Article Giant optical nonlinearity of Fermi polarons in atomically thin semiconductors

Liuxin Gu ; Lifu Zhang ; Ruihao Ni ; Ming Xie ; Dominik S. Wild ; Suji Park ; Houk Jang ; Takashi Taniguchi SAMURAI ORCID (National Institute for Materials Science) ; Kenji Watanabe SAMURAI ORCID (National Institute for Materials Science) ; Mohammad Hafezi ; You Zhou

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Liuxin Gu, Lifu Zhang, Ruihao Ni, Ming Xie, Dominik S. Wild, Suji Park, Houk Jang, Takashi Taniguchi, Kenji Watanabe, Mohammad Hafezi, You Zhou. Giant optical nonlinearity of Fermi polarons in atomically thin semiconductors. Nature Photonics. 2024, 18 (8), 816-822. https://doi.org/10.1038/s41566-024-01434-x

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(abstract)

Realizing strong nonlinear optical responses is a long-standing goal of both fundamental and technological importance. Recently significant efforts have focused on exploring excitons in solids to achieve nonlinearities even down to few-photon levels. However, a crucial tradeoff arises as strong light-matter interactions require large oscillator strength and short radiative lifetime of excitons, which limits their nonlinearity. Here we experimentally demonstrate strong nonlinear optical responses with large oscillator strength by exploiting the coupling between excitons and carriers in an atomically thin semiconductor. By controlling the electric field and electrostatic doping of trilayer WSe2, we observe the hybridization between intralayer and interlayer excitons and the formation of Fermi polarons. Substantial optical nonlinearity is observed under continuous wave and pulsed laser excitation, where the Fermi polaron resonance blueshifts by as much as ~10 meV. Intriguingly, we observe a remarkable asymmetry in the optical nonlinearity between electron and hole doping, which is tunable by the applied electric field. We attribute these features to the optically induced valley polarization due to the interactions between excitons and free charges. Our results establish atomically thin heterostructures as a highly versatile platform for engineering nonlinear optical response with applications to classical and quantum optoelectronics.

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  • In Copyright
    This version of the article has been accepted for publication, after peer review (when applicable) and is subject to Springer Nature’s AM terms of use, but is not the Version of Record and does not reflect post-acceptance improvements, or any corrections. The Version of Record is available online at: http://dx.doi.org/10.1038/s41566-024-01434-x

Keyword: Nonlinear Optical Responses, Excitons, Fermi Polarons

Date published: 2024-05-14

Publisher: Springer Science and Business Media LLC

Journal:

  • Nature Photonics (ISSN: 17494893) vol. 18 issue. 8 p. 816-822

Funding:

  • U.S. Department of Energy DE-SC-0022885
  • U.S. Department of Energy DE-SC-0022885
  • U.S. Department of Energy DE-SC-0022885
  • U.S. Department of Energy DE-SC0012704
  • U.S. Department of Energy DE-SC0012704
  • NSF | Directorate for Mathematical & Physical Sciences | Division of Materials Research DMR-2145712
  • National Science Foundation DMR-2145712
  • MEXT | Japan Society for the Promotion of Science 20H00354
  • MEXT | Japan Society for the Promotion of Science 20H00354

Manuscript type: Author's version (Accepted manuscript)

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First published URL: https://doi.org/10.1038/s41566-024-01434-x

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Updated at: 2025-09-05 16:30:40 +0900

Published on MDR: 2025-09-05 16:19:24 +0900

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