Resolving Interface Barrier Deviation from the Schottky–Mott Rule: A Mitigation Strategy via Engineering MoS2–Metal van der Waals Contact

The Schottky barrier (SB) in the ultraclean van der Waals contact between two-dimensional (2D) MoS₂ and three-dimensional (3D) indium (In) strikingly deviates from the Schottky-Mott limit (SML). Herein, on the basis of first-principles calculation, the origin of the SB deviation is brought to bear, as well as a strategy for mitigating the SB deviation. In light of the good agreement between the SB and the corrected SB by interface potential difference (ΔV) and Fermi -level shift (ΔE_F) based on the SML, the SB deviation is attributed to the combined effects of ΔV and ΔE_F. Furthermore, when a Au, Sc, or Ti thin film is coated on the back side of In, the SB deviation and the sum of ΔV and ΔE_F decrease similarly. Importantly, in the Ti coating situation, the SB is reduced to 0.12 eV, notably smaller than the value of 0.30 eV in the Au coating case. This interface engineering can be generalized to regulate the SB between a 2D semiconductor and a 3D alloy.