Remote control of chemistry in optical cavities

TL;DR

This paper proposes a theoretical method to remotely control chemical reactions in optical cavities by using strong light-matter coupling, enabling ultrafast and tunable reaction yield manipulation without direct contact.

Contribution

It introduces a novel polaritonic device design that allows remote photochemical control through cavity-mediated delocalization, expanding possibilities for non-invasive reaction regulation.

Findings

Remote catalyst excitation can significantly increase reaction efficiency.

Strong cavity-molecule coupling enables control over spatially separated reactants.

The approach is generalizable to various photochemical reactions.

Abstract

Manipulation of chemical reactivity often involves changing reagents or environmental conditions. Alternatively, strong coupling between light and matter offers a way to tunably hybridize their physicochemical properties and thereby change reaction dynamics without synthetic modifications to the starting material. Here, we theoretically design a polaritonic (hybrid photonic-molecular) device that supports ultrafast tuning of reaction yields even when the catalyst and its reactant are spatially separated across several optical wavelengths. We demonstrate how photoexcitation of a `remote catalyst' in an optical microcavity can control photochemistry of a reactant in another microcavity. Harnessing delocalization across the spatially separated compounds that arises from strong cavity-molecule coupling, this intriguing phenomenon is shown for the infrared-induced \textit{cis} $\rightarrow$ \textit{trans} conformational isomerization of nitrous acid (HONO). Indeed, increasing the excited-state population of the remote catalyst can enhance the isomerization efficiency by an order of magnitude. The theoretical proposal reported herein is generalizable to other reactions and thus introduces a versatile tool to control photochemistry.