Hybridization of Multiple Vibrational Modes via Strong Coupling Using Confined Light Fields

Abstract Strong coupling of molecules placed in an optical microcavity may lead to the formation of hybrid states called polaritons, states that inherit characteristics of both the optical cavity modes and the molecular resonance. This is possible for both excitonic and vibrational molecular resonances. Previous work has shown that strong coupling may be used to hybridize two different excitonic resonances; this can be achieved when more than one molecular species is included in the cavity. Here it is shown that under suitable conditions three different molecular vibrational resonances of the same molecular unit may also be coupled together, the resulting polariton having characteristics of all three vibrational resonances. These results suggest that strong coupling might be used to manipulate vibrational resonances in a richer and subtler way than previously considered, opening a path to greater control of molecular systems and molecular processes via vibrational strong coupling.