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Synthesis of ultrahigh-quality monolayer molybdenum disulfide through in-situ defect healing with thiol molecules

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 Added by Bilu Liu
 Publication date 2020
  fields Physics
and research's language is English




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Monolayer transition metal dichalcogenides (TMDCs) are two-dimensional (2D) materials with many potential applications. Chemical vapour deposition (CVD) is a promising method to synthesize these materials. However, CVD-grown materials generally have poorer quality than mechanically exfoliated ones and contain more defects due to the difficulties in controlling precursors distribution and concentration during growth where solid precursors are used. Here, we propose to use thiol as a liquid precursor for CVD growth of high quality and uniform 2D MoS2. Atomic-resolved structure characterizations indicate that the concentration of sulfur vacancies in the MoS2 grown from thiol is the lowest among all reported CVD samples. Low temperature spectroscopic characterization further reveals the ultrahigh optical quality of the grown MoS2. Density functional theory simulations indicate that thiol molecules could interact with sulfur vacancies in MoS2 and repair these defects during the growth of MoS2, resulting in high quality MoS2. This work provides a facile and controllable method for the growth of high-quality 2D materials with ultralow sulfur vacancies and high optical quality, which will benefit their optoelectronic applications.



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Edge structures are highly relevant to the electronic, magnetic and catalytic properties of two-dimensional (2D) transition metal dichalcogenides (TMDs) and their one dimensional (1D) counterpart, i.e., nanoribbons, which should be precisely tailored for the desirable applications. In this work, we report the formation of novel Mo6S6 nanowire (NW) terminated edges in a monolayer molybdenum disulfide (MoS2) via an e-beam irradiation process combined with high temperature heating in a scanning transmission electron microscope (STEM). Atomic structures of NW terminated edges and the dynamic formation process were observed experimentally. Further analysis shows that NW terminated edge could form on both Mo-zigzag (ZZ) edge and S-ZZ edge which can exhibit even higher stability superior to the pristine zigzag (ZZ) and armchair (AC) edge. In addition, the analogous edge structures can be also formed in MoS2 nanoribbon and other TMDs material such as MoxW1-xSe2. We believe that the presence of these novel edge structures in 2D and 1D TMD materials may provide novel properties and new opportunities for their versatile applications including catalytic, spintronic and electronic devices.
The microscopic process of oxidative etching of two-dimensional molybdenum disulfide (2D MoS2) at an atomic scale is investigated using a correlative TEM-etching study. MoS2 flakes on graphene TEM grids are precisely tracked and characterized by TEM before and after the oxidative etching. This allows us to determine the structural change with an atomic resolution on the edges of the domains, of well-oriented triangular pits and along the grain boundaries. We observe that the etching mostly starts from the open edges, grain boundaries and pre-existing atomic defects. A zigzag Mo edge is assigned as the dominant termination of the triangular pits, and profound terraces and grooves are observed on the etched edges. Based on the statistical TEM analysis, we reveal possible routes for the kinetics of the oxidative etching in 2D MoS2, which should also be applicable for other 2D transition metal dichalcogenide materials like MoSe2 and WS2.
Doping is an effective way to modify the electronic property of two-dimensional (2D) materials and endow them with new functionalities. However, wide-range control of the substitutional doping concentration with large scale uniformity remains challenging in 2D materials. Here we report in-situ chemical vapor deposition growth of vanadium (V) doped monolayer molybdenum disulfide (MoS2) with widely tunable doping concentrations ranging from 0.3 to 13.1 at%. The key to regulate the doping concentration lies in the use of appropriate V precursors with different doping abilities, which also generate a large-scale uniform doping effect. Artificial synaptic transistors were fabricated by using the heavily doped MoS2 as the channel material for the first time. Synaptic potentiation, depression and repetitive learning processes are mimicked by the gate-tunable channel conductance change in such transistors with abundant V atoms to trap/detrap electrons. This work shows a feasible method to dope monolayer 2D semiconductors and demonstrates their use in artificial synaptic transistors.
The two-dimensional (2D) semiconductor molybdenum disulfide (MoS2) has attracted widespread attention for its extraordinary electrical, optical, spin and valley related properties. Here, we report on spin polarized tunneling through chemical vapor deposited (CVD) multilayer MoS2 (~7 nm) at room temperature in a vertically fabricated spin-valve device. A tunnel magnetoresistance (TMR) of 0.5 - 2 % has been observed, corresponding to spin polarization of 5 - 10 % in the measured temperature range of 300 - 75 K. First principles calculations for ideal junctions results in a tunnel magnetoresistance up to 8 %, and a spin polarization of 26 %. The detailed measurements at different temperatures and bias voltages, and density functional theory calculations provide information about spin transport mechanisms in vertical multilayer MoS2 spin-valve devices. These findings form a platform for exploring spin functionalities in 2D semiconductors and understanding the basic phenomenon that control their performance.
76 - S. H. Liang , Y. Lu , B. S. Tao 2015
Molybdenum disulfide has recently emerged as a promising two-dimensional semiconducting material for nano-electronic, opto-electronic and spintronic applications. However, demonstrating spin-transport through a semiconducting MoS2 channel is challenging. Here we demonstrate the electrical spin injection and detection in a multilayer MoS2 semiconducting channel. A magnetoresistance (MR) around 1% has been observed at low temperature through a 450nm long, 6 monolayer thick channel with a Co/MgO spin injector and detector. From a systematic study of the bias voltage, temperature and back-gate voltage dependence of MR, it is found that the hopping via localized states in the contact depletion region plays a key role for the observation of the two-terminal MR. Moreover, the electron spin-relaxation is found to be greatly suppressed in the multilayer MoS2 channel for in-plan spin injection. The underestimated long spin diffusion length (~235nm) and large spin lifetime (~46ns) open a new avenue for spintronic applications using multilayer transition metal dichalcogenides.
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