RESUMO
Herein we report the successful doping of tellurium (Te) into molybdenum disulfide (MoS2) monolayers to form MoS2x Te2(1-x) alloy with variable compositions via a hydrogen-assisted post-growth chemical vapor deposition process. It is confirmed that H2 plays an indispensable role in the Te substitution into as-grown MoS2 monolayers. Atomic-resolution transmission electron microscopy allows us to determine the lattice sites and the concentration of introduced Te atoms. At a relatively low concentration, tellurium is only substituted in the sulfur sublattice to form monolayer MoS2(1-x)Te2x alloy, while with increasing Te concentration (up to â¼27.6% achieved in this study), local regions with enriched tellurium, large structural distortions, and obvious sulfur deficiency are observed. Statistical analysis of the Te distribution indicates the random substitution. Density functional theory calculations are used to investigate the stability of the alloy structures and their electronic properties. Comparison with experimental results indicate that the samples are unstrained and the Te atoms are predominantly substituted in the top S sublattice. Importantly, such ultimately thin Janus structure of MoS2(1-x)Te2x exhibits properties that are distinct from their constituents. We believe our results will inspire further exploration of the versatile properties of asymmetric 2D TMD alloys.
RESUMO
Direct observation of atomic migration both on and below surfaces is a long-standing but important challenge in materials science as diffusion is one of the most elementary processes essential to many vital material behaviors. Probing the kinetic pathways, including metastable or even transition states involved down to atomic scale, holds the key to the underlying physical mechanisms. Here, we applied aberration-corrected transmission electron microscopy (TEM) to demonstrate direct atomic-scale imaging and quasi-real-time tracking of diffusion of Mo adatoms and vacancies in monolayer MoS2, an important two-dimensional transition metal dichalcogenide (TMD) system. Preferred kinetic pathways and the migration potential-energy landscape are determined experimentally and confirmed theoretically. The resulting three-dimensional knowledge of the atomic configuration evolution reveals the different microscopic mechanisms responsible for the contrasting intrinsic diffusion rates for Mo adatoms and vacancies. The new insight will benefit our understanding of material processes such as phase transformation and heterogeneous catalysis.
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In this work, we have demonstrated the synthesis of high-quality monolayered α-In2Se3 using physical vapor deposition method under atmospheric pressure. The quality of the In2Se3 atomic layers has been confirmed by complementary characterization technologies such as Raman/photoluminescence spectroscopies and atomic force microscope. The atomically resolved images have been obtained by the annular dark-field scanning transmission electron microscope. The field-effect transistors have been fabricated using the atomically layered In2Se3 and exhibit p-type semiconducting behaviors with the mobility up to 2.5 cm(2)/ Vs. The In2Se3 layers also show a good photoresponsivity of 340A/W, as well as 6 ms response time for the rise and 12 ms for the fall. These results make In2Se3 atomic layers a promising candidate for the optoelectronic and photosensitive device applications.
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Controlled stacking of different two-dimensional (2D) atomic layers will greatly expand the family of 2D materials and broaden their applications. A novel approach for synthesizing MoS2 /WS2 heterostructures by chemical vapor deposition has been developed. The successful synthesis of pristine MoS2 /WS2 heterostructures is attributed to using core-shell WO3-x /MoO3-x nanowires as a precursor, which naturally ensures the sequential growth of MoS2 and WS2 . The obtained heterostructures exhibited high crystallinity, strong interlayer interaction, and high mobility, suggesting their promising applications in nanoelectronics. The stacking orientations of the two layers were also explored from both experimental and theoretical aspects. It is elucidated that the rational design of precursors can accurately control the growth of high-quality 2D heterostructures. Moreover, this simple approach opens up a new way for creating various novel 2D heterostructures by using a large variety of heteronanomaterials as precursors.
RESUMO
The microscopic process of oxidative etching of two-dimensional molybdenum disulfide (2D MoS2) at an atomic scale is investigated using a correlative transmission electron microscope (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.
RESUMO
As a common type of structural defect, grain boundaries (GBs) play an important role in tailoring the physical and chemical properties of bulk crystals and their two-dimensional (2D) counterparts such as graphene and molybdenum disulfide (MoS2). In this study, we explore the atomic structures and dynamics of three kinds of high-symmetry GBs (α, ß and γ) in monolayer MoS2. Atomic-resolution transmission electron microscopy (TEM) is used to characterize their formation and evolutionary dynamics, and atomistic simulation based analysis explains the size distribution of α-type GBs observed under TEM and the inter-GB interaction, revealing the stabilization mechanism of GBs by pre-existing sulfur vacancies. The results elucidate the correlation between the observed GB dynamics and the migration of sulfur atoms across GBs via a vacancy-mediated mechanism, offering a new perspective for GB engineering in monolayer MoS2, which may be generalized to other transition metal dichalcogenides.
RESUMO
Defects usually play an important role in tailoring various properties of two-dimensional materials. Defects in two-dimensional monolayer molybdenum disulphide may be responsible for large variation of electric and optical properties. Here we present a comprehensive joint experiment-theory investigation of point defects in monolayer molybdenum disulphide prepared by mechanical exfoliation, physical and chemical vapour deposition. Defect species are systematically identified and their concentrations determined by aberration-corrected scanning transmission electron microscopy, and also studied by ab-initio calculation. Defect density up to 3.5 × 10(13) cm(-2) is found and the dominant category of defects changes from sulphur vacancy in mechanical exfoliation and chemical vapour deposition samples to molybdenum antisite in physical vapour deposition samples. Influence of defects on electronic structure and charge-carrier mobility are predicted by calculation and observed by electric transport measurement. In light of these results, the growth of ultra-high-quality monolayer molybdenum disulphide appears a primary task for the community pursuing high-performance electronic devices.