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

• Published in: The Journal of chemical physics Vol. 154; no. 19; p. 191103
• Main Authors: Imperatore, Mario V., Asbury, John B., Giebink, Noel C.
• Format: Journal Article
• Language: English
• Published: Melville American Institute of Physics 21.05.2021
• Subjects: Chemical reactions; Coupling; Cyanates; Fabry-Perot interferometers; Physics; Polaritons; Reaction kinetics; Reproducibility
• ISSN: 0021-9606; 1089-7690
• DOI: 10.1063/5.0046307

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.