Electronic Tuning in WSe₂/Au via van der Waals Interface Twisting and Intercalation

The transition metal dichalcogenide (TMD)–metal interfaces constitute an active part of TMD-based electronic devices with optimized performances. Despite their decisive role, current strategies for nanoscale electronic tuning remain limited. Here, we demonstrate electronic tuning in the WSe₂/Au interface by twist engineering, capable of modulating the WSe₂ carrier doping from an intrinsic p-type to n-type. Scanning tunneling microscope/spectroscopy gives direct evidence of enhanced interfacial interaction induced doping in WSe₂ as the twist angle with respect to the topmost (100) lattice of gold changing from 15 to 0°. Taking advantage of the strong coupling interface achieved this way, we have moved a step further to realize an n–p–n-type WSe₂ homojunction. The intrinsic doping of WSe₂ can be recovered by germanium intercalation. Density functional theory calculations confirm that twist angle and intercalation-dependent charge transfer related doping are involved in our observations. Our work offers ways for electronically tuning the metal–2D semiconductor interface.