Hexagonal molybdenum diselenide (MoSe2) multilayers were grown by chemical vapor deposition (CVD). A relatively high pressure (>760 Torr) was used during the CVD growth to achieve multilayers by creating multiple nuclei based on the two-dimensional crystal growth model. Our CVD-grown multilayer MoSe2 thin-film transistors (TFTs) show p-type-dominant ambipolar behaviors, which are attributed to the formation of Se vacancies generated at the decomposition temperature (650 °C) after the CVD growth for 10 min. Our MoSe2 TFT with a reasonably high field-effect mobility (10 cm2/V · s) exhibits a high photoresponsivity (93.7 A/W) and a fast photoresponse time (τrise ~ 0.4 s) under the illumination of light, which demonstrates the practical feasibility of multilayer MoSe2 TFTs for photodetector applications.

Large-area and highly crystalline CVD-grown multilayer MoSe2 films exhibit a well-defined crystal structure (2H phase) and large grains reaching several hundred micrometers. Multilayer MoSe2 transistors exhibit high mobility up to 121 cm(2) V(-1) s(-1) and excellent mechanical stability. These results suggest that high mobility materials will be indispensable for various future applications such as high-resolution displays and human-centric soft electronics.

Local-gate multilayer MoS2 phototransistors exhibit a photoresponsivity of up to 342.6 A W(-1) , which is higher by 3 orders of magnitude than that of global-gate multilayer MoS2 phototransistors. These simulations indicate that the gate underlap is critical for the enhancement of the photoresponsivity. These results suggest that high photoresponsivity can be achieved in indirect-bandgap multilayer MoS2 phototransistors by optimizing the optoelectronic design.

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