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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 (WSe 2 ) 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.
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Detection of photon statistics and multimode field correlations by Raman processes
Glauber’s g(2)-function provides a common measure of quantum field statistics through two-photon coincidence counting in Hanbury Brown–Twiss measurements. Here, we propose to use nonlinear optical signals as a tool for the characterization of quantum light. In particular, we show that Raman measurements provide an alternative direct probe for a different component of the four-point correlation function underlying the g(2)-function. We illustrate this capacity for a specific quantum state obtained from a frequency conversion process. Our work points out how the analysis of controlled optical nonlinear processes can provide an alternative window toward the analysis of quantum light sources.
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- Award ID(s):
- 1953045
- PAR ID:
- 10593584
- Publisher / Repository:
- American Institute of Physics
- Date Published:
- Journal Name:
- The Journal of Chemical Physics
- Volume:
- 154
- Issue:
- 10
- ISSN:
- 0021-9606
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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