Resolving exciton and polariton multi-particle correlations in an optical microcavity in the strong coupling regime

Abstract

Multi-particle correlations of exciton-polaritons and reservoir-excitons in the strong light-matter coupling regime dictate the quantum dynamics of optical microcavities. In this letter, we examine the many-body exciton-polariton dynamics in a Fabry-Pérot microcavity of a two-dimensional metal-halide semiconductor over timescales involving polariton ($\ll 1$\,ps) and exciton ($\gg 1$\,ps) scattering. We find enhanced exciton nonlinear dynamics in the microcavity versus the bare semiconductor, concomitant with ultrafast polariton scattering dynamics. We measure, by means of coherent spectroscopy, the coupling between exciton-polaritons, bright excitons, and reservoir-excitons that highlight the complex scattering landscape that fundamentally drives polariton condensation.

Main manuscript plus supplementary material document. Accepted for publication in Physical Review B