Strong Coupling of Multimolecular Species to Soft Microcavities.

Can we couple multiple molecular species to soft cavities? The answer to this question has relevance in designing open cavities for polaritonic chemistry applications. Because of the differences in adhesiveness, it is difficult to couple multiple molecular species to open cavities in a controlled and precise manner. In this Letter, we discuss the procedure to coat multiple dyes, TDBC and S2275, onto a dielectric microsphere using a layer-by-layer deposition technique so as to facilitate the multimolecule coupling. We observed the formation of a middle polariton branch due to the intermolecular mixing facilitated by the whispering gallery modes. The coupling strength, 2g, of the TDBC molecules was found to be 98 meV, while that of the S2275 molecules was 78 meV. The coupling strength was found to be greater than the cavity line width and the molecular absorption line width, showing that the system is in the strong coupling regime.