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説明:

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.

権利情報:

• 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

キーワード: Nonlinear Optical Responses, Excitons, Fermi Polarons

刊行年月日: 2024-05-14

出版者: Springer Science and Business Media LLC

掲載誌:

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

研究助成金:

• 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

原稿種別: 著者最終稿 (Accepted manuscript)

MDR DOI:

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

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更新時刻: 2025-09-05 16:30:40 +0900

MDRでの公開時刻: 2025-09-05 16:19:24 +0900