In this talk, we report ultrafast spectroscopic investigation on coherent light-matter interactions of molecular vibrational polaritons. By employing two-dimensional infrared spectroscopy, unexpected dark modes excitations have been observed and a clear picture of how polariton sates interact with dark modes when the system is in equilibrium can be drawn. The early-time nonlinear responses due to polariton coherences can be disentangled and its nonlinearity can by controlled by manipulating the macroscopic parameters, such as the cavity longitudinal length or molecular concentration. We also apply the designed microcavity to modify the energetic properties of molecular vibrational modes. Our spectroscopic study shows that by sharing the same cavity mode, three polaritonic states can be formed out of two originally uncoupled molecular modes. A new energy transfer pathway is observed via the polariton states. This novel application further proves the potential of molecular vibrational polaritons in quantum gate operations, designing optical switches, mid-IR sensing and new reaction mechanism.

Ultrafast IR spectroscopic investigation on molecular vibrational polaritons

2019 Fall National Meeting

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