Edge‐Mediated Annihilation of Vacancy Clusters in Monolayer Molybdenum Diselenide (MoSe₂) under Electron Beam Irradiation

Abstract Annihilation of vacancy clusters in monolayer molybdenum diselenide (MoSe₂) under electron beam irradiation is reported. In situ high‐resolution transmission electron microscopy observation reveals that the annihilation is achieved by diffusion of vacancies to the free edge near the vacancy clusters. Monte Carlo simulations confirm that it is energetically favorable for the vacancies to locate at the free edge. By computing the minimum energy path for the annihilation of one vacancy cluster as a case study, it is further shown that electron beam irradiation and pre‐stress in the suspended MoSe₂ monolayer are necessary for the vacancies to overcome the energy barriers for diffusion. The findings suggest a new mechanism of vacancy healing in 2D materials and broaden the capability of electron beam for defect engineering of 2D materials, a promising way of tuning their properties for engineering applications.