Atomically Thin Twisted Heterostructure Optoelectronics Enhanced via vdW Interface Engineering

Abstract Two‐dimensional (2D) heterostructures have sparked widespread interest in physics and device applications. The interfacial band alignment engineering of 2D heterostructures opens promising routes for high‐performance electronics and optoelectronics. In this study, a 2D Te/MoS2 interface is engineered by tailoring the lattice mismatch and distance, which changed the band alignment. The photocurrent is significantly increased by optimizing the interface alignment. The corresponding device is designed to function as an ultrasensitive photodetector with a light on/off ratio of 104, responsivity of ≈1047 A W−1, and detectivity of >5 × 1012 Jones, as well as a spectral detection capability of up to 1550 nm. The proposed methods are robust and versatile and can be used to produce desired electronics; hence, this study may broaden the scope of 2D heterostructure optoelectronics.