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Nonlinear interactions between excitons strongly coupled to light are key for accessing quantum many-body phenomena in polariton systems. Atomically-thin two-dimensional semiconductors provide an attractive platform for strong light-matter coupling owing to many controllable excitonic degrees of freedom. Among these, the recently emerged exciton hybridization opens access to unexplored excitonic species, with a promise of enhanced interactions. Here, we employ hybridized interlayer excitons (hIX) in bilayer MoS2 to achieve highly nonlinear excitonic and polaritonic effects. Such interlayer excitons possess an out-of-plane electric dipole as well as an unusually large oscillator strength allowing observation of dipolar polaritons (dipolaritons) in bilayers in optical microcavities. Compared to excitons and polaritons in MoS2 monolayers, both hIX and dipolaritons exhibit ≈ 8 times higher nonlinearity, which is further strongly enhanced when hIX and intralayer excitons, sharing the same valence band, are excited simultaneously. This gives rise to a highly nonlinear regime which we describe theoretically by introducing the concepts of inter- exciton phase space filling and hole crowding. The presented insight into many-body interactions provides new tools for accessing few-polariton quantum correlations.

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• Creative Commons BY Attribution 4.0 International
  

Keyword: Nonlinear interactions, exciton hybridization, bilayer MoS2

Date published: 2023-06-27

Publisher: Springer Science and Business Media LLC

Journal:

• Nature Communications (ISSN: 20411723) vol. 14 issue. 1 3818

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Manuscript type: Publisher's version (Version of record)

MDR DOI:

First published URL: https://doi.org/10.1038/s41467-023-39358-9

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Updated at: 2025-02-15 12:31:41 +0900

Published on MDR: 2025-02-15 12:31:42 +0900