Toward an understanding of the mechanism of mixed-salt-mediated CVD growth of MoSe2

The use of liquid precursors in chemical vapor deposition (CVD) techniques is advantageous for growing large-area, uniform two-dimensional (2D) transition-metal dichalcogenides (TMDs) compared to conventional methods using solid precursors. While various liquid precursors have been explored, recent studies highlight the use of mixed-salt precursors for growing uniform and wafer-scale TMDs. In this study, we propose a growth mechanism and present our findings on the epitaxial growth of MoSe2 domains as a function of annealing/growth time and H2 flow rate using Na2MoO4 and Na2SeO3 mixed-salt precursors. We confirm that the increase in the annealing time enhances the distribution of spin-coated precursors, leading to a rise in flake number density. On the other hand, prolonged growth time results in better-aligned MoSe2 flakes along the c-sapphire substrate step-edges. A significant finding is the dynamic diffusion of dendritic structures within large domains over the growth period, owing to the constant dissolution and recrystallization in the presence of residual liquid alloys. An increase in the H2 flow during CVD growth yields small, triangular domains aligned with the step edges, a result of the efficient reduction of precursor alloys and subsequent selenization. Our results provide an insight on achieving uniform and aligned morphology in CVD growth of 2D TMDs using liquid-phase precursors, a crucial step toward large-area fabrication.