Hidden nonlinear optical susceptibilities in linear polaritonic spectra

Fuente: arXiv
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Autores principales: Koner, Arghadip, Yuen-Zhou, Joel
Formato: Preprint
Publicado: 2024
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author Koner, Arghadip
Yuen-Zhou, Joel
author_facet Koner, Arghadip
Yuen-Zhou, Joel
contents 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.
format Preprint
id arxiv_https___arxiv_org_abs_2411_09039
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Hidden nonlinear optical susceptibilities in linear polaritonic spectra
Koner, Arghadip
Yuen-Zhou, Joel
Quantum Physics
Other Condensed Matter
Chemical Physics
Optics
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.
title Hidden nonlinear optical susceptibilities in linear polaritonic spectra
topic Quantum Physics
Other Condensed Matter
Chemical Physics
Optics
url https://arxiv.org/abs/2411.09039