Theoretical modeling of edge-controlled growth kinetics and structural engineering of 2D-MoSe₂

We introduce the first reactive force field (ReaxFF) for Mo/Se/H interactions, which enables large-scale molecular dynamics simulations of the synthesis, processing, and characterization of 2D-MoSe₂ and whose parameters are trained primarily on first-principles energetics data including both periodic and non-periodic calculations. This new potential elucidates the structural transition from metallic to semiconducting phases, the energetics of various defects, and the Se-vacancy migration barrier. A theoretical model developed based on this potential and the Wulff construction also describes an observed morphology evolution of 2D-MoSe₂ domains during growth. Since controllable edge-mediated growth kinetics of 2D-MoSe₂ are of great interest to the 2D community, we believe that this new ReaxFF potential trained against the edge formation energies of MoSe₂ nanoribbons with different Se coverages will be a powerful complementary tool to experimental studies by simulating the edge-growth kinetics of 2D-MoSe₂ at high speed and low cost.