Role of defects in ultrafast charge recombination in monolayer MoS${}_2$

Abstract

In this work, we have systematically studied the role of point defects in the recombination time of monolayer MoS${}_2$ using time-dependent ab initio non-adiabatic molecular dynamics simulations. Various types of point defects, such as S vacancy, S interstitial, Mo vacancy and Mo interstitial have been considered. We show that defects strongly accelerate the electron-hole recombination, especially interstitial S atoms do that by 3 orders of magnitude higher compared to pristine MoS${}_2$. Mo defects (both vacancy and interstitial) introduce a multitude of de-excitation pathways via various defect levels in the energy gap. The results of this study provide some fundamental understanding of photoinduced de-excitation dynamics in presence of defects in highly technologically relevant 2D MoS${}_2$.

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