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Strong exciton-polariton correlations shape the many-body polariton dynamics in two-dimensional metal halide semiconductor microcavities: Competitive pathways for polariton condensation

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arXiv:2404.14744v1 Announce Type: cross
Abstract: Polariton condensation relies on the massive occupation of the lowest-energy polariton state beyond a required critical density. The mechanisms driving both the occupation and depopulation of the lowest-energy polariton state all rely on multi-particle scattering, and its dynamics determine the extent to which condensates can form spontaneously. To pinpoint many-body processes hindering polariton condensation in two-dimensional metal-halide semiconductors, we examine the exciton-polariton dynamics in a Fabry-P\'erot microcavity over timescales involving the dynamics of multi-particle polariton ($\ll 1$\,ps) and exciton scattering processes ($\gg 1$\,ps). We find evidence of enhanced nonlinear exciton-exciton scattering in the microcavity compared to that in the semiconductor, and that the exciton reservoir mediates polariton scattering. We posit that the complex scattering landscape between the exciton reservoir and polaritons limits the formation of polariton condensates in two-dimensional metal-halide semiconductors, and we discuss the generality of our conclusions for materials systems in which the lattice mediates strong multi-particle correlations.

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