Liquid-Metal-Assisted Growth of Vertical GaSe/MoS2 p–n Heterojunctions for Sensitive Self-Driven Photodetectors

van der Waals (vdW) vertical p–n junctions based on two-dimensional (2D) materials have shown great potential in flexible, self-driven, high-efficiency electronic and optoelectronic applications. However, due to the complex nucleation dynamics, the controllable synthesis of vertical heterostructures remains a daunting challenge. Here, we report the controlled growth of vertical GaSe/MoS2 p–n heterojunctions via a liquid gallium (Ga)-assisted chemical vapor deposition method. The growth mechanism can be interpreted by theoretical calculations based on the Burton–Cabrera–Frank theory. By analyzing the diffusion barriers and the Ehrlich–Schwoebel barriers of adatoms, we found that the growth modes between vertical and lateral can be precisely switched by means of adjusting the amount of Ga. Based on the achieved high-quality vertical GaSe/MoS2 p–n heterojunctions, photosensing devices are further designed and systematically investigated. Upon light illumination, prominent photovoltaic effects with large open-circuit voltage (0.61 V) and broadband detection capability from 375 to 633 nm are observed, which can further be employed for self-powered photodetection with high responsivity (900 mA/W) and fast response speed (5 ms). The developed liquid-metal-assisted strategy provides an effective method for controllable synthesis of vdW heterostructures and will give impetus to their applications in high-performance optoelectronic device.