Abstract
Understanding the transition from nonplanar to planar clusters is crucial for the controllable synthesis of transition metal dichalcogenide (TMDC) monolayers. Using PtSe2 as a model, we investigate how the chemical environment influences the nucleation and growth stages of monolayer PtSe2 through structure searching and first-principles calculations. We established a comprehensive database of platinum selenide clusters (PtxSey, x = 1-10), analyzing 2095 unique clusters and identifying 191 stable isomers and 63 structures with the lowest formation energy on the convex hull. Our findings reveal a chemical environment-dependent phase transition from 3D structures to the planar T-phase of PtxSey clusters, representing an evolutionary route for PtSe2 growth. Clusters such as PtSe6, Pt2Se9, Pt3Se10, and Pt7Se10 in Pt-rich environments, as well as Pt2Se15 and Pt10Se32 in Se-rich environments, have been found to exhibit high stability. Additionally, the impact of varying chemical potentials of Pt and Se on the stability of these clusters is explored. PtSe4 and PtSe6 are found to be highly stable under most experimentally achievable chemical potential conditions and may serve as dominant precursors during PtSe2 growth. This work advances our understanding of the nucleation processes of PtSe2 and other T-phase TMDC materials.
Published Version
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