The current theoretical understanding of collective vibrational strong coupling (VSC) relies mostly on simplified models and usually fails to explain experimental findings such as VSC catalysis. In order to bridge the gap between theory and experiments, we have developed a cavity molecular dynamics (CavMD) scheme to classically propagate the coupled photon-nuclear dynamics for a large number of realistic molecules forming VSC in Fabry-Perot microcavities. Currently, this approach can capture asymmetric Rabi splitting, polariton relaxation to vibrational dark modes, and polariton-enhanced multiphoton nonlinear absorption. We will also discuss how to understand chemical catalysis under collective VSC from this CavMD perspective.

Numerical insights of collective vibrational strong coupling via cavity molecular dynamics simulations

ACS Spring Meeting 2021

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