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Chemical Reactions in Imperfect Cavities: Enhancement, Suppression, and Resonance

John P. Philbin, Yu Wang, Prineha Narang, Wenjie Dou

2022The Journal of Physical Chemistry C31 citationsDOI

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–Pérot 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.

Topics & Concepts

Chemical reactionResonance (particle physics)Reaction rateBelousov–Zhabotinsky reactionWork (physics)Chemical physicsImperfectMaterials scienceChemical speciesChemistryMolecular physicsPhysicsAtomic physicsThermodynamicsPhysical chemistryOrganic chemistryCatalysisPhilosophyLinguisticsBiochemistryStrong Light-Matter InteractionsQuantum Information and CryptographyMechanical and Optical Resonators
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