Ultrafast Energy Dissipation <i>via</i> Coupling with Internal and External Phonons in Two-Dimensional MoS₂

Abstract

Atomically thin two-dimensional materials have emerged as a promising system for optoelectronic applications; however, the low quantum yield, mainly caused by nonradiative energy dissipation, has greatly limited practical applications. To reveal the details for nonradiative energy channels, femtosecond pump-probe spectroscopy with a detection wavelength ranging from visible to near-infrared to mid-infrared is performed on few-layer MoS₂. With this method, the many-body effects, occupation effects, and phonon dynamics are clearly identified. In particular, thermalization of the MoS₂ lattice via electron-phonon scattering is responsible for a redshift of the exciton resonance energy observed within tens to hundreds of picoseconds after photoexcitation, which provides a direct real-time sensor for measuring the change in lattice temperature. We find that the excess energy from the cooling of hot carriers and the formation of bound carriers is efficiently transferred to the internal phonon system within 2 ps, while that from Shockley-Read-Hall recombination (∼9 ps) is mainly dissipated from the MoS₂ surfaces to external phonons.