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

Abstract

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 CsPbBr 3 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 CsPbBr 3 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.

Authors:
; ; ; ; ; ; ; ; ORCiD logo; ; ; ; ; ; ; ORCiD logo
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (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 Org.:
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)
OSTI Identifier:
1565966
Alternate Identifier(s):
OSTI ID: 1577788
Grant/Contract Number:  
SC0004993; AC02-05CH11231; N00014-17-1-2588; 1725335; W911NF-17-1-0312
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 116 Journal Issue: 41; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING; Rydberg exciton; polariton; condensate; perovskite; cavity

Citation Formats

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., and Zhang, Xiang. Observation of Rydberg exciton polaritons and their condensate in a perovskite cavity. United States: N. p., 2019. Web. doi:10.1073/pnas.1909948116.
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. Observation of Rydberg exciton polaritons and their condensate in a perovskite cavity. United States. doi:10.1073/pnas.1909948116.
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., and Zhang, Xiang. Mon . "Observation of Rydberg exciton polaritons and their condensate in a perovskite cavity". United States. doi:10.1073/pnas.1909948116.
@article{osti_1565966,
title = {Observation of Rydberg exciton polaritons and their condensate in a perovskite cavity},
author = {Bao, Wei and Liu, Xiaoze and Xue, Fei and Zheng, Fan and Tao, Renjie and Wang, Siqi and Xia, Yang and Zhao, Mervin and Kim, Jeongmin and Yang, Sui and Li, Quanwei and Wang, Ying and Wang, Yuan and Wang, Lin-Wang and MacDonald, Allan H. and Zhang, Xiang},
abstractNote = {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 CsPbBr 3 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 CsPbBr 3 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.},
doi = {10.1073/pnas.1909948116},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 41,
volume = 116,
place = {United States},
year = {2019},
month = {9}
}

Journal Article:
Free Publicly Available Full Text
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DOI: 10.1073/pnas.1909948116

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Cited by: 3 works
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