Vibrational-polaritons are the hybrid excitations which arise when dipole-active molecular vibrations interact strongly with infrared optical cavities. These emergent states offer new ways to control chemical processes by introducing long-range coherence into molecular vibrations and by altering their relaxation dynamics. For instance, under strong coupling, molecular anharmonicities are converted into many-body polariton-polariton and polariton-dark state interactions. In this talk, I will discuss a recently-developed theory of pump-probe spectroscopy of vibrational polaritons based on the quantum Langevin equations. I will emphasize the main effects of electrical and mechanical anharmonicity on vibrational-polariton pump-probe spectra, and illustrate the theory by comparing its predictions to recently obtained experimental data.

Theory of pump-probe spectroscopy for vibrational-polaritons

256th National Meeting (2018)

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