Computational Guide to Optimize Electric Conductance in MoS₂ Films

Molybdenum disulfide (MoS₂) is a high-potential material for nanoelectronic applications, especially when thinned to a few layers. Liquid-phase exfoliation enables large-scale fabrication of thin films comprising single- and few-layer flakes of MoS₂ or other transition-metal dichalcogenides (TMDCs), exhibiting variations in the flake size, geometry, edge terminations, and overlapping areas. Electronic conductivity of such films is thus determined by two contributions: the intraflake conductivity, reflecting the value of each single layer, and charge transport across these overlapping flakes. Employing first-principles simulations, we investigate the influence of various edge terminations and the overlap between flakes on the charge transport in MoS₂ film models. We identify characteristic electronic edge states originating from the edge atoms and their chemical environment, which resemble donor and acceptor states of doped semiconductors. This makes either electrons or holes to majority carriers and enables selective control over the dominant charge carrier type (n-type or p-type). Compared to pristine nanosheets, overlapping flakes exhibit lower overall conductance. In the best-performing hexagonal flakes occurring in Mo-rich environments, the conductance is reduced by 18% compared to the pristine layer, while the drop by 46% and 58% is predicted for truncated triangular and triangular flakes, respectively, in S-rich environments. An overlap of 6.5 nm is sufficient to achieve the highest possible interflake conductance. These findings allow for rational optimization of experimental conditions for the preparation of MoS₂ and other TMDC semiconducting thin films.