Correlation-driven nonequilibrium exciton site transition in a WSe2/WS2 moiré supercell

Jinjae Kim, Jiwon Park, Hyojin Choi, Taeho Kim, Soonyoung Cha, Yewon Lee, Kenji Watanabe, Takashi Taniguchi, Jonghwan Kim, Moon-Ho Jo and Hyunyong Choi ()
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Jinjae Kim: Seoul National University
Jiwon Park: Seoul National University
Hyojin Choi: Seoul National University
Taeho Kim: Pohang University of Science and Technology
Soonyoung Cha: University of California
Yewon Lee: Pohang University of Science and Technology
Kenji Watanabe: National Institute for Materials Science
Takashi Taniguchi: National Institute for Materials Science
Jonghwan Kim: Pohang University of Science and Technology
Moon-Ho Jo: Pohang University of Science and Technology
Hyunyong Choi: Seoul National University

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract Moiré superlattices of transition metal dichalcogenides offer a unique platform to explore correlated exciton physics with optical spectroscopy. Whereas the spatially modulated potentials evoke that the exciton resonances are distinct depending on a site in a moiré supercell, there have been no clear demonstration how the moiré excitons trapped in different sites dynamically interact with the doped carriers; so far the exciton-electron dynamic interactions were presumed to be site-dependent. Thus, the transient emergence of nonequilibrium correlations are open questions, but existing studies are limited to steady-state optical measurements. Here we report experimental fingerprints of site-dependent exciton correlations under continuous-wave as well as ultrashort optical excitations. In near-zero angle-aligned WSe2/WS2 heterobilayers, we observe intriguing polarization switching and strongly enhanced Pauli blocking near the Mott insulating state, dictating the dominant correlation-driven effects. When the twist angle is near 60°, no such correlations are observed, suggesting the strong dependence of atomic registry in moiré supercell configuration. Our studies open the door to largely unexplored nonequilibrium correlations of excitons in moiré superlattices.

Date: 2024
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DOI: 10.1038/s41467-024-47768-6

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