Magnetic switching of exciton lifetime in CrSBr

Abstract: Exciton dynamics in layered magnetic semiconductors provide a sensitive probe of the interplay between spin order and light-matter interaction. Here, we study thin CrSBr layers using time-resolved photoluminescence spectroscopy in an external magnetic field, revealing a step-like reduction in the exciton lifetime from 11 to 7 ps, during the magnetization flip from the antiferromagnetic to the ferromagnetic phase. The reduction of the exciton lifetime in the ferromagnetic phase persists below the Néel temperature, as evidenced by its strong magnetic-field dependence that disappears in the paramagnetic phase. Ab initio calculations reveal a one-dimensional nature of free excitons accompanied by a pronounced change in the oscillator strength across the magnetic phase transition predicting a shorter radiative lifetime of free excitons in the antiferromagnetic phase of CrSBr contradicting the experimental observations. This discrepancy is explained by strong localization of excitons at low tempature. We show both experimentally and theoretically that the observed magnetic switching of the exciton lifetime is attributed to a larger exciton localization volume leading to a larger oscillator strength in the ferromagnetic phase. The results show that disorder-induced localization effects play a key role in exciton dynamics in CrSBr.