Скачать или смотреть Vibration-Cavity Coupling: Modulation of coupling strength and ground state reaction rates

Coupling between vacuum optical fields and materials excitations has provided a new means for altering fundamental optical, electrical, and chemical properties. Our efforts have aimed at developing an understanding of basic behaviors that can then be extended to predictive and practical use. We have examined vibrational strong coupling , , and the roles of molecular system properties (absorption, concentration, spatial distribution ). In this talk, we will focus on non-linear transient response probed in the ultrafast regime, real-time modulation of couple strength via electrochemical switching, and cavity-modified chemical reactivity.
Specifically, we find excited-state spectra that reveal coherences between populations of both cavity polaritons and so-called dark states and explore cavity-modified saturable absorption and polariton kinetics. Our work has also extended to two electrochemical redox systems. We monitored the benzoquinone / dihydroquinone redox couple and achieved complete modulation of the Rabi splitting as well as the methylene blue / leucomethylene blue redox dye system, which exhibits strong exciton-cavity couplinng in the visible regime. Lastly, we monitor transmission spectra of the Fabry-Pérot microcavity filled with species that participate in a simple addition reaction. Both reactants and products have strong molecular vibrations that couple to the optical cavity modes, resulting in quantifiable vacuum Rabi splittings. We examine the reaction rates in and out of the cavity to expose the influence of vibrational strong coupling on reaction kinetics. Our results will extend the potential of cavity-modified material properties, which will have important implications for ultrafast optical devices and chemical synthesis and catalysis.

This talk was given by Dr. Blake Simpkins from US Naval Research Laboratory on Nov/18/2020.