4.8 Article

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

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NATURE COMMUNICATIONS
卷 12, 期 1, 页码 -

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NATURE RESEARCH
DOI: 10.1038/s41467-021-22537-x

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资金

  1. National Science Foundation through the MRSEC program [DMR-2011738]
  2. ARO MURI program [W911NF-17-1-0312]
  3. MRSEC program [DMR-2011738]
  4. National Science Foundation [DMR-1708457]
  5. Gordon and Betty Moore Foundation's EPiQS Initiative [GBMF9462]
  6. Alexander von Humboldt Foundation
  7. Laboratory Directed Research and Development Program of Lawrence Berkeley National Laboratory under U.S. Department of Energy [DE-AC02-05CH11231]
  8. NSERC Discovery Grant Program
  9. Canada Research Chairs
  10. Carlsberg Foundation through the Semper Ardens Research Project
  11. DFG [SPP1929]
  12. European Commission [800942]
  13. Danish National Research Foundation through the Center of Excellence CCQ [DNRF156]

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Exciton-polaritons formed using excited excitonic states in materials like monolayer tungsten diselenide exhibit enhanced nonlinear responses, showing potential for strong exciton-polariton interactions in solid-state quantum photonic technologies.
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 similar to g(pol-pol)(2s) similar to 46.4 +/- 13.9 mu eV mu m(2) which is similar to 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.

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