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Quantum Chemistry

Hidden nonlinear optical susceptibilities in linear polaritonic spectra

arXiv
Authors: Arghadip Koner, Joel Yuen-Zhou

Year

2024

Paper ID

36793

Status

Preprint

Abstract Read

~2 min

Abstract Words

106

Citations

N/A

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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  • 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...

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References & Citation Signals

[1] DOI https://doi.org/arXiv:2411.09039 [2] arXiv https://arxiv.org/abs/2411.09039 [3] Publisher https://arxiv.org/abs/2411.09039

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