Reproducibility of cavity-enhanced chemical reaction rates in the vibrational strong coupling regime

Mario V. Imperatore, John B. Asbury, Noel C. Giebink

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60 Scopus citations

Abstract

One of the most exciting and debated aspects of polariton chemistry is the possibility that chemical reactions can be catalyzed by vibrational strong coupling (VSC) with confined optical modes in the absence of external illumination. Here, we report an attempt to reproduce the enhanced rate of cyanate ion hydrolysis reported by Hiura et al. [chemRxiv:7234721 (2019)] when the collective OH stretching vibrations of water (which is both the solvent and a reactant) are strongly coupled to a Fabry-Pérot cavity mode. Using a piezo-tunable microcavity, we reproduce the reported vacuum Rabi splitting but fail to observe any change in the reaction rate as the cavity thickness is tuned in and out of the strong coupling regime during a given experiment. These findings suggest that there are subtleties involved in successfully realizing VSC-catalyzed reaction kinetics and therefore motivate a broader effort within the community to validate the claims of polariton chemistry in the dark.

Original languageEnglish (US)
Article number191103
JournalJournal of Chemical Physics
Volume154
Issue number19
DOIs
StatePublished - May 21 2021

All Science Journal Classification (ASJC) codes

  • General Physics and Astronomy
  • Physical and Theoretical Chemistry

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