Chemical reactions in imperfect cavities: enhancement, suppression, and resonance

TL;DR

This paper investigates how imperfect optical cavities influence chemical reaction rates, revealing that cavity effects depend on friction regimes and spectral broadening, with potential for rate enhancement or suppression.

Contribution

It introduces a model for reaction rates in imperfect cavities using non-Markovian dynamics, highlighting the impact of spectral broadening on resonance and reaction control.

Findings

Cavities can enhance reaction rates in low-friction regimes.

High friction cavities tend to suppress reactions.

Spectral broadening causes blue shifts and sharper resonances.

Abstract

The use of optical cavities to control chemical reactions has been of great interest recently, following demonstrations of enhancement, suppression, and negligible effects on chemical reaction rates depending on the specific reaction and cavity frequency. In this work, we study the reaction rate inside imperfect cavities, where we introduce a broadening parameter in the spectral density to mimic Fabry-P\'erot cavities. We investigate cavity modifications to reaction rates using non-Markovian Langevin dynamics with frictional and random forces to account for the presence of imperfect optical cavities. We demonstrate that in the regime of weak solvent and cavity friction, the cavity can enhance chemical reaction rates. On the other hand, in the high friction regime, cavities can suppress chemical reactions. Furthermore, we find that the broadening of the cavity spectral density gives rise to blue shifts of the resonance conditions and, surprisingly, increases the sharpness of the resonance effect.