The formation of half-light half-matter quasiparticle exciton polariton and its condensation in semiconductor microcavities are striking phenomena for the macroscopically 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 are expected to be much 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. Such REPs exhibit strong nonlinear behavior and anisotropic, enabling an anomalous dynamic process that leads to a coherent polariton condensate with prominent blue shift. This discovery presents a unique platform to study quantum coherent many-body physics, and enables unprecedented manipulation of these Rydberg states by new means such as chemical composition engineering, structural phase control, and external gauge fields. The solid state REP and its condensates also hold great potential for important applications, such as sensing, communication, and quantum computing.
The second harmonic generation (SHG) produced from two-dimensional atomic crystals have been utilized recently in studying the grain boundaries and electronic structure of such ultra-thin materials. However, the SHG in many of these crystals, such as transition metal dichalcogenides (TMDCs), only occur in odd numbered layers with limited intensity due to their noncentrosymmetric nature. Here, we probe the SHG from the bulk noncentrosymmetric molybdenum disulfide (MoS2). Whereas the commonly studied 2H crystal phase’s anti-parallel nonlinear dipoles in adjacent layers give an oscillatory SH response, the parallel nonlinear dipoles of each atomic layer in the 3R phase constructively interfere to amplify the nonlinear light. Due to this interference, we observed the atomically phase-matched condition yielding a quadratic dependence between the intensity and layer number. Additionally, we probed the layer evolution of the A and B excitonic transitions in 3R-MoS2 using SHG spectroscopy and found distinct electronic structure differences arising from the crystal geometry. These findings demonstrate the dramatic effect of the symmetry and layer stacking of these atomic crystals.
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