Whispering gallery modes in a microwire are characterized by a nearly equidistant energy spectrum. In the strong exciton-photon coupling regime, this system represents a bosonic cascade: a ladder of discrete energy levels that sustains stimulated transitions between neighboring steps. Here, by using a femtosecond angle-resolved spectroscopic imaging technique, the ultrafast dynamics of polaritons in a bosonic cascade based on a one-dimensional ZnO whispering gallery microcavity are explicitly visualized. Clear ladder-form build-up processes from higher to lower energy branches of the polariton condensates are observed, which are well reproduced by modeling using rate equations. Remarkably, a pronounced superbunching feature, which could serve as solid evidence for bosonic cascades, is demonstrated by the measured second-order time correlation factor. In addition, the nonlinear polariton parametric scattering dynamics on a time scale of hundreds of femtoseconds are revealed. Our understandings pave the way toward ultrafast coherent control of polaritons at room temperature.
Keywords: angle-resolved photoluminescence spectroscopy; bosonic cascade; exciton polariton; second-order time correlation factor; ultrafast dynamics.