Two-dimensional (2D) semiconducting transition metal dichalcogenides (TMDs) have emerged as attractive platforms in next-generation nanoelectronics and optoelectronics for reducing device sizes down to a 10 nm scale. To achieve this, the controlled synthesis of wafer-scale single-crystal TMDs with high crystallinity has been a continuous pursuit. However, previous efforts to epitaxially grow TMD films on insulating substrates (e.g., mica and sapphire) failed to eliminate the evolution of antiparallel domains and twin boundaries, leading to the formation of polycrystalline films. Herein, we report the epitaxial growth of wafer-scale single-crystal MoS2 monolayers on vicinal Au(111) thin films, as obtained by melting and resolidifying commercial Au foils. The unidirectional alignment and seamless stitching of the MoS2 domains were comprehensively demonstrated using atomic- to centimeter-scale characterization techniques. By utilizing onsite scanning tunneling microscope characterizations combined with first-principles calculations, it was revealed that the nucleation of MoS2 monolayer is dominantly guided by the steps on Au(111), which leads to highly oriented growth of MoS2 along the ⟨110⟩ step edges. This work, thereby, makes a significant step toward the practical applications of MoS2 monolayers and the large-scale integration of 2D electronics.

Achieving homogeneous phase transition and uniform charge distribution is essential for good cycle stability and high capacity when phase conversion materials are used as electrodes. Herein, we show that chemical lithiation of bulk 2H-MoS distorts its crystalline domains in three primary directions to produce mosaic-like 1T' nanocrystalline domains, which improve phase and charge uniformity during subsequent electrochemical phase conversion. 1T'-LiMoS, a macroscopic dense material with interconnected nanoscale grains, shows excellent cycle stability and rate capability in a lithium rechargeable battery compared to bulk or exfoliated-restacked MoS. Transmission electron microscopy studies reveal that the interconnected MoS nanocrystals created during the phase change process are reformable even after multiple cycles of galvanostatic charging/discharging, which allows them to play important roles in the long term cycling performance of the chemically intercalated TMD materials. These studies shed light on how bulk TMDs can be processed into quasi-2D nanophase material for stable energy storage.

As a new member of the MXene group, 2D Mo C has attracted considerable interest due to its potential application as electrodes for energy storage and catalysis. The large-area synthesis of Mo C film is needed for such applications. Here, the one-step direct synthesis of 2D Mo C-on-graphene film by molten copper-catalyzed chemical vapor deposition (CVD) is reported. High-quality and uniform Mo C film in the centimeter range can be grown on graphene using a Mo-Cu alloy catalyst. Within the vertical heterostructure, graphene acts as a diffusion barrier to the phase-segregated Mo and allows nanometer-thin Mo C to be grown. Graphene-templated growth of Mo C produces well-faceted, large-sized single crystals with low defect density, as confirmed by scanning transmission electron microscopy (STEM) measurements. Due to its more efficient graphene-mediated charge-transfer kinetics, the as-grown Mo C-on-graphene heterostructure shows a much lower onset voltage for hydrogen evolution reactions as compared to Mo C-only electrodes.

We report the fast growth of high-quality millimeter-size monolayer MoSe crystals on molten glass using an ambient pressure CVD system. We found that the isotropic surface of molten glass suppresses nucleation events and greatly improves the growth of large crystalline domains. Triangular monolayer MoSe crystals with sizes reaching ∼2.5 mm, and with a room-temperature carrier mobility up to ∼95 cm/(V·s), can be synthesized in 5 min. The method can also be used to synthesize millimeter-size monolayer MoS crystals. Our results demonstrate that "liquid-state" glass is a highly promising substrate for the low-cost growth of high-quality large-size 2D transition metal dichalcogenides (TMDs).

Among van der Waals layered ferromagnets, monolayer vanadium diselenide (VSe2) stands out due to its robust ferromagnetism. However, the exfoliation of monolayer VSe2 is challenging, not least because the monolayer flake is extremely unstable in air. Using an electrochemical exfoliation approach with organic cations as the intercalants, monolayer 1T‐VSe2 flakes are successfully obtained from the bulk crystal at high yield. Thiol molecules are further introduced onto the VSe2 surface to passivate the exfoliated flakes, which improves the air stability of the flakes for subsequent characterizations. Room‐temperature ferromagnetism is confirmed on the exfoliated 2D VSe2 flakes using a superconducting quantum interference device (SQUID), X‐ray magnetic circular dichroism (XMCD), and magnetic force microscopy (MFM), where the monolayer flake displays the strongest ferromagnetic properties. Se vacancies, which can be ubiquitous in such materials, also contribute to the ferromagnetism of VSe2, although density functional theory (DFT) calculations show that such effect can be minimized by physisorbed oxygen molecules or covalently bound thiol molecules.