Related papers: Vibropolaritonic Reaction Rates in the Collective Strong Coupling Regime: Pollak-Grabert-H\"anggi Theory

Vibropolaritonic Reaction Rates in the Collective Strong Coupling Regime: Pollak-Grabert-H\"anggi Theory

URL: http://arxiv.org/abs/2211.05820v2
Date: Mon, 9 Jan 2023 19:54:01 GMT
Title: Vibropolaritonic Reaction Rates in the Collective Strong Coupling Regime: Pollak-Grabert-H\"anggi Theory
Authors: Matthew Du, Yong Rui Poh, Joel Yuen-Zhou
Abstract summary: We show that the Pollak-Grabert-H"anggi (PGH) theory fails to capture the ensemble effects present in experiments. We show how this model succumbs to the polariton "large $N$ problem", that is, the situation whereby the single reacting molecule feels only a tiny $1/N$ part of the collective light-matter interaction intensity.
Score: 0.0
License: http://creativecommons.org/licenses/by/4.0/
Abstract: Following experimental evidence that vibrational polaritons, formed from collective vibrational strong coupling (VSC) in optical microcavities, can modify ground-state reaction rates, a spate of theoretical explanations relying on cavity-induced frictions has been proposed through the Pollak-Grabert-H\"anggi (PGH) theory, which goes beyond transition state theory (TST). However, by considering only a single reacting molecule coupled to light, these works do not capture the ensemble effects present in experiments. Moreover, the relevant light-matter coupling should have been $\sqrt{N}$ times smaller than those used by preceding works, where $N\approx10^{6}-10^{12}$ is the ensemble size. In this work, we explain why this distinction is significant and can nullify effects from these cavity-induced frictions. By analytically extending the cavity PGH model to realistic values of $N$, we show how this model succumbs to the polariton "large $N$ problem", that is, the situation whereby the single reacting molecule feels only a tiny $1/N$ part of the collective light-matter interaction intensity, where $N$ is large.

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