Hybridization of multiple vibrational modes via strong coupling using confined light fields (article)

This is the final version. Available on open access from Wiley via the DOI in this record.Data associated with this paper can be found at https://doi.org/10.24378/exe.1403Strong 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 we show 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. Our results lead us to 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.Engineering and Physical Sciences Research Council (EPSRC)European Research Counci