Exciton–Polaritons in CsPbBr3 Crystals Revealed by Optical Reflectivity in High Magnetic Fields and Two-Photon Spectroscopy

Yakovlev, Dmitri R.; Crooker, Scott A.; Semina, Marina A.; Rautert, Janina; Mund, Johannes; Dirin, Dmitry N.; Kovalenko, Maksym V.; Bayer, Manfred

doi:10.1002/pssr.202300407

Exciton–Polaritons in CsPbBr₃ Crystals Revealed by Optical Reflectivity in High Magnetic Fields and Two-Photon Spectroscopy

Journal Article · Mon Nov 06 00:00:00 EST 2023 · Physica Status Solidi. Rapid Research Letters

DOI:https://doi.org/10.1002/pssr.202300407· OSTI ID:2208801

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Technische Universität Dortmund (Germany)
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Russian Academy of Sciences (RAS), St. Petersburg (Russian Federation)
Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland); Swiss Federal Laboratories for Materials Science and Technology (Empa), Dübendorf (Switzerland)

Cesium lead bromide (CsPbBr3) is a representative material of the emerging class of lead halide perovskite semiconductors that possess remarkable optoelectronic properties. Its optical properties in the vicinity of the bandgap energy are greatly contributed by excitons, which form exciton polaritons due to strong light–matter interactions. Exciton–polaritons in solution-grown CsPbBr₃ crystals are examined by means of circularly polarized reflection spectroscopy measured in high magnetic fields up to 60 T. The excited 2P exciton state is measured by two-photon absorption. Comprehensive modeling and analysis provides detailed quantitative information about the exciton–polariton parameters: exciton binding energy of 32.5 meV, oscillator strength characterized by longitudinal–transverse splitting of 5.3 meV, damping of 6.7 meV, reduced exciton mass of 0.18$$m$$₀, exciton diamagnetic shift of 1.6 μeV T^-2, and exciton Landé factor $$g$$_x = + 2.35. It is shown that the exciton states can be described within a hydrogen-like model with an effective dielectric constant of 8.7. From the measured exciton longitudinal–transverse splitting, Kane energy of E_p = 15 eV is evaluated, which is in reasonable agreement with values of 11.8–12.5 eV derived from the carrier effective masses.

View Accepted Manuscript (DOE)

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: National Science Foundation (NSF); Swiss National Science Foundation (SNSF); USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 2208801

Report Number(s):: LA-UR--23-30253

Journal Information:: Physica Status Solidi. Rapid Research Letters, Journal Name: Physica Status Solidi. Rapid Research Letters Journal Issue: 3 Vol. 18; ISSN 1862-6254

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

References (53)

Monolayer and Few-Layer All-Inorganic Perovskites as a New Family of Two-Dimensional Semiconductors for Printable Optoelectronic Devices Song, Jizhong; Xu, Leimeng; Li, Jianhai Advanced Materials, Vol. 28, Issue 24 https://doi.org/10.1002/adma.201600225	journal	April 2016
Sensitive Direct Converting X‐Ray Detectors Utilizing Crystalline CsPbBr ₃ Perovskite Films Fabricated via Scalable Melt Processing Matt, Gebhard J.; Levchuk, Ievgen; Knüttel, Judith Advanced Materials Interfaces, Vol. 7, Issue 4 https://doi.org/10.1002/admi.201901575	journal	January 2020
Solution‐Processed MAPbBr ₃ and CsPbBr ₃ Single‐Crystal Detectors with Improved X‐Ray Sensitivity via Interfacial Engineering Fan, Zhengfang; Liu, Jiang; Zuo, Wentao physica status solidi (a), Vol. 217, Issue 9 https://doi.org/10.1002/pssa.202000104	journal	March 2020
Longitudinal and Transverse Excitons in Semiconductors Denisov, M. M.; Makarov, V. P. Physica Status Solidi (b), Vol. 56, Issue 1 https://doi.org/10.1002/pssb.2220560102	journal	March 1973
Longitudinal-transverse splitting in Wannier excitons and polariton states Andreani, L. C.; Bassani, F.; Quattropani, A. Il Nuovo Cimento D, Vol. 10, Issue 12 https://doi.org/10.1007/BF02454213	journal	December 1988
Semiconductor Optics Klingshirn, Claus Advanced Texts in Physics https://doi.org/10.1007/b138175	book	January 2005
Cesium-trihalogen-plumbates a new class of ionic semiconductors Fröhlich, D.; Heidrich, K.; Künzel, H. Journal of Luminescence, Vol. 18-19 https://doi.org/10.1016/0022-2313(79)90146-7	journal	January 1979
Band structure of indium antimonide Kane, Evan O. Journal of Physics and Chemistry of Solids, Vol. 1, Issue 4 https://doi.org/10.1016/0022-3697(57)90013-6	journal	January 1957
On some observable properties of longitudinal excitons Hopfield, J. J.; Thomas, D. G. Journal of Physics and Chemistry of Solids, Vol. 12, Issue 3-4 https://doi.org/10.1016/0022-3697(60)90049-4	journal	February 1960
Optical properties and electronic structure of CsPbCl3 and CsPbBr3 Heidrich, K.; Künzel, H.; Treusch, J. Solid State Communications, Vol. 25, Issue 11 https://doi.org/10.1016/0038-1098(78)90294-6	journal	March 1978
Magnetoabsorption of the lowest exciton in perovskite-type compound (CH3NH3)PbI3 Hirasawa, M.; Ishihara, T.; Goto, T. Physica B: Condensed Matter, Vol. 201 https://doi.org/10.1016/0921-4526(94)91130-4	journal	July 1994
Comparative study on the excitons in lead-halide-based perovskite-type crystals CH₃NH₃PbBr₃ CH₃NH₃PbI₃ Tanaka, Kenichiro; Takahashi, Takayuki; Ban, Takuma Solid State Communications, Vol. 127, Issue 9-10, p. 619-623 https://doi.org/10.1016/S0038-1098(03)00566-0	journal	September 2003
Solution-Grown CsPbBr ₃ Perovskite Single Crystals for Photon Detection Dirin, Dmitry N.; Cherniukh, Ihor; Yakunin, Sergii Chemistry of Materials, Vol. 28, Issue 23 https://doi.org/10.1021/acs.chemmater.6b04298	journal	November 2016
How Important Is the Organic Part of Lead Halide Perovskite Photovoltaic Cells? Efficient CsPbBr ₃ Cells Kulbak, Michael; Cahen, David; Hodes, Gary The Journal of Physical Chemistry Letters, Vol. 6, Issue 13 https://doi.org/10.1021/acs.jpclett.5b00968	journal	June 2015
Cesium Enhances Long-Term Stability of Lead Bromide Perovskite-Based Solar Cells Kulbak, Michael; Gupta, Satyajit; Kedem, Nir The Journal of Physical Chemistry Letters, Vol. 7, Issue 1 https://doi.org/10.1021/acs.jpclett.5b02597	journal	December 2015
Unraveling the Exciton Binding Energy and the Dielectric Constant in Single-Crystal Methylammonium Lead Triiodide Perovskite Yang, Zhuo; Surrente, Alessandro; Galkowski, Krzysztof The Journal of Physical Chemistry Letters, Vol. 8, Issue 8 https://doi.org/10.1021/acs.jpclett.7b00524	journal	April 2017
Exciton Binding Energy in CdSe Nanoplatelets Measured by One- and Two-Photon Absorption Shornikova, Elena V.; Yakovlev, Dmitri R.; Gippius, Nikolay A. Nano Letters, Vol. 21, Issue 24 https://doi.org/10.1021/acs.nanolett.1c04159	journal	December 2021
Giant Fine Structure Splitting of the Bright Exciton in a Bulk MAPbBr₃ Single Crystal Baranowski, Michał; Galkowski, Krzysztof; Surrente, Alessandro Nano Letters, Vol. 19, Issue 10 https://doi.org/10.1021/acs.nanolett.9b02520	journal	September 2019
Impact of the Halide Cage on the Electronic Properties of Fully Inorganic Cesium Lead Halide Perovskites Yang, Z.; Surrente, A.; Galkowski, K. ACS Energy Letters, Vol. 2, Issue 7 https://doi.org/10.1021/acsenergylett.7b00416	journal	June 2017
Efficient Photon Recycling and Radiation Trapping in Cesium Lead Halide Perovskite Waveguides Dursun, Ibrahim; Zheng, Yangzi; Guo, Tianle ACS Energy Letters, Vol. 3, Issue 7 https://doi.org/10.1021/acsenergylett.8b00758	journal	May 2018
Crystal Growth of the Perovskite Semiconductor CsPbBr ₃ : A New Material for High-Energy Radiation Detection Stoumpos, Constantinos C.; Malliakas, Christos D.; Peters, John A. Crystal Growth & Design, Vol. 13, Issue 7 https://doi.org/10.1021/cg400645t	journal	June 2013
Transformation of Sintered CsPbBr ₃ Nanocrystals to Cubic CsPbI ₃ and Gradient CsPbBr _x I _{3– x} through Halide Exchange Hoffman, Jacob B.; Schleper, A. Lennart; Kamat, Prashant V. Journal of the American Chemical Society, Vol. 138, Issue 27 https://doi.org/10.1021/jacs.6b04661	journal	June 2016
Bright triplet excitons in caesium lead halide perovskites Becker, Michael A.; Vaxenburg, Roman; Nedelcu, Georgian Nature, Vol. 553, Issue 7687 https://doi.org/10.1038/nature25147	journal	January 2018
Exciton diamagnetic shifts and valley Zeeman effects in monolayer WS2 and MoS2 to 65 Tesla Stier, Andreas V.; McCreary, Kathleen M.; Jonker, Berend T. Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms10643	journal	February 2016
Direct measurement of the exciton binding energy and effective masses for charge carriers in organic–inorganic tri-halide perovskites Miyata, Atsuhiko; Mitioglu, Anatolie; Plochocka, Paulina Nature Physics, Vol. 11, Issue 7 https://doi.org/10.1038/nphys3357	journal	June 2015
Coherent spin dynamics of electrons and holes in CsPbBr3 perovskite crystals Belykh, Vasilii V.; Yakovlev, Dmitri R.; Glazov, Mikhail M. Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-08625-z	journal	February 2019
Dynamic emission Stokes shift and liquid-like dielectric solvation of band edge carriers in lead-halide perovskites Guo, Yinsheng; Yaffe, Omer; Hull, Trevor D. Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-09057-5	journal	March 2019
The Landé factors of electrons and holes in lead halide perovskites: universal dependence on the band gap Kirstein, E.; Yakovlev, D. R.; Glazov, M. M. Nature Communications, Vol. 13, Issue 1 https://doi.org/10.1038/s41467-022-30701-0	journal	June 2022
Perovskite semiconductors for room-temperature exciton-polaritonics Su, Rui; Fieramosca, Antonio; Zhang, Qing Nature Materials, Vol. 20, Issue 10 https://doi.org/10.1038/s41563-021-01035-x	journal	July 2021
Halide perovskites enable polaritonic XY spin Hamiltonian at room temperature Tao, Renjie; Peng, Kai; Haeberlé, Louis Nature Materials, Vol. 21, Issue 7 https://doi.org/10.1038/s41563-022-01276-4	journal	June 2022
Observation of exciton polariton condensation in a perovskite lattice at room temperature Su, Rui; Ghosh, Sanjib; Wang, Jun Nature Physics, Vol. 16, Issue 3 https://doi.org/10.1038/s41567-019-0764-5	journal	January 2020
Effective-mass model and magneto-optical properties in hybrid perovskites Yu, Z. G. Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/srep28576	journal	June 2016
Determination of the exciton binding energy and effective masses for methylammonium and formamidinium lead tri-halide perovskite semiconductors Galkowski, Krzysztof; Mitioglu, Anatolie; Miyata, Atsuhiko Energy & Environmental Science, Vol. 9, Issue 3 https://doi.org/10.1039/C5EE03435C	journal	January 2016
Low defects density CsPbBr ₃ single crystals grown by an additive assisted method for gamma-ray detection Feng, Yuanxiang; Pan, Lei; Wei, Haotong Journal of Materials Chemistry C, Vol. 8, Issue 33 https://doi.org/10.1039/D0TC02706E	journal	January 2020
Electron–phonon coupling in CsPbBr₃ Zhou, Xianzhong; Zhang, Ziyang AIP Advances, Vol. 10, Issue 12 https://doi.org/10.1063/5.0017149	journal	December 2020
Charge carrier mobility of halide perovskite single crystals for ionizing radiation detection Zhang, Zheng; Saparov, Bayram Applied Physics Letters, Vol. 119, Issue 3 https://doi.org/10.1063/5.0057411	journal	July 2021
Halide Perovskites for Photonics Vinattieri, Anna; Giorgi, Giacomo https://doi.org/10.1063/9780735423633	book	December 2021
Observation of Rydberg exciton polaritons and their condensate in a perovskite cavity Bao, Wei; Liu, Xiaoze; Xue, Fei Proceedings of the National Academy of Sciences, Vol. 116, Issue 41 https://doi.org/10.1073/pnas.1909948116	journal	September 2019
Energy levels of a neutral hydrogen-like system in a constant magnetic field of arbitrary strength Makado, P. C.; McGill, N. C. Journal of Physics C: Solid State Physics, Vol. 19, Issue 6 https://doi.org/10.1088/0022-3719/19/6/008	journal	February 1986
Diamagnetic excitons and exciton magnetopolaritons in semiconductors Seisyan, R. P. Semiconductor Science and Technology, Vol. 27, Issue 5 https://doi.org/10.1088/0268-1242/27/5/053001	journal	April 2012
Theoretical and Experimental Effects of Spatial Dispersion on the Optical Properties of Crystals Hopfield, J. J.; Thomas, D. G. Physical Review, Vol. 132, Issue 2 https://doi.org/10.1103/PhysRev.132.563	journal	October 1963
Electronic structure, photoemission spectra, and vacuum-ultraviolet optical spectra of CsPb Cl 3 and CsPb Br 3 Heidrich, K.; Schäfer, W.; Schreiber, M. Physical Review B, Vol. 24, Issue 10 https://doi.org/10.1103/PhysRevB.24.5642	journal	November 1981
Energy Levels of Direct Excitons in Semiconductors with Degenerate Bands Baldereschi, A.; Lipari, Nunzio C. Physical Review B, Vol. 3, Issue 2 https://doi.org/10.1103/PhysRevB.3.439	journal	January 1971
Magneto-optical study on excitonic spectra in ( C 6 H 13 NH 3 ) 2 PbI 4 Kataoka, Takeshi; Kondo, Takashi; Ito, Ryoichi Physical Review B, Vol. 47, Issue 4 https://doi.org/10.1103/PhysRevB.47.2010	journal	January 1993
Short-range versus long-range electron-hole exchange interactions in semiconductor quantum dots Franceschetti, A.; Wang, L. W.; Fu, H. Physical Review B, Vol. 58, Issue 20 https://doi.org/10.1103/PhysRevB.58.R13367	journal	November 1998
Spherical Model of Shallow Acceptor States in Semiconductors Baldereschi, A.; Lipari, Nunzio O. Physical Review B, Vol. 8, Issue 6 https://doi.org/10.1103/PhysRevB.8.2697	journal	September 1973
Electronic model for self-assembled hybrid organic/perovskite semiconductors: Reverse band edge electronic states ordering and spin-orbit coupling Even, J.; Pedesseau, L.; Dupertuis, M. -A. Physical Review B, Vol. 86, Issue 20 https://doi.org/10.1103/PhysRevB.86.205301	journal	November 2012
Cubic contributions to the spherical model of shallow acceptor states Baldereschi, A.; Lipari, Nunzio O. Physical Review B, Vol. 9, Issue 4 https://doi.org/10.1103/PhysRevB.9.1525	journal	February 1974
Evidence of Large Polarons in Photoemission Band Mapping of the Perovskite Semiconductor CsPbBr 3 Puppin, M.; Polishchuk, S.; Colonna, N. Physical Review Letters, Vol. 124, Issue 20 https://doi.org/10.1103/PhysRevLett.124.206402	journal	May 2020
Large polarons in lead halide perovskites Miyata, Kiyoshi; Meggiolaro, Daniele; Trinh, M. Tuan Science Advances, Vol. 3, Issue 8 https://doi.org/10.1126/sciadv.1701217	journal	August 2017
Electronic and Excitonic Structures of Inorganic–Organic Perovskite-Type Quantum-Well Crystal (C ₄ H ₉ NH ₃ ) ₂ PbBr ₄ Tanaka, Kenichiro; Takahashi, Takayuki; Kondo, Takashi Japanese Journal of Applied Physics, Vol. 44, Issue 8 https://doi.org/10.1143/JJAP.44.5923	journal	August 2005
Optical and Photoelectronic Studies of CsPbCl₃and CsPbBr₃ Ito, Hisao; Onuki, Hideo; Onaka, Ryumyo Journal of the Physical Society of Japan, Vol. 45, Issue 6 https://doi.org/10.1143/JPSJ.45.2043	journal	December 1978
Exciton binding energy and effective mass of CsPbCl ₃ : a magneto-optical study Baranowski, Michal; Plochocka, Paulina; Su, Rui Photonics Research, Vol. 8, Issue 10 https://doi.org/10.1364/PRJ.401872	journal	January 2020

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Exciton–Polaritons in CsPbBr3 Crystals Revealed by Optical Reflectivity in High Magnetic Fields and Two-Photon Spectroscopy

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Exciton–Polaritons in CsPbBr₃ Crystals Revealed by Optical Reflectivity in High Magnetic Fields and Two-Photon Spectroscopy