Reproducibility of cavity-enhanced chemical reaction rates in the vibrational strong coupling regime
TLDR
In this paper, a piezo-tunable microcavity was used to reproduce the reported vacuum Rabi splitting but failed 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.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-Perot 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.read more
Citations
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Chemistry under Vibrational Strong Coupling.
TL;DR: Vibrational strong coupling (VSC) as discussed by the authors is a new tool to control chemical reactivity, and it also gives insight into which vibrations are involved in a reaction in a chemical reaction.
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Molecular Polaritonics: Chemical Dynamics Under Strong Light–Matter Coupling
TL;DR: In this article , the authors review the present status of strong light-matter coupling and present applications to energy conversion processes, and present technical issues in the construction of theoretical approaches are briefly described in Section 5.
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Mode-Specific Chemistry through Vibrational Strong Coupling (or A Wish Come True)
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Vibration-Cavity Polariton Chemistry and Dynamics.
TL;DR: In this article , the ability of vibration-cavity polaritons to modify chemical and physical processes including chemical reactivity, as well as steady-state and transient spectroscopy was discussed.
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A Roadmap Toward the Theory of Vibrational Polariton Chemistry
Derek S. Wang,Susanne Yelin +1 more
TL;DR: The field of vibrational polariton chemistry was firmly established in 2016 when a chemical reaction rate at room temperature was modified within a resonantly tuned infrared cavity without externally driving the system.
References
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Journal ArticleDOI
Hybrid Light-Matter States in a Molecular and Material Science Perspective.
TL;DR: It is shown that light-matter hybridization is quite easy to achieve: all that is needed is to place molecules or a material in a resonant optical cavity under the right conditions and to use it as a tool in (bio)molecular science and spectroscopy.
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Modifying chemical landscapes by coupling to vacuum fields.
TL;DR: It is demonstrated here that one can indeed influence a chemical reaction by strongly coupling the energy landscape governing the reaction pathway to vacuum fields.
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Ultrastrong coupling between light and matter
TL;DR: A review of ultrastrong coupling between light and matter can be found in this paper, where the authors discuss entangled ground states with virtual excitations, new avenues for nonlinear optics, and connections to several important physical models.
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Tilting a ground-state reactivity landscape by vibrational strong coupling
Anoop Thomas,Lucas Lethuillier-Karl,Kalaivanan Nagarajan,Robrecht M. A. Vergauwe,Jino George,Thibault Chervy,Atef Shalabney,Eloïse Devaux,Cyriaque Genet,Joseph Moran,Thomas W. Ebbesen +10 more
TL;DR: The reactivity of a compound bearing two possible silyl bond cleavage sites is studied as a function of VSC of three distinct vibrational modes in the dark, showing that VSC can indeed tilt the reactivity landscape to favor one product over the other.
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Cavity-Controlled Chemistry in Molecular Ensembles
Felipe Herrera,Frank C. Spano +1 more
TL;DR: It is shown that strong resonant coupling of a cavity field with an electronic transition can effectively decouple collective electronic and nuclear degrees of freedom in a disordered molecular ensemble, even for molecules with high-frequency quantum vibrational modes having strong electron-vibration interactions.