An Atomically Resolved Schottky Barrier Height Approach for Bridging the Gap between Theory and Experiment at...

We propose an atomically resolved approach to capture the spatial variations of the Schottky barrier height (SBH) at metal-semiconductor heterojunctions. This proposed scheme, based on atom-specific partial density of states (PDOS) calculations, further enables calculation of the effective SBH that aligns with conductance measurements. We apply this approach to study the variations of SBH at MoS₂@Au heterojunctions, in which MoS₂ contains conducting and semiconducting grain boundaries (GBs). Our results reveal that there are significant variations in SBH at atoms in the defected heterojunctions. Of particular interest is the fact that the SBH in some areas with extended defects approaches zero, indicating Ohmic contact. One important implication of this finding is that the effective SBH should be intrinsically dependent on the defect density and character. Remarkably, the obtained effective SBH values demonstrate good agreement with existing experimental measurements. Thus, the present study addresses two long-standing challenges associated with SBH in MoS₂-metal heterojunctions: the wide variation in experimentally measured SBH values at MoS₂@metal heterojunctions and the large discrepancy between density-functional-theory-predicted and experimentally measured SBH values. Our proposed approach points out a valuable pathway for understanding and manipulating SBHs at metal-semiconductor heterojunctions.