@article{c34566730a5a42a880256e6cd55ae8cc,
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 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{\textquoteright}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.",
keywords = "Cavit, Condensate, Perovskite, Polariton, Rydberg exciton",
author = "Wei Bao and Xiaoze Liu and Fei Xue and Fan Zheng and Renjie Tao and Siqi Wang and Yang Xia and Mervin Zhao and Jeongmin Kim and Sui Yang and Quanwei Li and Ying Wang and Yuan Wang and Wang, {Lin Wang} and MacDonald, {Allan H.} and Xiang Zhang",
note = "Funding Information: ACKNOWLEDGMENTS. W.B. thanks Prof. E. Yablonovitch for valuable advice and discussion of the manuscript. W.B., X.L., R.T., S.W., Y.X., M.Z., J.K., S.Y., Q.L., Ying Wang, Yuan Wang, and X.Z. acknowledge the support from the US Office of Naval Research Multidisciplinary University Research Initiatives (MURI) program (Grant N00014-17-1-2588) and the NSF under Major Research Instrumentation Grant 1725335. Work at University of Texas at Austin was supported by the Army Research Office Grant W911NF-17-1-0312 (MURI). F.X. acknowledges support under the Cooperative Research Agreement between the University of Maryland and the National Institute of Standards and Technology Physical Measurement Laboratory, Award 70NANB14H209, through the University of Maryland. F.Z. and L.-W.W. thank the Joint Center for Artificial Photosynthesis, a US Department of Energy Innovation Hub, supported through the Office of Science of the US Department of Energy under Award DE-SC0004993. F.Z. and L.-W.W. used the resources of National Energy Research Scientific Computing Center located in Lawrence Berkeley National Laboratory and the computational resources of the Oak Ridge Leadership Computing Facility at the Oak Ridge National Laboratory, under the Innovative and Novel Computational Impact on Theory and Experiment project. The authors also acknowledge the facility support at the Molecular Foundry by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract DE-AC02-05CH11231. Funding Information: W.B. thanks Prof. E. Yablonovitch for valuable advice and discussion of the manuscript. W.B., X.L., R.T., S.W., Y.X., M.Z., J.K., S.Y., Q.L., Ying Wang, Yuan Wang, and X.Z. acknowledge the support from the US Office of Naval Research Multidisciplinary University Research Initiatives (MURI) program (Grant N00014-17-1-2588) and the NSF under Major Research Instrumentation Grant 1725335. Work at University of Texas at Austin was supported by the Army Research Office Grant W911NF-17-1-0312 (MURI). F.X. acknowledges support under the Cooperative Research Agreement between the University of Maryland and the National Institute of Standards and Technology Physical Measurement Laboratory, Award 70NANB14H209, through the University of Maryland. F.Z. and L.-W.W. thank the Joint Center for Artificial Photosynthesis, a US Department of Energy Innovation Hub, supported through the Office of Science of the US Department of Energy under Award DE-SC0004993. F.Z. and L.-W.W. used the resources of National Energy Research Scientific Computing Center located in Lawrence Berkeley National Laboratory and the computational resources of the Oak Ridge Leadership Computing Facility at the Oak Ridge National Laboratory, under the Innovative and Novel Computational Impact on Theory and Experiment project. The authors also acknowledge the facility support at the Molecular Foundry by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract DE-AC02-05CH11231. Publisher Copyright: {\textcopyright} 2019 National Academy of Sciences. All rights reserved.",
year = "2019",
month = oct,
day = "8",
doi = "10.1073/pnas.1909948116",
language = "English (US)",
volume = "116",
pages = "20274--20279",
journal = "Proceedings of the National Academy of Sciences of the United States of America",
issn = "0027-8424",
publisher = "National Academy of Sciences",
number = "41",
}