Multimode Vibrational Strong Coupling of Methyl Salicylate to a Fabry-Pérot Microcavity.

Abstract

The strong coupling of an IR-active molecular transition with an optical mode of the cavity results in vibrational polaritons, which opens a new way to control chemical reactivity via confined electromagnetic fields of the cavity. In this study, we design a voltage-tunable open microcavity and we show the formation of multiple vibrational polaritons in methyl salicylate. A Rabi splitting and polariton anticrossing behavior is observed when the cavity mode hybridizes with the C═O stretching vibration of methyl salicylate. Furthermore, the proposed theoretical model based on coupled harmonic oscillators reveals that the absorption of uncoupled molecules must also be considered to model the experimental spectra properly and that simultaneous coupling of multiple molecular vibrations to the same cavity mode has a significant influence on the transmission spectral profile.