranes for water purification,and efficient electrocatalysts for hydrogen evolution reactions.This work paves ways for the low-cost,mass production of versatile transition metal dichalcogenides powder-like materials with designable structures and properties,toward energy/environmental-related applications and beyond.

Hydrogenic donor impurity states and intersubband optical absorption spectra of monolayer transition metal dichalcogenides in dielectric environments

The hydrogenic donor impurity states and intersubband optical absorption spectra in monolayer transition metal dichalcogenides(ML TMDs) under dielectric environments are theoretically investigated based on a two-dimensional(2D)nonorthogonal associated Laguerre basis set. The 2D quantum confinement effect together with the strongly reduced dielectric screening results in the strong attractive Coulomb potential between electron and donor ion, with exceptionally large impurity binding energy and huge intersubband oscillator strength. These lead to the strong interaction of the electron with light in a 2D regime. The intersubband optical absorption spectra exhibit strong absorption lines of the non-hydrogenic Rydberg series in the mid-infrared range of light. The strength of the Coulomb potential can be controlled by changing the dielectric environment. The electron affinity difference leads to charge transfer between ML TMD and the dielectric environment, generating the polarization-electric field in ML TMD accompanied by weakening the Coulomb interaction strength. The larger the dielectric constant of the dielectric environment, the more the charge transfer is, accompanied by the larger polarization-electric field and the stronger dielectric screening. The dielectric environment is shown to provide an efficient tool to tune the wavelength and output of the mid-infrared intersubband devices based on ML TMDs.

ZnCo_(2)O_(4)-ZnO@C@CoS核壳复合材料的制备及其在超级电容器中的应用

超级电容器以其高功率性能、稳定的循环性能和优良的安全性等独特优势,作为储能器件在新能源汽车和移动电子设备等方面极具前景。然而,其能量密度相对较低,限制了实际应用。为提升电化学活性,本研究通过简便的溶剂热法、煅烧处理和电化学沉积技术,在碳包覆的ZnCo_(2)O_(4)-ZnO微球上沉积了CoS纳米片(ZCO-ZO@C@CoS)。碳层不仅可以促进电子传输,增强导电性,还提升了结构的稳定性;CoS纳米片之间形成的开放网络空间促进了离子快速传输。此外,CoS纳米片具备丰富的电活性位点,实现了快速可逆的氧化还原反应;核壳结构内部的纳米线、碳层和外层纳米片的共同作用,有效提升了材料的整体电化学性能。因此,ZCO-ZO@C@CoS在1.5 A·g^(−1)时的比电容达到1944 F·g^(−1)(972.0 C·g^(−1)),20 A·g^(−1)高电流密度下循环10000次后比容量保持率为75%。由ZCO-ZO@C@CoS(正极)和活性炭(负极)组成的非对称超级电容器器件也表现出优异的比电容、高的倍率性能和优异的循环稳定性,显示出良好的应用前景。

大电流密度过渡金属硫族化合物析氢催化剂界面工程展望

氢能是未来可持续社会中理想的能量载体,利用可再生能源电解水制取绿氢的技术受到研究人员的广泛关注.电解水制绿氢技术由实验室向工业应用跨越的前提是发展大电流密度下性能优异且稳定的电催化剂.析氢反应(HER)是一种非均相反应,涉及催化剂-基底、催化剂-电解液、催化剂-气体三个界面.界面性质会影响电化学传质行为、电荷传输行为和催化剂的力学性质,从而影响大电流密度下制氢性能.因此,优化界面结构和性质是提升大电流密度下电解水催化剂性能并解决电解水技术工业应用挑战的关键.二维过渡金属硫族化合物(TMDCs)具有电子结构可调、活性位点丰富、合成方法多样等优势,自1976年首次应用于光电催化水分解反应、加氢脱硫反应以来,已有大量工作报道了TMDCs催化剂应用于HER.本文以TMDCs催化剂为例研究界面工程对大电流密度下HER的提升作用及机制.探讨了电化学反应中上述三个界面上发生的物理化学过程,系统分析了大电流密度下质量传输、电荷传输速率受限和力学强度不足三方面挑战,并总结了适用于大电流密度的催化剂性能描述符.分别归纳了针对以上三个界面的界面工程策略及相应作用,简要概括为:(1)催化剂-基底界面结合力增强、界面电阻降低、界面电子结构调控等策略;(2)催化剂-电解液界面形貌调控、表面化学、电解液环境调控等策略;(3)催化剂-气体界面疏气性调控、外场作用等策略.从反应机理研究、膜电极界面设计及电解槽界面性质调控三个角度对电解水反应界面工程未来的发展与应用提出了建议及展望.在反应机理方面,大电流条件下的界面性质如界面电阻、传质行为等仍需更深入的认识.在膜电极中,催化剂、离子交换膜、离子型聚合物、气体扩散层所形成的多元界面,尤其是催化剂-膜界面、催化剂-气体扩散层界面的结构仍需进一步优化以提升膜电极的活性及稳定性.在电解槽界面性质调控方面,催化剂-基底界面结合力等参数与催化剂寿命间的关系,电解过程中界面处的温度场及流场分布,适配于实际生产系统的电流密度等仍需深入研究.综上,本文从基本物理化学过程、策略及作用、挑战与展望等多个方面介绍了界面工程.本文有助于研究人员理解非均相电化学反应过程中界面的重要作用,提出催化剂、膜电极、电解槽界面设计新策略,并开发新型表征方法以深入对界面性质的认识,推动高效电解水技术的开发及应用.

探测激子极化激元在超薄范德华微晶中的光传播

激子极化激元是一种准粒子,过渡金属二硫族化合物材料即使在室温下也能支持传播激子极化子,是非常好的纳米光子学研究平台.已有研究表明,通过散射型扫描近场光学显微镜可以对过渡金属二硫族化合物薄片中激子极化激元进行实空间探测,但波导厚度仅限于低至30 nm.本文采用三种不同波长的入射光(1550和1064 nm的近红外以及633 nm的可见光),通过基于原子力显微镜的散射型扫描近场光学显微镜测量,探测到MoS2和WSe2薄片中激子极化子普通横电模式的纳米光学成像.在厚度分别低至~3 nm(相当于4原子层)和~8 nm(相当于12原子层)的超薄MoS2和WSe2薄片上,可以清楚地观察到干涉条纹图案,大大打破了之前的测量厚度限制.当厚度接近几个原子层时,波矢量始终保持在1.6k0~1.7k0左右,而不是理论预言的1k0.这些模式的特性表明,体系是由近乎悬浮的过渡金属二硫族化合物薄片的三层对称波导构成,其对激子极性子的传播产生限域效应.研究结果为探索基于超薄过渡金属二硫族化合物材料的近红外区极化器件提供了深入的理解和开辟了新的途径.

Atomically Substitutional Engineering of Transition Metal Dichalcogenide Layers for Enhancing Tailored Properties and Superior Applications

Transition metal dichalcogenides(TMDs)are a promising class of layered materials in the post-graphene era,with extensive research attention due to their diverse alternative elements and fascinating semiconductor behavior.Binary MX2 layers with different metal and/or chalcogen elements have similar structural parameters but varied optoelectronic properties,providing opportunities for atomically substitutional engineering via partial alteration of metal or/and chalcogenide atoms to produce ternary or quaternary TMDs.The resulting multinary TMD layers still maintain structural integrity and homogeneity while achieving tunable(opto)electronic properties across a full range of composition with arbitrary ratios of introduced metal or chalcogen to original counterparts(0–100%).Atomic substitution in TMD layers offers new adjustable degrees of freedom for tailoring crystal phase,band alignment/structure,carrier density,and surface reactive activity,enabling novel and promising applications.This review comprehensively elaborates on atomically substitutional engineering in TMD layers,including theoretical foundations,synthetic strategies,tailored properties,and superior applications.The emerging type of ternary TMDs,Janus TMDs,is presented specifically to highlight their typical compounds,fabrication methods,and potential applications.Finally,opportunities and challenges for further development of multinary TMDs are envisioned to expedite the evolution of this pivotal field.

Unveiling the pressure-driven metal–semiconductor–metal transition in the doped TiS_(2)

Conventional theories expect that materials under pressure exhibit expanded valence and conduction bands,leading to increased electrical conductivity.Here,we report the electrical properties of the doped 1T-TiS_(2) under high pressure by electrical resistance investigations,synchrotron x-ray diffraction,Raman scattering and theoretical calculations.Up to 70 GPa,an unusual metal-semiconductor-metal transition occurs.Our first-principles calculations suggest that the observed anti-Wilson transition from metal to semiconductor at 17 GPa is due to the electron localization induced by the intercalated Ti atoms.This electron localization is attributed to the strengthened coupling between the doped Ti atoms and S atoms,and the Anderson localization arising from the disordered intercalation.At pressures exceeding 30.5 GPa,the doped TiS_(2) undergoes a re-metallization transition initiated by a crystal structure phase transition.We assign the most probable space group as P2_12_12_1.Our findings suggest that materials probably will eventually undergo the Wilson transition when subjected to sufficient pressure.

Two-Dimensional Transition Metal Dichalcogenides and Their Charge Carrier Mobilities in Field-Effect Transistors

Two-dimensional(2D) materials have attracted extensive interest due to their excellent electrical, thermal,mechanical, and optical properties. Graphene has been one of the most explored 2D materials. However, its zero band gap has limited its applications in electronic devices. Transition metal dichalcogenide(TMDC), another kind of 2D material,has a nonzero direct band gap(same charge carrier momentum in valence and conduction band) at monolayer state,promising for the efficient switching devices(e.g., field-effect transistors). This review mainly focuses on the recent advances in charge carrier mobility and the challenges to achieve high mobility in the electronic devices based on 2DTMDC materials and also includes an introduction of 2D materials along with the synthesis techniques. Finally, this review describes the possible methodology and future prospective to enhance the charge carrier mobility for electronic devices.

Photodetectors based on junctions of two-dimensional transition metal dichalcogenides

Transition metal dichalcogenides （TMDCs） have gained considerable attention because of their novel properties and great potential applications. The flakes of TMDCs not only have great light absorption from visible to near infrared, but also can be stacked together regardless of lattice mismatch like other two-dimensional （2D） materials. Along with the studies on intrinsic properties of TMDCs, the junctions based on TMDCs become more and more important in applications of photodetection. The junctions have shown many exciting possibilities to fully combine the advantages of TMDCs, other 2D materials, conventional and organic semiconductors together. Early studies have greatly enriched the application of TMDCs in photodetection. In this review, we investigate the efforts in photodetectors based on the junctions of TMDCs and analyze the properties of those photodetectors. Homojunctions based on TMDCs can be made by surface chemical doping, elemental doping and electrostatic gating. Heterojunction formed between TMDCs/2D materials, TMDCs/conventional semiconductors and TMDCs/organic semiconductor also deserve more attentions. We also compare the advantages and disadvantages of different junctions, and then give the prospects for the development of junctions based on TMDCs.

Electronic structure of transition metal dichalcogenides PdTe_2 and Cu_(0.05)PdTe_2 superconductors obtained by angle-resolved photoemission spectroscopy

The layered transition metal chalcogenides have been a fertile land in solid state physics for many decades. Various MX2-type transition metal dichalcogenides, such as WTe2, IrTe2, and MoS2, have triggered great attention recently, either for the discovery of novel phenomena or some extreme or exotic physical properties, or for their potential applications. PdTe2 is a superconductor in the class of transition metal dichalcogenides, and superconductivity is enhanced in its Cu- intercalated form, Cuo.05PdTe2. It is important to study the electronic structures of PdTe2 and its intercalated form in order to explore for new phenomena and physical properties and understand the related superconductivity enhancement mecha- nism. Here we report systematic high resolution angle-resolved photoemission （ARPES） studies on PdTe2 and Cuo.05PdTe2 single crystals, combined with the band structure calculations. We present in detail for the first time the complex multi-band Fermi surface topology and densely-arranged band structure of these compounds. By carefully examining the electronic structures of the two systems, we find that Cu-intercalation in PdTe2 results in electron-doping, which causes the band structure to shift downwards by nearly 16 meV in Cuo.05PdTe2. Our results lay a foundation for further exploration and investigation on PdTe2 and related superconductors.

Electronic structures and elastic properties of monolayer and bilayer transition metal dichalcogenides MX_2(M= Mo,W;X= O,S,Se,Te):A comparative first-principles study

First-principle calculations with different exchange-correlation functionals, including LDA, PBE, and vd W-DF functional in the form of opt B88-vd W, have been performed to investigate the electronic and elastic properties of twodimensional transition metal dichalcogenides（TMDCs） with the formula of MX2（M = Mo, W; X = O, S, Se, Te） in both monolayer and bilayer structures. The calculated band structures show a direct band gap for monolayer TMDCs at the K point except for MoO2 and WO2. When the monolayers are stacked into a bilayer, the reduced indirect band gaps are found except for bilayer WTe2, in which the direct gap is still present at the K point. The calculated in-plane Young moduli are comparable to that of graphene, which promises possible application of TMDCs in future flexible and stretchable electronic devices. We also evaluated the performance of different functionals including LDA, PBE, and opt B88-vd W in describing elastic moduli of TMDCs and found that LDA seems to be the most qualified method. Moreover, our calculations suggest that the Young moduli for bilayers are insensitive to stacking orders and the mechanical coupling between monolayers seems to be negligible.

Catalyst activation: Surface doping effects of group Ⅵ transition metal dichalcogenides towards hydrogen evolution reaction in acidic media

Two-dimensional(2D) transition metal dichalcogenides(TMDs) have emerged as promising alternatives to the platinum-based catalysts for hydrogen evolution reaction(HER). The edge site of these2D materials exhibits HER-active properties, whereas the large-area basal plane is inactive.Therefore, recent studies and methodologies have been investigated to improve the performance of TMD-based materials by activating inactive sites through elemental doping strategies. In this review,we focus on the metal and non-metal dopant effects on group VI TMDs such as MoS_(2) MoSe_(2) WS_(2)and WSe_(2) for promoting HER performances in acidic electrolytes. A general introduction to the HER is initially provided to explain the parameters in accessing the catalytic performance of dopedTMDs. Then, synthetic methods for doped-TMDs and their HER performances are introduced in order to understand the effect of various dopants including metallic and non-metallic elements. Finally, the current challenges and future opportunities are summarized to provide insights into developing highly active and stable doped-TMD materials and valuable guidelines for engineering TMD-based nanocatalysts for practical water splitting technologies.

Dual bound states in the continuum enhanced second harmonic generation with transition metal dichalcogenides monolayer

The emergence of two dimensional(2D)materials has opened new possibilities for exhibiting second harmonic genera-tion(SHG)at the nanoscale,due to their remarkable optical response related to stable excitons at room temperature.However,the ultimate atomic-scale interaction length with light makes the SHG of Transition Metal Dichalcogenides(TM-Ds)monolayers naturally weak.Here,we propose coupling a monolayer of TMDs with a photonic grating slab that works with doubly resonant bound states in the continuum(BIC).The BIC slabs are designed to exhibit a pair of BICs,reson-ant with both the fundamental wave(FW)and the second harmonic wave(SHW).Firstly,the spatial mode matching can be fulfilled by tilting FW's incident angle.We theoretically demonstrate that this strategy leads to more than four orders of magnitude enhancement of SHG efficiency than a sole monolayer of TMDs,under a pump light intensity of 0.1 GW/cm^(2).Moreover,we demonstrate that patterning the TMDs monolayer can further enhance the spatial overlap coefficient,which leads to an extra three orders of magnitude enhancement of SHG efficiency.These results demonstrate remarkable pos-sibilities for enhancing SHG with nonlinear 2D materials,opening many opportunities for chip-based light sources,nano-lasers,imaging,and biochemical sensing.

In situ TEM revealing the effects of dislocations on lithium-ion migration in transition metal dichalcogenides

The two-dimensional (2D) structure of layered transition metal dichalcogenides (TMDs) provides unusual physical properties [1,2]and chemical reactivity [3,4], which can be influenced by defects such as dislocations [5,6]. For example, dislocations can act as nucleation sites for the onset of deformation when subjected to stress [7].

Two-dimensional transition metal dichalcogenides for lead halide perovskites-based photodetectors: band alignment investigation for the case of CsPbBr3/MoSe2

The distinguished electronic and optical properties of lead halide perovskites(LHPs)make them good candidates for active layer in optoelectronic devices.Integrating LHPs and two-dimensional(2 D)transition metal dichalcogenides(TMDs)provides opportunities for achieving increased performance in heterostructured LHPs/TMDs based optoelectronic devices.The electronic structures of LHPs/TMDs heterostructures,such as the band offsets and interfacial interaction,are of fundamental and technological interest.Here CsPbBr3 and MoSe2 are taken as prototypes of LHPs and 2 D TMDs to investigate the band alignment and interfacial coupling between them.Our GGA-PBE and HSE06 calculations reveal an intrinsic type-II band alignment between CsPbBr3 and MoSe2.This type-II band alignment suggests that the performance of CsPbBr3-based photodetectors can be improved by incorporating MoSe2 monolayer.Furthermore,the absence of deep defect states at CsPbBr3/MoSe2 interfaces is also beneficial to the better performance of photodetectors based on CsPbBr3/MoSe2 heterostructure.This work not only offers insights into the improved performance of photodetectors based on LHPs/TMDs heterostructures but it also provides guidelines for designing high-efficiency optoelectronic devices based on LHPs/TMDs heterostructures.

Transition Metal Dichalcogenides(WS2 and MoS2)Saturable Absorbers for Mode-Locked Erbium-Doped Fiber Lasers

We demonstrate an ultrafast fiber laser based on transition metal dichalcogenide materials which are tungsten disulfide (WS2) and molybdenum disulfide (MoS2) as saturable absorber (SA). These materials are fabricated via a simple drop-casting method. By employing WS2, we obtain a stable harmonic mode-locking at the threshold pump power of 184 mW, and the generated soliton pulse has 3.48 MHz of repetition rate. At the maximum pump power of 250 mW, we also obtain a small value of pulse duration, 2.43 ps with signal-to-noise ratio (SNR) of 57 dB. For MoS2 SA, the pulse is generated at 105 mW pump power with repetition rate of 1.16 MHz. However, the pulse duration cannot be detected by the autocorrelator device as the pulse duration recorded is 468 ns, with the SNR value of 35 dB.