Theory for Nonlinear Spectroscopy of Vibrational Polaritons*

Vibrational polaritons are hybrid excitations of optical resonators and molecules which offer new ways to control chemical processes in the electronic ground-state by introducing long-range coherence into molecular vibrational excited-states. In this talk, I will provide an overview of a recently-developed theory of pump-probe spectroscopy of vibrational polaritons based on the quantum Langevin equations. I will give emphasis to aspects of the polariton nonlinear optical response which are unique to the vibrational case, and show how information gathered from nonlinear optical measurements provides guidance for the manipulation of chemical reactivity in optical cavities.