Strong Coupling of Coherent Phonons to Excitons in Semiconducting Monolayer MoTe$_2$

Abstract

The coupling of the electron system to lattice vibrations and their time-dependent control and detection provides unique insight into the non-equilibrium physics of semiconductors. Here, we investigate the ultrafast transient response of semiconducting monolayer 2$H$-MoTe$_2$ encapsulated with $h$BN using broadband optical pump-probe microscopy. The sub-40-fs pump pulse triggers extremely intense and long-lived coherent oscillations in the spectral region of the A' and B' exciton resonances, up to $\sim$20% of the maximum transient signal, due to the displacive excitation of the out-of-plane $A_{1g}$ phonon. Ab-initio calculations reveal a dramatic rearrangement of the optical absorption of monolayer MoTe$_2$ induced by an out-of-plane stretching and compression of the crystal lattice, consistent with an $A_{1g}$-type oscillation. Our results highlight the extreme sensitivity of the optical properties of monolayer TMDs to small structural modifications and their manipulation with light.