Suppressed Fermi Level Pinning and Wide-Range Tunable Schottky Barrier in CrX₃ (X = I, Br)/2D Metal Contacts

CrX3 (X = I, Br) monolayers exhibit outstanding performance in spintronic devices. However, the Schottky barrier at the CrX3/electrode interface severely impedes the charge injection efficiency. Herein, we propose two-dimensional (2D) metals as electrodes to form van der Waals (vdW) contact with CrX3 monolayers and systematically explore the contact properties of CrX3/metal by density functional theory (DFT) calculations. The results demonstrate that the strongly suppressed Fermi level pinning (FLP) effect and the wide-range tunable Schottky barrier can be achieved in CrX3/metal contacts. Specifically, the n-type and the p-type Schottky contacts can be realized in CrX3/metal contacts by choosing 2D metal electrodes with different work functions. Importantly, the pinning factors for CrX3/metal contacts are exceptionally larger than other commonly studied 2D semiconductors, indicating the strongly suppressed FLP in CrX3/metal contacts, which leads to the wide-range tunable Schottky barrier. Our findings provide guidance to the choice of electrodes and promote the development of CrX3-based spin devices.