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Reproducibility of Effects of Vibrational Strong Coupling on Chemical Reaction Rates

Abstract

The ability to conduct new chemical reactions, or to control known reactions in new ways, is a key area of academic and societal interest. In recent years, developments in the field of photonics have revealed phenomena that occur when molecules strongly interact with light. One area of interest is in vibrational strong coupling, which occurs when molecular bond vibrations strongly interact with electromagnetic fields in the mid-infrared regime. In a fascinating series of experiments, reactions were performed under vibrational strong coupling and observed to be dramatically modified. Given the impact that these findings imply, independent verification and a thorough understanding of the underlying mechanisms is critical. One such reaction, where the ester para-nitrophenyl acetate is hydrolyzed by tetrabutylammonium fluoride in ethyl acetate, reportedly accelerated by an order of magnitude. An attempt to reproduce these findings with the goal of further investigating the mechanism of reaction modification is presented. While experimental procedures and conditions were performed closely to those of the original work, no reaction modification was observed. Furthermore, no significant change in reaction rate with detuning was found. An analysis of the reaction system was performed using Jaynes-Cummings coupled oscillator and transfer matrix method models to confirm vibrational strong coupling and investigate the lack of observed reaction modification. The potential of vibrational strong coupling as new tool for reaction control is tantalizing and may usher in a new era of chemical synthesis, however a robust understanding of the underlying mechanisms involved are crucial to its realization.

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