Nonequilibrium polariton dynamics in organic microcavities

Microcavities containing a J-aggregate forming organic dye were prepared in the strong-coupling regime. Changing the position of the neat organic films within the microcavity allows a tuning of the giant Rabi splitting observed. We set the Rabi splitting to 25 meV and study the thermal activation of the higher-energy polariton emission under excitation off resonance. This is found to exhibit an Arrhenius activation with an energy corresponding to the polariton branch splitting. A constant offset to the upper polariton is observed at low temperature. Microsecond gated spectroscopy reveals that thermalization of the system occurs on the time scale of milliseconds, which contrasts with the polariton lifetime in the range of picoseconds. Bulk sample heating cannot fully account for the slow polariton thermalization observed in steady-state experiments, suggesting that long-lived macroscopic polariton coherence influences the polariton relaxation.