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Title: Remote Control of Chemistry in Optical Cavities

Journal Article · · Chem

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

Research Organization:
Univ. of California, San Diego, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
Grant/Contract Number:
SC0019188
OSTI ID:
1617959
Alternate ID(s):
OSTI ID: 1504576; OSTI ID: 1547618
Journal Information:
Chem, Journal Name: Chem Vol. 5 Journal Issue: 5; ISSN 2451-9294
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 54 works
Citation information provided by
Web of Science

Cited By (7)

Cavity Catalysis by Cooperative Vibrational Strong Coupling of Reactant and Solvent Molecules journal July 2019
Cavity Catalysis by Cooperative Vibrational Strong Coupling of Reactant and Solvent Molecules journal July 2019
Manipulating nonadiabatic conical intersection dynamics by optical cavities journal January 2020
Triplet harvesting in the polaritonic regime: A variational polaron approach journal August 2019
Multi-level quantum Rabi model for anharmonic vibrational polaritons journal October 2019
Ultrafast dynamics in the vicinity of quantum light-induced conical intersections journal September 2019
Ground state chemistry under vibrational strong coupling: dependence of thermodynamic parameters on the Rabi splitting energy journal February 2020