Abstract
Nonequilibrium dynamics of TO phonons and low-frequency interlayer shear modes are mapped in femtosecond mid-infrared pump-probe experiments. Time-resolved changes of TO phonon absorption reveal a TO phonon lifetime of 1.2 ps, while the low-frequency excitations decay with a time constant of approximately 20 ps. The coupling of intralayer TO and interlayer motions manifests in a quasi-instantaneous redshift of the TO phonon resonance by some 10 cm −1. Theoretical calculations account for the coupling scenario and underline the relevance of inter-phonon interactions for the nonlinear phonon response of few-layer materials.