Ultrafast polariton dynamics in strongly coupled zinc porphyrin microcavities at room temperature

Abstract

Time and angle-resolved measurements reveal ultrafast dynamics of excitations in organic microcavities leading to dramatic modulation of probe transmission $(\ensuremath{\sim}30%)$. We find that the induced changes have both fast and long-lived components. Fast response times are defined by vibronic relaxation and intersystem crossing $({S}_{1}\ensuremath{\rightarrow}{T}_{1})$, whereas long-lived changes are attributed to a build up of carriers in the nonradiative triplet state whose lifetime is longer than the repetition rate of the laser pulses, resulting thus in incomplete recovery of the ground state. Blueshifts of the lower polariton branch in the presence of the pump pulse indicate the presence of nonlinear interactions in the sample. However, there is no evidence yet for the pair-type scattering processes in porphyrin microcavities.