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

Journal Article · 05 November 2023 · Physica Status Solidi. Rapid Research Letters

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

Yakovlev, Dmitri R.  ^[1]; Crooker, Scott A.  ^[2]; Semina, Marina A.  ^[3]; Rautert, Janina  ^[1]; Mund, Johannes  ^[1]; Dirin, Dmitry N.  ^[4]; Kovalenko, Maksym V.  ^[4]; Bayer, Manfred  ^[1]

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1. Technische Universität Dortmund (Germany)
2. Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
3. Russian Academy of Sciences (RAS), St. Petersburg (Russian Federation)
4. 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.

• Research Organization: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
• Sponsoring Organization: USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF); Swiss National Science Foundation (SNSF)
• 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