Tuning the Coherent Propagation of Organic Exciton‐Polaritons through the Cavity Q‐factor

Transport of excitons in organic materials can be enhanced through polariton formation when the interaction strength between these excitons and the confined light modes of an optical resonator exceeds their decay rates. While the polariton lifetime is determined by the Q(uality)‐factor of the optical resonator, the polariton group velocity is not. Instead, the latter is solely determined by the polariton dispersion. Yet, experiments suggest that the Q‐factor also controls the polariton propagation velocity. To understand this observation, the authors perform molecular dynamics simulations of Rhodamine chromophores strongly coupled to Fabry–Pérot cavities with various Q‐factors. The results suggest that propagation in the aforementioned experiments is initially dominated by ballistic motion of upper polariton states at their group velocities, which leads to a rapid expansion of the wavepacket. Cavity decay in combination with non‐adiabatic population transfer into dark states, rapidly depletes these bright states, causing the wavepacket to contract. However, because population transfer is reversible, propagation continues, but as a diffusion process, at lower velocity. By controlling the lifetime of bright states, the Q‐factor determines the duration of the ballistic phase and the diffusion coefficient in the diffusive regime. Thus, polariton propagation in organic microcavities can be effectively tuned through the Q‐factor.