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

TL;DR

This study uses advanced simulations to reveal how different point defects in monolayer MoS$_2$ significantly accelerate electron-hole recombination, especially sulfur interstitials, impacting its optoelectronic properties.

Contribution

It systematically analyzes the effects of various point defects on charge recombination times in monolayer MoS$_2$ using ab initio non-adiabatic molecular dynamics.

Findings

Sulfur interstitials increase recombination rates by 3 orders of magnitude.

Defects create additional de-excitation pathways via defect levels.

All studied defects accelerate electron-hole recombination.

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$_2$.