Prediction of Hot Zone-center Optical Phonons in Laser Irradiated Molybdenum Disulfide with a Semiconductor Multitemperature Model

Abstract: Previous multitemperature model (MTM) resolving phonon temperatures at the polarization level and measurements have uncovered remarkable nonequilibrium among different phonon polarizations in laser irradiated graphene and metals. Here, we develop a semiconductor-specific MTM (SC-MTM) by including electron-hole pair generation, diffusion, and recombination, and show that a phonon polarization-level model does not yield observable polarization-based nonequilibrium in laser-irradiated molybdenum disulfide (MoS$_2$). In contrast, appreciable nonequilibrium is predicted between zone-center optical phonons and the other modes. The momentum-based nonequilibrium ratio is found to increase with decreasing laser spot size and interaction with a substrate. This finding is relevant to the understanding of the energy relaxation process in two-dimensional optoelectronic devices and Raman measurements of thermal transport.