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Enhanced nonlinear interaction of polaritons via excitonic Rydberg states in monolayer WSe2

Jie Gu, Valentin Walther, Lutz Waldecker, Daniel Rhodes, Archana Raja, James C. Hone, Tony F. Heinz, Stéphane Kéna-Cohen, Thomas Pohl and Vinod M. Menon

Article (2021)

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Strong optical nonlinearities play a central role in realizing quantum photonic technologies. Exciton-polaritons, which result from the hybridization of material excitations and cavity photons, are an attractive candidate to realize such nonlinearities. While the interaction between ground state excitons generates a notable optical nonlinearity, the strength of such interactions is generally not sufficient to reach the regime of quantum nonlinear optics. Excited states, however, feature enhanced interactions and therefore hold promise for accessing the quantum domain of single-photon nonlinearities. Here we demonstrate the formation of exciton-polaritons using excited excitonic states in monolayer tungsten diselenide (WSe2) embedded in a microcavity. The realized excited-state polaritons exhibit an enhanced nonlinear response ∼g2spol−pol∼46.4±13.9μeVμm2 which is ∼4.6 times that for the ground-state exciton. The demonstration of enhanced nonlinear response from excited exciton-polaritons presents the potential of generating strong exciton-polariton interactions, a necessary building block for solid-state quantum photonic technologies.

Uncontrolled Keywords

Condensed-matter physics; Optical materials and structures

Subjects: 3100 Physics > 3100 Physics
3100 Physics > 3110 Optics (see also Photon devices, 2505)
Department: Department of Engineering Physics
Funders: National Science Foundation - MRSEC program DMR, ARO MURI program, Gordon and Betty Moore Foundation’s EPiQS Initiative, Alexander von Humboldt Foundation - Fellowship, Lawrence Berkeley National Laboratory - Laboratory Directed Research and Development Program, CRSNG / NERSC - Discovery Grant Program, Canada Research Chairs, Carlsberg Foundation - “Semper Ardens” Research Project QCooL, Deustche Forschungsgemeinschaft - SSP1929, European Commission - H2020-FETOPEN project ErBeStA, Danish National Research Foundation - Center of Excellence “CCQ”
Grant number: DMR 2011738, W911NF-17-1-0312, DMR-1708457, GBMF9462, DE-AC02-05CH11231, 800942, DNRF156
PolyPublie URL: https://publications.polymtl.ca/9284/
Journal Title: Nature Communications (vol. 12, no. 1)
Publisher: Springer Nature
DOI: 10.1038/s41467-021-22537-x
Official URL: https://doi.org/10.1038/s41467-021-22537-x
Date Deposited: 02 Sep 2022 13:58
Last Modified: 12 May 2024 12:01
Cite in APA 7: Gu, J., Walther, V., Waldecker, L., Rhodes, D., Raja, A., Hone, J. C., Heinz, T. F., Kéna-Cohen, S., Pohl, T., & Menon, V. M. (2021). Enhanced nonlinear interaction of polaritons via excitonic Rydberg states in monolayer WSe2. Nature Communications, 12(1), 7 pages. https://doi.org/10.1038/s41467-021-22537-x


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