Danhui Lv

Exploring atomic defects in molybdenum disulphide monolayers

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 × 1013 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.

Controlled Synthesis of High-Quality Monolayered α-In2Se3 via Physical Vapor Deposition

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.

Two‐Dimensional Layered Heterostructures Synthesized from Core–Shell Nanowires

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.

Capture the growth kinetics of CVD growth of two-dimensional MoS 2

Understanding the microscopic mechanism is fundamental for function-oriented controlled chemical vapor deposition growth of two-dimensional (2D) materials. In this work, we reveal the growth kinetics of 2D MoS2 by capturing the nucleation seeds, evolving morphology, edge structure, and edge terminations at the atomic scale during chemical vapor deposition growth using the transmission electron microscopy and scanning transmission electron microscopy. The direct growth of few-layer and mono-layer MoS2 onto graphene-based transmission electron microscopy grids helped us to perform the subsequent transmission electron microscopy characterization without any solution-based transfer. Two seeding centers are observed: (i) Mo-oxysulfide (MoOxS2−y) nanoparticles either in multi-shelled fullerene-like structures or as compact nanocrystals for the growth of fewer-layer MoS2; (ii) Mo-S atomic clusters. In the early stage growth, irregular polygons with two primary edge terminations, S-Mo Klein edges and Mo zigzag edges, appear approximately in equal numbers. The morphology evolves into a near-triangle shape in which Mo zigzag edges predominate. Results from density-functional theory calculations are consistent with the inferred growth kinetics, and thus support the growth mechanism we proposed. In general, the growth mechanisms found here should also be applicable in other 2D materials, such as MoSe2, WS2 and WSe2.2D molybdenum disulfide under the microscopeThe growth kinetics of two-dimensional (2D) molybdenum disulfide (MoS2) atomic layers has been captured using atomic-resolution transmission electron microscopy (TEM). In a regular process, 2D growth is usually performed on a silicon dioxide substrate. This makes studying the atomic-scale structures difficult because small layers can be damaged while transfering onto TEM grids. A team led by Chuanhong Jin at Zhejiang University, China, grew atomic layers of MoS2 directly on graphene-layer-based TEM grids in a regular chemical vapor deposition system. With this method intermediate and few-nanometer scale layers have been successfully monitored. These results are important for understanding the growth mechanism of MoS2 and other relevant 2D materials.

Direct Imaging of Kinetic Pathways of Atomic Diffusion in Monolayer Molybdenum Disulfide

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.

Advanced anodes composed of graphene encapsulated nano-silicon in a carbon nanotube network

High-capacity silicon-based anode materials with high conductivity to promote electron/ion transfer and excellent elasticity to alleviate volume expansion during repeated lithiation/delithiation process are highly desirable for next-generation lithium-ion batteries. Herein, we developed a facile in situ synthesis method based on chemical vapor deposition to fabricate Si-based nanocomposites integrated with interlinked graphene (Gra) and carbon nanotube (CNT). With melt-assembly nanosized Cu as the catalyst, hierarchical three-dimensional conductive Gra/CNT networks were in situ grown onto Si nanoparticles (SNPs) to achieve the Si@Gra@CNT composite. Such a hierarchical structure combines multiple advantages from SNPs with a super high capacity, Gra/CNT framework with continuous electrical conductivity, and void space for tolerance of Si volume expansion. Moreover, the SNPs were conformally encapsulated by few-layer Gra (fGra), which can protect the SNPs from direct exposure to electrolyte, resulting in a stable solid–electrolyte interface. As an anode material for Li-ion battery, the as-prepared Si@Gra@CNT composite exhibited a high initial specific capacity of 1197 mA h g−1 at a current density 2.0 A g−1 and ∼82% capacity retention over 1200 cycles, which was much better than those of Si@Gra and Si@CNT composites. The mechanism for the improved electrochemical performance was further analysed from the aspect of the synergetic effect arising from the construction components.

Atomic process of oxidative etching in monolayer molybdenum disulfide

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.

Hydrogen-assisted post-growth substitution of tellurium into molybdenum disulfide monolayers with tunable compositions

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 ∼27.6% 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.