Modeling Nonadiabatic Dynamics with Dissipation: Application to Cavity Polaritons

Nonadiabatic simulation methods are indispensable tools for investigating dynamical processes, including those involving polaritons formed through the hybridization of matter degrees of freedom and photons. Due to the finite lifetime of photons, polaritons intrinsically constitute an open quantum system. To properly account for dissipation, we combine the Schrödinger-Langevin equation with the split-operator Fourier transform and mixed quantum-classical simulation methods such as Ehrenfest dynamics and fewest-switches surface hopping to study nonadiabatic processes in open quantum systems. We test our method on the spontaneous emission of a two-level atom, the extended Tully-I (single avoided crossing) model with dissipation, and an isomerization model within a lossy cavity. The results obtained from these methods are consistent with each other and demonstrate that the dissipative nature of the polariton can alter the isomerization reaction. Our method provides a distinct approach to modeling nonadiabatic dynamics with dissipation and has the potential to be widely applied in related fields.