Chemical Vapor Deposition Synthesis of MoS2 Layers from the Direct Sulfidation of MoO3 Surfaces Using Reactive Molecular Dynamics Simulations

Atomically thin MoS2 layer, a promising transition metal dichalcogenide (TMDC) material, has great potential for application in next-generation electronic and optoelectronic devices. Chemical vapor deposition (CVD) is the most effective technique for the synthesis of high-quality MoS2 layers. During CVD synthesis, monolayered MoS2 is generally synthesized by sulfidation of MoO3. Although qualitative reaction mechanisms for the sulfidation of MoO3 have been investigated by previous studies, the detailed reaction processes, including atomic-scale reaction pathways and growth kinetics, have yet to be fully understood. Here, we present quantum-mechanically informed and validated reactive molecular dynamics simulations of the direct sulfidation of MoO3 surfaces using S2 gas precursors. Our work clarifies the reaction mechanisms and kinetics of the sulfidation of MoO3 surfaces as follows: the reduction and sulfidation of MoO3 surfaces occur primarily at O-termination sites, followed by unsaturated Mo sites; the...