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Title: Remote Control of Chemistry in Optical Cavities

Abstract

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.

Authors:
 [1];  [1];  [1]
  1. Univ. of California, San Diego, CA (United States). Dept. of Chemistry and Biochemistry
Publication Date:
Research Org.:
Univ. of California, San Diego, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1504576
Alternate Identifier(s):
OSTI ID: 1547618
Grant/Contract Number:  
SC0019188
Resource Type:
Accepted Manuscript
Journal Name:
Chem
Additional Journal Information:
Journal Name: Chem; Journal ID: ISSN 2451-9294
Publisher:
Cell Press, Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; polariton; remote control; chemistry; cavities; quantum electrodynamics

Citation Formats

Du, Matthew, Ribeiro, Raphael F., and Yuen-Zhou, Joel. Remote Control of Chemistry in Optical Cavities. United States: N. p., 2019. Web. doi:10.1016/j.chempr.2019.02.009.
Du, Matthew, Ribeiro, Raphael F., & Yuen-Zhou, Joel. Remote Control of Chemistry in Optical Cavities. United States. doi:10.1016/j.chempr.2019.02.009.
Du, Matthew, Ribeiro, Raphael F., and Yuen-Zhou, Joel. Mon . "Remote Control of Chemistry in Optical Cavities". United States. doi:10.1016/j.chempr.2019.02.009. https://www.osti.gov/servlets/purl/1504576.
@article{osti_1504576,
title = {Remote Control of Chemistry in Optical Cavities},
author = {Du, Matthew and Ribeiro, Raphael F. and Yuen-Zhou, Joel},
abstractNote = {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.},
doi = {10.1016/j.chempr.2019.02.009},
journal = {Chem},
number = ,
volume = ,
place = {United States},
year = {2019},
month = {3}
}

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Works referencing / citing this record:

Cavity Catalysis by Cooperative Vibrational Strong Coupling of Reactant and Solvent Molecules
journal, July 2019

  • Lather, Jyoti; Bhatt, Pooja; Thomas, Anoop
  • Angewandte Chemie, Vol. 131, Issue 31
  • DOI: 10.1002/ange.201905407

Cavity Catalysis by Cooperative Vibrational Strong Coupling of Reactant and Solvent Molecules
journal, July 2019

  • Lather, Jyoti; Bhatt, Pooja; Thomas, Anoop
  • Angewandte Chemie International Edition, Vol. 58, Issue 31
  • DOI: 10.1002/anie.201905407