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Twist-angle Dependent Optoelectronics in a few-layer Transition-Metal Dichalcogenides Heterostructure
摘要： Lattice matching has been supposed to play an important role in the coupling between two materials in vertical heterostructure (HS). To investigate this role, we fabricated a heterojunction device with a few layers of p-type WSe2 and n-type MoSe2 with different crystal orientation angles. The crystal orientations of WSe2 and MoSe2 were estimated by using high-resolution X-ray diffraction. Heterojunction devices were fabricated with twist angles of 0?, 15? and 30?. The I-V curve of the sample with the twist angle of 0° under the dark condition showed a diode-like behavior. The strong coupling due to lattice matching caused a well-established p-n junction. In cases of 15° and 30° samples, the van der Waals gap was built due to lattice mismatching, which resulted in the formation of a potential barrier. However, when the LED light of 365 nm (3.4 eV) was illuminated, excited electrons and holes were possible to jump beyond the potential barrier and the current flowed well in both forward and reverse directions. The effects of the twist angle were analyzed by spectral responsivity and external quantum efficiency, where it was found that the untwisted HS exhibited higher sensitivity under IR illumination while the twisting effect was not noticeable under UV illumination. From the photoluminescence and Raman spectroscopy, it was confirmed that the twisted HS showed a weak coupling due to the lattice mismatch.
关键词： p-n junction,optoelectronics,transition-metal dichalcogenides,heterostructure,a few-layer TMD,twist angle
更新于2025-09-04 15:30:14
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Chemical Vapor Deposition Growth of Single Crystalline CoTe <sub/>2</sub> Nanosheets with Tunable Thickness and Electronic Properties
摘要： Two-dimensional (2D) metallic transition metal dichalcogenides (MTMDs) have recently drawn increasing interest for fundamental studies and potential applications in catalysis, charge density wave (CDW), interconnections, spin-torque devices, as well superconductors. Despite some initial efforts, the thickness-tunable synthesis of atomically thin MTMDs remains a considerable challenge. Here we report controlled synthesis of 2D cobalt telluride (CoTe2) nanosheets with tunable thickness using an atmospheric pressure chemical vapor deposition (APCVD) approach and investigate their thickness-dependent electronic properties. The resulting nanosheets show a well-faceted hexagonal or triangular geometry with a lateral dimension up to ～200 μm. Systematic studies of growth at varying growth temperatures or flow rates demonstrate that nanosheets thickness is readily tunable from over 30 nm down to 3.1 nm. X-ray diffraction (XRD), transmission electron microscopy (TEM), and high-resolution scanning transmission electron microscope (STEM) studies reveal the obtained CoTe2 nanosheets are high-quality single crystals in the hexagonal 1T phase. Electrical transport studies show the 2D CoTe2 nanosheets display excellent electrical conductivities up to 4.0 × 105 S m?1 and very high breakdown current densities up to 2.1 × 107 A/cm2, both with strong thickness tunability.
关键词： Two-dimensional (2D),cobalt telluride (CoTe2),electronic properties,chemical vapor deposition (CVD),metallic transition metal dichalcogenides (MTMDs)
更新于2025-09-04 15:30:14
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1T-Phase Tungsten Chalcogenides (WS <sub/>2</sub> , WSe <sub/>2</sub> , WTe <sub/>2</sub> ) Decorated with TiO <sub/>2</sub> Nanoplatelets with Enhanced Electron Transfer Activity for Biosensing Applications
摘要： Layered transition metal dichalcogenides (TMDs) have received a great deal of attention due to fact that they have varied band gap, depending on their metal/chalcogen composition and on the crystal structure. Furthermore, these materials demonstrate great potential application in a myriad of electrochemical technologies. Heterogeneous electron transfer (HET) abilities of TMD materials toward redox-active molecules occupy a key role in their suitability for electrochemical devices. Herein, we introduce a promising biosensing strategy based on improved heterogeneous electron transfer rate of WS2, WSe2, and WTe2 nanosheets exfoliated using tert-butyllithium (t-BuLi) and n-butyllithium (n-BuLi) intercalators decorated with vertically aligned TiO2 nanoplatelets. By comparison of all the nanohybrids, decoration of TiO2 on t-BuLi WS2 (TiO2@t-BuLi WS2) results in the fastest HET rate of 5.39 × 10?3 cm s?1 toward ferri/ferrocyanide redox couple. In addition, the implications of decorating tungsten dichalcogenides (WX2) with TiO2 nanoplatelets in enzymatic biosensor applications for H2O2 detection are explored. TiO2@t-BuLi WS2 outperforms all other nanohybrid counterparts and is demonstrated to be an outstanding sensing platform in enzyme-based biosensor with wide linear range, low detection limit, and high selectivity. Such conceptually new electrocatalytic detection systems shall find the way to the next generation biosensors.
关键词： heterogeneous electron transfer,H2O2 detection,nanosheets,TiO2 nanoplatelets,transition metal dichalcogenides
更新于2025-09-04 15:30:14
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Exchange-driven intravalley mixing of excitons in monolayer transition metal dichalcogenides
摘要： Monolayer transition metal dichalcogenides (TMDCs) are promising two-dimensional (2D) semiconductors for application in optoelectronics. Their optical properties are dominated by two series of photo-excited exciton states—A (XA) and B (XB)1,2—that are derived from direct interband transitions near the band extrema. These exciton states have large binding energies and strong optical absorption3–6, and form an ideal system to investigate many-body effects in low dimensions. Because spin–orbit coupling causes a large splitting between bands of opposite spins, XA and XB are usually treated as spin-polarized Ising excitons, each arising from interactions within a specific set of states induced by interband transitions between pairs of either spin-up or spin-down bands (TA or TB). Here, by using monolayer MoS2 as a prototypical system and solving the first-principles Bethe–Salpeter equations, we demonstrate a strong intravalley exchange interaction between TA and TB, indicating that XA and XB are mixed states instead of pure Ising excitons. Using 2D electronic spectroscopy, we observe that an optical excitation of the lower-energy TA induces a population of the higher-energy TB, manifesting the intravalley exchange interaction. This work elucidates the dynamics of exciton formation in monolayer TMDCs, and sheds light on many-body effects in 2D materials.
关键词： intravalley exchange interaction,2D electronic spectroscopy,exciton states,many-body effects,monolayer transition metal dichalcogenides
更新于2025-09-04 15:30:14
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Effects of spin-orbit coupling on the optical response of a material
摘要： We investigate the effects of spin-orbit coupling on the optical response of materials. In particular, we study the effects of the commutator between the spin-orbit coupling part of the potential and the position operator on the optical matrix elements using density functional theory calculations within the generalized gradient approximation. By means of a formalism that separates a fully relativistic Kleinman-Bylander pseudopotential into the scalar-relativistic and spin-orbit-coupling parts, we calculate the contribution of the commutator arising from spin-orbit coupling to the squared optical matrix elements of isolated atoms, monolayer transition-metal dichalcogenides, and topological insulators. In the case of isolated atoms from H (Z = 1) to Bi (Z = 83), the contribution of spin-orbit coupling to the squared matrix elements can be as large as 14%. On the other hand, in the cases of monolayer transition-metal dichalcogenides and topological insulators, we find that this contribution is less than 1% and that it is sufficient to calculate the optical matrix elements and subsequent physical quantities without considering the commutator arising from spin-orbit coupling.
关键词： optical response,spin-orbit coupling,transition-metal dichalcogenides,topological insulators,density functional theory
更新于2025-09-04 15:30:14
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Piezotronics and piezo-phototronics in two-dimensional materials
摘要： This article discusses recent studies of piezotronics and piezo-phototronics of two-dimensional (2D) materials. Two-dimensional semiconductor materials have demonstrated excellent electronic and optoelectronic properties, and these ultrathin materials are candidates for next-generation devices. Among 2D semiconductors, transition-metal dichalcogenides in particular have large in-place piezoelectricity due to the noncentrosymmetry along the armchair direction. A strong coupling of piezoelectric and semiconducting properties has been reported for Schottky contacts and p–n junctions, even in single-layer materials. Since the carrier concentration of ultrathin 2D materials can be easily modulated by external piezocharges, layered composites of ferroelectric/2D materials also show promising piezotronic and piezo-phototronic properties.
关键词： piezo-phototronics,piezoelectricity,transition-metal dichalcogenides,piezotronics,two-dimensional materials
更新于2025-09-04 15:30:14
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Centimeter-Scale Nanoporous 2D Membranes and Ion Transport: Porous MoS2 Monolayers in a Few-Layer Matrix
摘要： Two-dimensional nanoporous membranes have received attention as catalysts for energy generation and membranes for liquid and gas purification but controlling their porosity and facilitating large-scale production is challenging. We show the growth and fabrication of cm-scale molybdenum disulfide (MoS2) membranes with tunable porous areas up to ~ 10% of the membrane and average nanopore diameters as large as ~ 30 nm, controlled by the etch time. We also measure ionic conductance between 0.1 and 16 μS per μm2 through variably-etched nanoporous membranes. Ensuring the mechanical robustness and large-area of the membrane, bilayer and few-layer regions form a strong supporting matrix around monolayer regions, observed by aberration-corrected scanning transmission electron microscopy. During etching, nanopores form in thin, primarily monolayer areas while thicker multi-layer regions remain essentially intact. Atomic-resolution imaging reveals that after exposure to the etchant, the number of V1Mo vacancies increases and nanopores form along grain boundaries in monolayers, suggesting that etching starts at intrinsic defect sites. This work provides an avenue for scalable production of nanoporous atomically thin membranes.
关键词： Transition metal dichalcogenides,molybdenum disulfide,nanoporous atomically thin membranes,defects,PAN etchant,nanopore
更新于2025-09-04 15:30:14
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2-Level Quantum Systems in 2-D Materials for Single Photon Emission
摘要： Single photon emission (SPE) by a solid state source requires presence of a distinct two-level quantum system, usually provided by point defects. Here we note that a number of qualities offered by novel, two dimensional materials—their all-surface openness and optical transparence, tighter quantum confinement, and reduced charge screening—are advantageous for achieving an ideal SPE. Based on first principles calculations and point-group symmetry analysis, a strategy is proposed to design paramagnetic defect complex with reduced symmetry, meeting all the requirements for SPE: its electronic states are well isolated from the host material bands, belong to a majority spin eigenstate, and can be controllably excited by polarized light. The defect complex is thermodynamically stable, and appears feasible for experimental realization, to serve as a SPE-source, essential for quantum computing, with ReMoVS in MoS2 as one most practical candidate.
关键词： diamane,boron nitride,ab initio,Photonic qubits,color centers,paramagnetic defects,transition metal dichalcogenides
更新于2025-09-04 15:30:14
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Theoretical Study of Auger Recombination of Excitons in Monolayer Transition-metal Dichalcogenides
摘要： Excitons are the most prominent features of the optical properties of monolayer transition-metal dichalcogenides(TMDC). In view of optoelectronics it is very important to understand the decay mechanisms of the excitons of these materials. Auger recombination of excitons are regarded as one of the dominant decay processes. In this paper the Auger constant of recombination is computed based on the approach proposed by Kavoulakis and Baym. We obtain both temperature dependent (from type A, A’ processes) and temperature independent (from type B, B’ processes) contributions, and a numerical estimate of theoretical result yields the value of constant in the order of 10?2 cm2s?1, being consistent with existing experimental data. This implies that Auger decay processes severely limit the photoluminescence yield of TMDC-based optoelectronic devices.
关键词： Auger recombination,Transition-metal dichalcogenides,Exciton
更新于2025-09-04 15:30:14
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Electron–phonon coupling in single-layer MoS2
摘要： The electron–phonon coupling strength in the spin–split valence band maximum of single-layer MoS2 is studied using angle-resolved photoemission spectroscopy and density functional theory-based calculations. Values of the electron–phonon coupling parameter λ are obtained by measuring the linewidth of the spin–split bands as a function of temperature and fitting the data points using a Debye model. The experimental values of λ for the upper and lower spin–split bands at K are found to be 0.05 and 0.32, respectively, in excellent agreement with the calculated values for a free-standing single-layer MoS2. The results are discussed in the context of spin and phase-space restricted scattering channels, as reported earlier for single-layer WS2 on Au(111). The fact that the absolute valence band maximum in single-layer MoS2 at K is almost degenerate with the local valence band maximum at Γ can potentially be used to tune the strength of the electron–phonon interaction in this material.
关键词： Density functional theory,Angle-resolved photoemission spectroscopy,Transition metal dichalcogenides,Electron-phonon coupling
更新于2025-09-04 15:30:14