Strong Coupling of Coherent Phonons to Excitons in Semiconducting Monolayer MoTe2

CJ Sayers, A Genco, C Trovatello, SD Conte… - Nano Letters, 2023 - ACS Publications
Nano Letters, 2023ACS Publications
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 H-MoTe2
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∼ 20% of the maximum transient signal …
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 2H-MoTe2 encapsulated with hBN 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 A1g phonon. Ab initio calculations reveal a dramatic rearrangement of the optical absorption of monolayer MoTe2 induced by an out-of-plane stretching and compression of the crystal lattice, consistent with an A1g -type oscillation. Our results highlight the extreme sensitivity of the optical properties of monolayer TMDs to small structural modifications and their manipulation with light.
ACS Publications
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