Bose–Einstein condensation of exciton polariton in a perovskite cavity

The formation of half-light half-matter quasiparticle exciton polariton and its condensation in semiconductor optical cavities are striking phenomena for the macroscopic quantum coherence at elevated temperature. The matter constituent of exciton polariton dictates the interacting behaviors of these bosonic particles primarily via exciton-exciton interactions. However, these interactions are all limited to the ground state exciton, although they can be orders of magnitude stronger at Rydberg states with higher principal numbers. Here, for the first time, we observe the spontaneous formed Rydberg exciton polaritons (REPs) in a high quality Fabry-Perot cavity embedded with single crystal inorganic perovskite, CsPbBr₃. Such REPs exhibit strong nonlinear behavior, enabling an anomalous dynamic process that leads to a coherent polariton condensate with prominent blue shift. Furthermore, we discover the first anisotropic REP with large extinction ratio over 50, arising from the perovskite’s asymmetric orthorhombic crystal structure. Our observation not only sheds light on the importance of coherent many-body Rydberg interactions in polariton systems, but also paves the way for exploring these coherent interactions for solid state quantum optical information processing.