Two-dimensional transition-metal dichalcogenides (TMDCs) possess unique electronic and optical properties, which open up a new opportunity for atomically thin optoelectronic devices. Synthesizing large-scale monolayer TMDCs on the SiO 2 /Si substrate is crucial for practical applications, however, it remains a big challenge. In this work, a method which combines chemical vapor deposition (CVD) and thermal evaporation was employed to grow monolayer tungsten disulfide (WS 2 ) crystals. Through controlling the density and the distribution of W precursors, a wafer-scale continuous uniform WS 2 film was achieved, with the structural and spectral characterizations confirming a monolayer configuration and a high crystalline quality. Wafer-scale field-effect transistor arrays based on the monolayer WS 2 were fabricated. The devices show superior electrical performances, and the maximal mobility is almost 1 order of magnitude higher than those of CVD-grown large-scale TMDC devices reported so far.

Among large numbers of transition metal dichalcogenides (TMDCs), monolayer rhenium disulfide (ReS2) is of particular interest due to its unique structural anisotropy, which opens up unprecedented opportunities in dichroic atomical electronics. Understanding the domain structure and controlling the anisotropic evolution of ReS2 during the growth is considered critical for increasing the domain size toward a large-scale growth of monolayer ReS2. Herein, by employing angle-resolved Raman spectroscopy, we reveal that the hexagonal ReS2 domain is constructed by six well-defined subdomains with each b-axis parallel to the diagonal of the hexagon. By further combining the first-principles calculations and the transmission electron microscopy (TEM) characterization, a dislocation-involved anisotropic evolution is proposed to explain the formation of the domain structures and understand the limitation of the domain size. Based on these findings, growth rates of different crystal planes are well controlled to enlarge the domain size, and moreover, single-crystal domains with a triangle shape are obtained. With the improved domain size, large-scale uniform, strictly monolayer ReS2 films are grown further. Scalable field-effect transistor (FET) arrays are constructed, which show good electrical performances comparable or even superior to that of the single domains reported at room temperature. This work not only sheds light on comprehending the novel growth mechanism of ReS2 but also offers a robust and controllable strategy for the synthesis of large-area and high-quality two-dimensional materials with low structural symmetry.

We perform a systematic investigation of MnPSe3/CrBr3 two-dimensional (2D) van der Waals heterostructures through first-principles calculations. The most stable stacking configuration of MnPSe3/CrBr3 heterostructures is found to have an indirect type-II band structure. Biaxial tensile strain is employed to tailor the spin–valley properties of the heterostructures in terms of the momentum, energy and spin components of the valleys. A novel opposite spin splitting evolution appears at the K and K′ valleys of the top valance band (TVB) with increasing tensile strain. A change from an indirect to a direct band gap is found at 7% tensile strain. A maximum spin splitting of 34.7 meV at the K′ valley is produced simultaneously with valley polarization under a tensile strain of 10%. The spin components distributed at the TVB are found to be controlled by strain-related competition between direct exchange interaction and indirect superexchange interaction of Se (px  +  py ) and Se pz orbitals. Spin polarization precisely regulated by strain can facilitate the manipulation of valley and spin degrees of freedom in MnPSe3/CrBr3 heterostructures, which opens up great potential for novel applications, such as strained sensor, spintronic and valleytronic devices.

Resonant plasmonic coupling has been considered as a promising strategy to enhance the optical response and manipulate the polarization of two-dimensional (2D) layer materials toward the practical applications. Here, a hybrid structure with periodic Ag nanoprism arrays was designed and fabricated on 2D GaSe layers to enhance these optical properties. By using the optimized hybrid structure with well-matched resonance, significant enhanced Raman scattering and band edge emission were successfully realized, and it is also interestingly found that the higher enhancement would be achieved while decreasing the thickness of GaSe layers. Theoretical simulation indicated that the strongly enhanced local field and the modified charge densities are the main reasons. By further introducing the patterned gratings on the plasmonic hybrid structure, selective excitation with controllable polarization was readily realized, besides the strongly enhanced photoluminescence intensity. This work provides a strategy for the plasmonic engineering of polarization controllable 2D optoelectronic devices.

In this work, the electronic and spintronic properties of GaSe/HfSe2 heterostructure under different strains are investigated through first-principles calculations. The results indicate that GaSe/HfSe2 heterostructure has an intrinsic type I band alignment, and the band structure is sensitive to the strain. A transition from type-I to type-II band alignment is found under a tensile stress. The evolution of the band structures is analyzed by the decomposed-projected band structures. Moreover, switchable spin textures of GaSe/HfSe2 heterostructure with different strains are also predicted. The controllable electronic spintronic properties of GaSe/HfSe2 heterostructure hold a great promise in applications of nanoelectronics and spintronics.