Exciton-polaron Rydberg states in monolayer MoSe2 and WSe2

Erfu Liu, Jeremiah Baren, Zhengguang Lu, Takashi Taniguchi, Kenji Watanabe, Dmitry Smirnov, Yia-Chung Chang () and Chun Hung Lui ()
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Erfu Liu: University of California
Jeremiah Baren: University of California
Zhengguang Lu: National High Magnetic Field Laboratory
Takashi Taniguchi: National Institute for Materials Science
Kenji Watanabe: National Institute for Materials Science
Dmitry Smirnov: National High Magnetic Field Laboratory
Yia-Chung Chang: Academia Sinica
Chun Hung Lui: University of California

Nature Communications, 2021, vol. 12, issue 1, 1-8

Abstract: Abstract Exciton polaron is a hypothetical many-body quasiparticle that involves an exciton dressed with a polarized electron-hole cloud in the Fermi sea. It has been evoked to explain the excitonic spectra of charged monolayer transition metal dichalcogenides, but the studies were limited to the ground state. Here we measure the reflection and photoluminescence of monolayer MoSe2 and WSe2 gating devices encapsulated by boron nitride. We observe gate-tunable exciton polarons associated with the 1 s–3 s exciton Rydberg states. The ground and excited exciton polarons exhibit comparable energy redshift (15~30 meV) from their respective bare excitons. The robust excited states contradict the trion picture because the trions are expected to dissociate in the excited states. When the Fermi sea expands, we observe increasingly severe suppression and steep energy shift from low to high exciton-polaron Rydberg states. Their gate-dependent energy shifts go beyond the trion description but match our exciton-polaron theory. Our experiment and theory demonstrate the exciton-polaron nature of both the ground and excited excitonic states in charged monolayer MoSe2 and WSe2.

Date: 2021
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DOI: 10.1038/s41467-021-26304-w

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