Controlling and utilizing vibration-cavity polaritons (Conference Presentation)

Abstract

Molecular vibrations can couple to optical cavities to create new hybrid states called polaritons. The magnitude of this coupling, measured as the vacuum Rabi splitting (Ω), correlates with modified materials processes such as photon emission, molecular energy transfer, and chemical reaction rates. In this talk, I will first discuss active control of cavity coupling strength. We demonstrate active tuning of excitonic strong coupling in a system where organic dyes strongly couple to propagating surface plasmon polaritons (SPPs) and modulation of vibrational strong coupling in a Fabry-Perot cavity coupled to an organic charge shuttling molecule. Next, I will discuss results indicating modified chemical reaction rates for an alcoholysis addition reaction forming urethane monomers. Cavity tuning was used to selectively couple to reactant, solvent, and product vibrational modes resulting in a chemical response that is cavity tuning dependent. Lastly, and in light of the search for an understanding of the mechanisms leading to modified chemical and physical properties, I will present a theoretical description of the density of polariton states relative to molecular dark states. This work will also discuss the differences between polariton states generated in microcavities, slabs, and in the bulk.