Uncovering the Conduction Behavior of van der Waals Ambipolar Semiconductors

Abstract A long‐standing puzzle about van der Waals semiconductors (vdWS) is regarding the origin(s) of the conduction behavior they exhibit. Of particular interest are those with ambipolar conduction, which may provide an alternative choice for practical applications when considering the difficulties of doping the ultrathin bodies of vdWS. Here, the conduction behavior of ambipolar vdWS is analytically and theoretically studied. Using numerical simulation, it is shown that ambipolar vdWS can be fully captured by a Schottky‐barrier FET model. Based on this, it is found that the widely observed conduction polarity transition while changing the body thickness mainly comes from the tuning of band alignment at the metal/vdWS interfaces. This transition can be suppressed/inversed by introducing an inert hBN layer between the vdWS and the substrate. Through first‐principles calculations, it is demonstrated that metal/vdWS/substrate interactions play a crucial role in tuning the Schottky‐barrier heights, which finally determines the conduction behavior that ambipolar vdWS exhibit.