Vertically stacking two-dimensional (2D) materials can enable the design of novel electronic and optoelectronic devices and realize complex functionality. However, the fabrication of such artificial heterostructures on a wafer scale with an atomically sharp interface poses an unprecedented challenge. Here, we demonstrate a convenient and controllable approach for the production of wafer-scale 2D GaSe thin films by molecular beam epitaxy. In situ reflection high-energy electron diffraction oscillations and Raman spectroscopy reveal a layer-by-layer van der Waals epitaxial growth mode. Highly efficient photodetector arrays were fabricated, based on few-layer GaSe on Si. These photodiodes show steady rectifying characteristics and a high external quantum efficiency of 23.6%. The resultant photoresponse is super-fast and robust, with a response time of 60 μs. Importantly, the device shows no sign of degradation after 1 million cycles of operation. We also carried out numerical simulations to understand the underlying device working principles. Our study establishes a new approach to produce controllable, robust, and large-area 2D heterostructures and presents a crucial step for further practical applications.
Keywords: 2D materials; GaSe; molecular beam epitaxy; p-n junctions; photodiodes; van der Waals heterostructure.