Hidden nonlinear optical susceptibilities in linear polaritonic spectra

• URL: http://arxiv.org/abs/2411.09039v2
• Date: Sat, 16 Nov 2024 08:30:07 GMT
• Title: Hidden nonlinear optical susceptibilities in linear polaritonic spectra
• Authors: Arghadip Koner, Joel Yuen-Zhou,
• Abstract summary: Linear spectra of molecular polaritons formed by $N$ molecules coupled to a microcavity photon mode are usually well described by classical linear optics. We derive a general expression for the polaritonic linear spectra that reveal previously overlooked finite-size quantum corrections due to vacuum-mediated molecular Raman processes.
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• Abstract: Linear spectra of molecular polaritons formed by $N$ molecules coupled to a microcavity photon mode are usually well described by classical linear optics, raising the question of where the expected nonlinear effects in these strongly coupled systems are. In this work, we derive a general expression for the polaritonic linear spectra that reveal previously overlooked finite-size quantum corrections due to vacuum-mediated molecular Raman processes. Using a $1/N$ expansion, we demonstrate that these nonlinearities are suppressed in typical low-Q cavities due to an emergent timescale separation in polariton dynamics yet manifest in high-Q single-mode cavities where the photon loss is comparable to the single-molecule light-matter coupling strength.

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