Strong Coupling of Coherent Phonons to Excitons in Semiconducting Monolayer MoTe<sub>2</sub>.

Sayers, Charles J; Genco, Armando; Trovatello, Chiara; Conte, Stefano Dal; Khaustov, Vladislav O; Cervantes-Villanueva, Jorge; Sangalli, Davide; Molina-Sanchez, Alejandro et al. · Nano Lett · 2023

basic_science · Level V

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Abstract

The coupling of the electron system to lattice vibrations and their time-dependent control and detection provide unique insight into the nonequilibrium physics of semiconductors. Here, we investigate the ultrafast transient response of semiconducting monolayer 2<i>H</i>-MoTe<sub>2</sub> encapsulated with <i>h</i>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 ∼20% of the maximum transient signal, due to the displacive excitation of the out-of-plane <i>A</i><sub>1g</sub> phonon. Ab initio calculations reveal a dramatic rearrangement of the optical absorption of monolayer MoTe<sub>2</sub> induced by an out-of-plane stretching and compression of the crystal lattice, consistent with an <i>A</i><sub>1g</sub> -type oscillation. Our results highlight the extreme sensitivity of the optical properties of monolayer TMDs to small structural modifications and their manipulation with light.