Anomalous Dynamics of Defect-Assisted Phonon Recycling in Few-Layer Mo0.5W0.5S2.

Abstract

Alloying has emerged as a new strategy to tune the function of 2D transition metal dichalcogenides (TMDCs). However, the lack of research on the electrical and structural properties of these alloys limits their practical applications. Here, femtosecond transient absorption spectroscopy with pump pulse tunability is performed to elucidate the ultrafast carrier dynamics in the few-layer Mo0.5W0.5S2 prepared by the liquid phase exfoliation method. An anomalous rebleaching of the ground state is observed at high pump fluence by 3.1 eV excitation. We ascribe this rebleaching of the ground state to the mechanism that the carriers trapped in the defect are thermally excited back to the untrapped exciton state due to the phonon recycling, which hinders the dissipation of nonradiative energy, through comparative experiments and global analysis. Our findings demonstrate a novel energy transfer channel assisted by defect in few-layer TMDCs which is critical for their advanced applications.