From Metal-Organic Precursors to Coalesced Thin Films: A Predictive, End-to-End Atomistic Framework for MOCVD Multilayer TMD Growth
Year: 2026
Type: preprint
Abstract: Metal-organic chemical vapor deposition (MOCVD) enables scalable synthesis of layered two-dimensional semiconductors such as transition metal dichalcogenides (TMDs), yet the atomistic mechanisms linking precursor chemistry to multilayer nucleation and film evolution remain elusive, limiting synthesis control. Here, we establish a predictive mechanistic framework for multilayer TMD growth using MoS 2 as a representative system. Combining density functional theory, ReaxFF molecular dynamics, machine learning, and experimental validation, we reveal how metal antisites occupying chalcogen vacancies intrinsically form through surface interactions and serve as transient nucleation centers under experimentally relevant conditions. These defects stabilize epitaxial registry through covalent bonding and ultimately diffuse into the epilayer to form van der Waals interfaces. During this process, H 2 S vapor pressure influences metal-organic precursor decomposition by lowering the complete Mo(CO) 6 decomposition temperature, thereby promoting nucleation-center formation. This framework shifts layered-material synthesis from empirical trial-and-error toward predictive control, providing a computational route for growth of next-generation two-dimensional materials.
Source: ChemRxiv
Language: English
Subfield: Materials Chemistry
Field: Materials Science
Domain: Physical Sciences
Open Access status: green
OpenAlex ID: W7214609763