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Coherent Phonon-Mediated Many-Body Interaction in Monolayer WSe<sub>2</sub>

Jiading Zou, Ruidan Zhu, Jiayu Wang, Hanting Meng, Zhuan Wang, Hailong Chen, Yuxiang Weng

2023The Journal of Physical Chemistry Letters18 citationsDOI

Abstract

Due to the strong Coulomb interaction, the optical and electrical properties of two-dimensional transition metal dichalcogenides (TMDCs) are greatly determined by the emergence of many-body complexes such as excitons or trions. To fully realize the potential functionalities of these atomically thin materials, a comprehensive understanding of their many-body interaction mechanism is essential. Here, using the advanced femtosecond two-dimensional electronic spectroscopy technique combined with broadband transient absorption spectroscopy, a strong electron–exciton coupling effect in monolayer WSe 2 following the ultrafast photoexcitation is revealed. We demonstrate that such many-body complexes can be generated effectively through the band-edge optical excitation, with a ∼1.5 ps stabilization process. The coherent optical phonon plays a dominant role in this electron–exciton interaction, and the coherence of the electron (exciton)–phonon coupling can last for ∼4.5 ps. This finding offers new insight into the formation mechanism of photoinduced many-body complexes in TMDCs.

Topics & Concepts

PhotoexcitationExcitonMonolayerFemtosecondPhononMaterials scienceUltrashort pulseUltrafast laser spectroscopySpectroscopyCoulombFemtochemistryCondensed matter physicsCoupling (piping)Coherent spectroscopyElectronExcitationPhysicsNanotechnologyRaman spectroscopyOpticsRaman scatteringLaserCoherent anti-Stokes Raman spectroscopyQuantum mechanicsMetallurgy2D Materials and ApplicationsPerovskite Materials and ApplicationsGraphene research and applications
Coherent Phonon-Mediated Many-Body Interaction in Monolayer WSe<sub>2</sub> | Litcius