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

Bao, Wei; Liu, Xiaoze; Xue, Fei; Zheng, Fan; Tao, Renjie; Wang, Siqi; Xia, Yang; Zhao, Mervin; Kim, Jeongmin; Yang, Sui; Li, Quanwei; Wang, Ying; Wang, Yuan; Wang, Lin-Wang; MacDonald, Allan H.; Zhang, Xiang

doi:10.1073/pnas.1909948116

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

Journal Article · 23 September 2019 · Proceedings of the National Academy of Sciences of the United States of America

DOI: https://doi.org/10.1073/pnas.1909948116 · OSTI ID:1565966

Bao, Wei ^[1]; Liu, Xiaoze ^[1]; Xue, Fei ^[2]; Zheng, Fan ^[3]; Tao, Renjie ^[1]; Wang, Siqi ^[1]; Xia, Yang ^[1]; Zhao, Mervin ^[1];

^[1]; Yang, Sui ^[1]; Li, Quanwei ^[1]; Wang, Ying ^[1]; Wang, Yuan ^[1]; Wang, Lin-Wang ^[3]; MacDonald, Allan H. ^[4];

^[5]

Univ. of California, Berkeley, CA (United States). National Science Foundation (NSF) Nanoscale Science and Engineering Center
Univ. of Texas, Austin, TX (United States); Univ. of Maryland, College Park, MD (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
Univ. of Texas, Austin, TX (United States)
Univ. of California, Berkeley, CA (United States). National Science Foundation (NSF) Nanoscale Science and Engineering Center; Univ. of Hong Kong (China)

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 CsPbBr₃perovskite cavity without any external fields. We report these polaritons exhibit strong nonlinear behavior that leads to a coherent polariton condensate with a prominent blue shift. Furthermore, the REPs in CsPbBr₃are 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.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Computing California Inst. of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis (JCAP); Univ. of California, Oakland, CA (United States); Nanoscale Science Research Centers (NSRCs) (United States). The Molecular Foundry (TMF)

Sponsoring Organization:: USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR); US Department of the Navy, Office of Naval Research (ONR); National Science Foundation (NSF); US Army Research Office (ARO); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; SC0004993; N00014-17-1-2588; 1725335; W911NF-17-1-0312

OSTI ID:: 1565966

Alternate ID(s):: OSTI ID: 1577788

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Vol. 116, Issue 41; ISSN 0027-8424

Publisher:: National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 38 works

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

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