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 ()
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Jie Gu: City College of New York
Valentin Walther: Aarhus University
Lutz Waldecker: Stanford University
Daniel Rhodes: Columbia University
Archana Raja: Lawrence Berkeley National Laboratory
James C. Hone: Columbia University
Tony F. Heinz: Stanford University
Stéphane Kéna-Cohen: École Polytechnique de Montréal
Thomas Pohl: Aarhus University
Vinod M. Menon: City College of New York

Nature Communications, 2021, vol. 12, issue 1, 1-7

Abstract: Abstract 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 ∼ $${g}_{{pol}-{pol}}^{2s} \sim 46.4\pm 13.9\,\mu {eV}\mu {m}^{2}$$ g p o l − p o l 2 s ~ 46.4 ± 13.9 μ e V μ m 2 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.

Date: 2021
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DOI: 10.1038/s41467-021-22537-x

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