Resonance between the excitation frequency of an ensemble of molecules and the electromagnetic mode of a microcavity produces a hybrid light-matter system. In this regime, the molecule and cavity can no longer be treated as separate subsystems but as a hybrid polaritonic system, which has a number of interesting photochemical properties and applications. In this work, we modify the time-dependent spin-orbit configuration interaction (TDSOCI) method to include the resonant effects of a microcavity. The TDSOCI method is an ab initio quantum dynamical method that explicitly includes spin-orbit coupling in the electron dynamics. The Tavis-Cummings model is implemented to include the effects of a microcavity within the TDSOCI framework. This method is used to study the dipole-switching dynamics, spin flipping, and polaritonic state transitions in small polar molecules arising from the inclusion of both a microcavity and spin-orbit coupling.

Time-dependent spin-orbit configuration interaction theory for strong light-molecule coupling

ACS Spring 2022

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