Polariton-induced Purcell effects via a reduced semiclassical electrodynamics approach

The Journal of Chemical Physics, Год журнала: 2025, Номер 162(12)

Опубликована: Март 24, 2025

Recent experiments have demonstrated that polariton formation provides a novel strategy for modifying local molecular processes when large ensemble of molecules is confined within an optical cavity. Herein, numerical based on coupled Maxwell–Schrödinger equations examined simulating in realistic cavity structure under collective strong coupling. In this approach, only few molecules, referred to as quantum impurities, are treated mechanically, while the remaining macroscopic layer and modeled using dielectric functions. When single electronic two-level system embedded Lorentz medium two-dimensional Bragg resonator, our simulations reveal polariton-induced Purcell effect: radiative decay rate impurity significantly enhanced by frequency matches frequency, can sometimes be greatly suppressed near resonance with bulk forming addition, approach demonstrates absorption light exhibits Rabi-splitting-dependent suppression due inclusion structure. Our also identify fundamental limitation approach—an inaccurate description dephasing rates into dark modes. This arises because dark-mode degrees freedom not explicitly included most simple As effect alters differently from weak coupling, may facilitate understanding origin polariton-modified photochemistry

Язык: Английский

Simulations of photoinduced processes with the exact factorization: State of the art and perspectives

Physical Chemistry Chemical Physics, Год журнала: 2024, Номер 26(42), С. 26693 - 26718

Опубликована: Янв. 1, 2024

This perspective offers an overview of the applications exact factorization electron-nuclear wavefunction in simulations ultrafast processes molecules with main focus on photochemistry.

Язык: Английский