Strong coupling-induced frequency shifts of highly detuned photonic modes in multimode cavities

Abstract

Strong coupling between light and molecules is a fascinating topic exploring the implications of the hybridization of photonic and molecular states. For example, many recent experiments have explored the possibility that strong coupling of photonic and vibrational modes might modify chemical reaction rates. In these experiments, reactants are introduced into a planar cavity, and the vibrational mode of a chemical bond strongly couples to one of the many photonic modes supported by the cavity. Some experiments quantify reaction rates by tracking the spectral shift of higher-order cavity modes that are highly detuned from the vibrational mode of the reactant. Here, we show that the spectral position of these cavity modes, even though they are highly detuned, can still be influenced by strong coupling. We highlight the need to consider this strong coupling-induced frequency shift of cavity modes if one is to avoid underestimating cavity-induced reaction rate changes. We anticipate that our work will assist in the re-analysis of several high-profile results and has implications for the design of future strong coupling experiments.