Impact of Interface and Surface Oxide Defects on WS2 Electronic Properties from First Principles

The industrial-scale growth of dielectrics on top of a 2D material transistor channel without deterioration of its transport characteristics remains challenging today. Here, we investigate the origin of the performance degradation issue by constructing several atomistic interface models between a WS2 monolayer and an amorphous Al2O3 or HfO2 thin film. We then computed their properties using first-principles methods. We show that, while it is in principle possible to achieve a van der Waals interface between these materials, surface defects (e.g., undercoordinated metal atoms at the surface) are detrimental since they create localized states close to the bottom of the conduction band of WS2. Even in their absence, the inhomogeneity of the surface topology creates a nonuniform potential that is felt by charge carriers in WS2. While surface defects can potentially be kept under control with an appropriate oxide choice, the surface inhomogeneity appears to act as a bottleneck, limiting the performance of WS2 as a transistor channel and, in general, for all 2D materials.