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As an emerging two-dimensional (2D) semiconductor material, monolayer molybdenum disulfide (MoS2) films have a natural atomic-level thickness, excellent optoelectronic and mechanical properties, and have the potential to be used in very large-scale integration technology in the future. This article summarizes the progress made by our research group in the research of monolayer MoS2 films in the past few years. The controlled growth of large-size MoS2 single crystals has been achieved by oxygen-assisted chemical vapor deposition method. Through a unique facile multisource CVD growth method, the epitaxial growth of highly oriented and large domain size ML MoS2 films at a 4inch wafer scale is realized. Almost only 0 and 60° oriented domains are present in films, and the domain size, on average, is greater than 180 μm at the largest. The samples suggest their best optical and electrical quality ever obtained, as evidenced from their wafer-scale homogeneity, nearly perfect lattice structure, average room-temperature device mobility of 70 cm2V?1s?1 and high on/off ratio of 109 on SiO2 substrates. By adjusting the oxygen doping concentration of the MoS2 film with an effective CVD technique, a significant modulation on electrical and optical properties can be achieved, greatly improves carrier mobilities and controllable n-type electronic doping effects resulted from optimized oxygen doping levels of MoS2-xOx are revealed. In terms of MoS2 thin film devices and applications, the 4inch wafer-scale high-quality MoS2 monolayers are used to fabricate transparent MoS2-based transistors and logic circuits on flexible substrates. This large-area flexible FET device shows excellent electrical performance with a high device density (1,518 transistors per cm2) and yield (97%), and exhibit high on/off ratios (1010), current densities (~35μAμm?1), mobilities (~55cm2V-1s-1) and flexibility. Based on the vertically integrated multilayer devices via the layer-by-layer stacking process, an individual layer of all-2D multifunctional FETS are successfully achieved with nearly multiplied on-current density, equivalent device mobility, and persevered on/off ratio and SS of the individual layers, the combined performance of the device is fully utilized, and the integration of "sensing-storing-computing" is realized. A two-terminal floating-gate memory (2TFGM) based artificial synapse built from all-2D van der Waals materials is prepared, the 2TFGM synaptic device exhibits excellent linear and symmetric weight update characteristics with high reliability and tunability, A large number of states up to ≈3000, high switching speed of 40 ns and low energy consumption of 18 fJ for a single pulse have been demonstrated experimentally. The introduction of structural domain boundaries in the basal plane of monolayer MoS2 can greatly enhance its hydrogen evolution reaction performance by serving as active sites. The progress we have made in the preparation of monolayer MoS2 films and the research on device characteristics is of guiding significance for the basic and application research of MoS2, and is universal and instructive for other 2D transition metal dichalcogenides.

Cotrollable growth of monolayer MoS<sub>2</sub> films and their applications in devices