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The condensation of half-light half-matter exciton polaritons insemiconductor optical cavities is a striking example of macroscopic quantumcoherence in a solid state platform. Quantum coherence is possible only whenthere are strong interactions between the exciton polaritons provided by theirexcitonic constituents. Rydberg excitons with high principle value exhibitstrong dipole-dipole interactions in cold atoms. However, polaritons with theexcitonic constituent that is an excited state, namely Rydberg excitonpolaritons (REPs), have not yet been experimentally observed. Here, for thefirst time, we observe the formation of REPs in a single crystal CsPbBr3perovskite cavity without any external fields. These polaritons exhibit strongnonlinear behavior that leads to a coherent polariton condensate with aprominent blue shift. Furthermore, the REPs in CsPbBr3 are highly anisotropicand have a large extinction ratio, arising from the perovskite's orthorhombiccrystal structure. Our observation not only sheds light on the importance ofmany-body physics in coherent polariton systems involving higher-order excitedstates, but also paves the way for exploring these coherent interactions forsolid state quantum optical information processing.

Observation of Rydberg exciton polaritons and their condensate in a perovskite cavity