Phonon-Mediated Ultrafast Electron Relaxation Dynamics in Monolayer Black Phosphorus: Instantaneous Coherent...

Understanding carrier relaxation processes in semiconductors is crucial for designing high-performance optoelectronic and photocatalytic devices. Recent transient spectroscopic experiments on two-dimensional materials have revealed ultrafast optical responses within several tens of femtoseconds, which are usually ascribed to electron-electron scattering. Here, by conducting quantum dynamics simulations for monolayer black phosphorus, we show that electron-phonon scattering also profoundly influences the early stage of carrier dynamics. The photogenerated electron generally undergoes phonon-mediated instantaneous coherent delocalization in reciprocal space, accompanied by an entropy-driven sharp change in electronic energy. The distribution of the density of states controls the energy exchange between the electron and lattice vibrations. The phonon-induced quantum coherence significantly suspends the energy relaxation time, which is very beneficial for harvesting electron excess energy. These findings offer novel insights into the ultrafast carrier dynamics and energy flow in two-dimensional materials and may prompt new opportunities for regulation of carrier dynamic behaviors.