Title: High-Throughput Computational Screening of All-MXene Metal–Semiconductor Junctions for Schottky-Barrier-Free Contacts with Weak Fermi-Level Pinning

Van der Waals (vdW) metal–semiconductor junctions (MSJs) exhibit huge potential to reduce the contact resistance and suppress the Fermi-level pinning (FLP) for improving the device performance, but they are limited by optional (2D) metals with a wide range of work functions. Here a new class of vdW MSJs entirely composed of atomically thin MXenes is reported. Using high-throughput first-principles calculations, highly stable 80 metals and 13 semiconductors are screened from 2256 MXene structures. The selected MXenes cover a broad range of work functions (1.8–7.4 eV) and bandgaps (0.8–3 eV), providing a versatile material platform for constructing all-MXene vdW MSJs. The contact type of 1040 all-MXene vdW MSJs based on Schottky barrier heights (SBHs) is identified. Unlike conventional 2D vdW MSJs, the formation of all-MXene vdW MSJs leads to interfacial polarization, which is responsible for the FLP and deviation of SBHs from the prediction of Schottky–Mott rule. Based on a set of screening criteria, six Schottky-barrier-free MSJs with weak FLP and high carrier tunneling probability (>50%) are identified. This work offers a new way to realize vdW contacts for the development of high-performance electronic and optoelectronic devices.