Recent studies have demonstrated coherent coupling between the vibrational modes of polymers, liquids, and solvated compounds and a Fabry-Perot optical cavity mode. This coupling creates vibration-cavity polariton modes whose energy tunes with the cavity length and incidence angle. We use pump-probe infrared spectroscopy to make the first measurements of the dynamics of vibration-cavity polaritons.  At very early times, we observe quantum beating between the two polariton states. After this quantum beating, we directly observe excited-state absorption from both polariton modes and uncoupled reservoir modes. The polariton mode relaxes ten times more quickly than the uncoupled vibrational mode and the polariton lifetime depends on the angle of incidence of the infrared pulses. We show that coupling to an optical cavity gives a means of control of the frequency and lifetime of vibration-cavity polaritons and could have important implications for future experiments that extend this control to chemical reactivity.

Vibrational energy relaxation of vibration-cavity polariton modes

252nd National Meeting (2016)

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