Photoinduced Contact Evolution and Junction Rearrangement in Two‐Dimensional van der Waals Heterostructure

Abstract Devices based on 2DMs van der Waals (vdW) heterostructures always compose of multiple contacts. Due to the instability of nanoscale 2DMs and interfaces, these contacts can be affected by the operation‐induced photo or thermal effect. They can trigger the evolution of junctions and rearrange the junctions across a device, which are detrimental for applications. Herein, vdW heterostructure of indium selenide (InSe) and black phosphorus (BP) on Au electrodes are investigated to reveal the contact evolution and its relation to device performance. During operation, light irradiation changes the I–V characteristics from symmetry to strong rectification. Photocurrent mapping and Kelvin‐probe force microscopy (KPFM) reveal triple junctions in this heterostructure, i.e., Au‐InSe junction, InSe homojunction, and InSe‐BP heterojunction. The variation of I–V characteristics of vdW heterostructure is ascribed to the evolution of Au‐InSe junction from quasi‐ohmic junction with a near‐zero work function difference ( Δφ ) to a strong Schottky junction ( Δφ = ≈0.27 eV). The stabilized device demonstrates distinguished time‐domain response at individual junctions and overall device, indicating the evolution of contacts and the consequent opposite junction directions degrade the overall device performance. This research emphasizes the importance of dealing with heterogeneous contacts and junction directions in designing vdW heterostructure photodetectors.