Inherent Resistance of Seed-Mediated Grown MoSe₂ Monolayers to Defect Formation

Recent progress in the chemical vapor deposition technique toward growing large-area and single-crystalline two-dimensional (2D) transition metal dichalcogenides (TMDs) has resulted in an electronic/optoelectronic device performance that rivals that of their top-down counterparts, despite the extensive use of hydrogen, a common reducing agent that readily generates defects in TMDs. Herein, we report that 2D MoSe₂ domains containing oxide seeds are resistant to hydrogen-induced defect generation. Specifically, we observed that the etching of the edges of seed-containing MoSe₂ was significantly less than that of pristine MoSe₂, without apparent seed particles, under the same H₂ annealing conditions. Our systematic approach for controlling the H₂ exposure time indicates that the oxidation of Mo and the edge roughening of seedless MoSe₂ coincidentally increase after H₂ exposure owing to the formation of Se vacancy followed by Mo oxidation, which is not the case with seed-containing MoSe₂. An ab initio calculation indicates that hydrogen preferentially adsorbs more onto O bonded to Mo than onto Se, providing further evidence of the resistance of seeded MoSe₂ to hydrogen etching. This finding provides an insight into controlling defect formation in 2D TMDs by employing sacrificial adsorption sites for reactive species (i.e., hydrogen).