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

Observation of Rydberg exciton polaritons and their condensate in a perovskite cavity
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DOI:
10.1073/pnas.1909948116
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发表时间:
2019-10-08
影响因子:
11.1
通讯作者:
Zhang, Xiang
Zhang, Xiang
中科院分区:
综合性期刊1区
文献类型:
--
作者:
Bao, Wei;Liu, Xiaoze;Zhang, Xiang

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半导体光腔中半光半物质激子极化子的凝聚是固体平台中宏观量子相干的一个显著例子。只有当激子组分提供的激子极化子之间存在强相互作用时,量子相干才是可能的。冷原子中具有高主值的里德堡激子表现出很强的偶极-偶极相互作用。然而,激子组分为激发态的里德堡激子极化子(REP)尚未被实验观测到。在这里,我们观察了在没有任何外场的情况下,CsPbBr3单晶钙钛矿腔中REP的形成。这些极化子表现出强烈的非线性行为,导致了具有显著蓝移的相干极化子凝聚体。此外,CsPbBr3中的REP是高度各向异性的,具有很大的消光比,这是由于钙钛矿的正交晶体结构造成的。我们的观测不仅揭示了高阶激发态相干极化系统中多体物理的重要性,而且为探索固态量子光学信息处理中的相干相互作用铺平了道路。
The condensation of half-light half-matter exciton polaritons in semiconductor optical cavities is a striking example of macroscopic quantum coherence in a solid-state platform. Quantum coherence is possible only when there are strong interactions between the exciton polaritons provided by their excitonic constituents. Rydberg excitons with high principal value exhibit strong dipole-dipole interactions in cold atoms. However, polaritons with the excitonic constituent that is an excited state, namely Rydberg exciton polaritons (REPs), have not yet been experimentally observed. Here, we observe the formation of REPs in a single crystal CsPbBr3 perovskite cavity without any external fields. These polaritons exhibit strong nonlinear behavior that leads to a coherent polariton condensate with a prominent blue shift. Furthermore, the REPs in CsPbBr3 are highly anisotropic and have a large extinction ratio, arising from the perovskite's orthorhombic crystal structure. Our observation not only sheds light on the importance of many-body physics in coherent polariton systems involving higher-order excited states, but also paves the way for exploring these coherent interactions for solid-state quantum optical information processing.