What Is the Role of a Magnetic Mo Antisite Defect on Carrier Relaxation and Spin Dynamics in 2-D MoS<sub>2</sub>?

Lei, Chengan; Qian, Zhao; Ma, Yandong; Ahuja, Rajeev · Nano Lett · 2025

basic_science · Level V

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Abstract

Antisite defects significantly influence the dynamic properties of monolayer MoS<sub>2</sub>, yet the carrier relaxation and spin dynamics in spin-polarized Mo antisite-defective MoS<sub>2</sub> remain unclear. Understanding these processes is crucial for advancing optoelectronic, spintronic, and valleytronic devices. Here, we employ first-principles calculations and <i>ab initio</i> nonadiabatic molecular dynamics with spin-orbit coupling (SOC) to explore carrier relaxation and spin dynamics in MoS<sub>2</sub> with a Mo antisite defect. This defect alters the material's magnetic properties, leading to distinct relaxation behaviors: electron relaxation is slower than hole relaxation, and charge carriers in different spin channels exhibit varied dynamics. These differences arise from variations in electron-phonon coupling, SOC strength, and phonon mode activation. Our findings provide key insights into charge and spin dynamics in MoS<sub>2</sub> with magnetic defects and suggest strategies to enhance the performance of next-generation optoelectronic, spintronic, and valleytronic devices.