Steering Non-Equilibrium Molecular Dynamics in Optical Cavities

TL;DR

This paper presents a theoretical model for controlling chemical bond stability in molecules by manipulating vibrational strong coupling within optical cavities, revealing new pathways for chemical reactivity control.

Contribution

It introduces a novel theoretical framework to analyze non-equilibrium molecular dynamics in optical cavities with auxiliary ensembles, highlighting control over thermalization rates.

Findings

Coupling with cavity mode introduces colored noise and negative feedback.

Control over thermalization rates of reactive molecules.

Potential to steer chemical bond stability under vibrational strong coupling.

Abstract

Optical resonators have shown outstanding abilities to tailor chemical landscapes through enhanced light-matter interaction between confined optical modes and molecule vibrations. We propose a theoretical model to study cooperative vibrational strong coupling in an open quantum system. The non-equilibrium stochastic molecular dynamics in an optical cavity with an auxiliary ensemble is investigated. It shows that coupling with a cavity mode introduces an additional colored noise and a negative feedback, both of which enable control over thermalization rates (i.e. the lifetime of excitation) of reactive molecules. Our work offers a pathway to steer stability of chemical bonds for chemical reactivity under cooperative vibrational strong coupling.