Strong Electron–Phonon Coupling and Self-Trapped Excitons in the Defect Halide Perovskites A3M2I9 (A = Cs, Rb; M = Bi, Sb)
Abstract
The optical and electronic properties of Bridgman grown single crystals of the wide-bandgap semiconducting defect halide perovskites A3M2I9 (A = Cs, Rb; M = Bi, Sb) have been investigated. Intense Raman scattering was observed at room temperature for each compound, indicating high polarizability and strong electron–phonon coupling. Both low-temperature and room-temperature photoluminescence (PL) were measured for each compound. Cs3Sb2I9 and Rb3Sb2I9 have broad PL emission bands between 1.75 and 2.05 eV with peaks at 1.96 and 1.92 eV, respectively. The Cs3Bi2I9 PL spectra showed broad emission consisting of several overlapping bands in the 1.65–2.2 eV range. Evidence of strong electron–phonon coupling comparable to that of the alkali halides was observed in phonon broadening of the PL emission. Effective phonon energies obtained from temperature-dependent PL measurements were in agreement with the Raman peak energies. A model is proposed whereby electron–phonon interactions in Cs3Sb2I9, Rb3Sb2I9, and Cs3Bi2I9 induce small polarons, resulting in trapping of excitons by the lattice. The recombination of these self-trapped excitons is responsible for the broad PL emission. Finally, Rb3Bi2I9, Rb3Sb2I9, and Cs3Bi2I9 exhibit high resistivity and photoconductivity response under laser photoexcitation, indicating that these compounds possess potential as semiconductor hard radiation detector materials.
- Authors:
-
[1];
[2];
[2];
[3]
- Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry and Dept. of Materials Science and Engineering
- Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
- Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
- Publication Date:
- Research Org.:
- Northwestern Univ., Evanston, IL (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1494819
- Grant/Contract Number:
- NA0002522; AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 29; Journal Issue: 9; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
McCall, Kyle M., Stoumpos, Constantinos C., Kostina, Svetlana S., Kanatzidis, Mercouri G., and Wessels, Bruce W. Strong Electron–Phonon Coupling and Self-Trapped Excitons in the Defect Halide Perovskites A3M2I9 (A = Cs, Rb; M = Bi, Sb). United States: N. p., 2017.
Web. doi:10.1021/acs.chemmater.7b01184.
McCall, Kyle M., Stoumpos, Constantinos C., Kostina, Svetlana S., Kanatzidis, Mercouri G., & Wessels, Bruce W. Strong Electron–Phonon Coupling and Self-Trapped Excitons in the Defect Halide Perovskites A3M2I9 (A = Cs, Rb; M = Bi, Sb). United States. https://doi.org/10.1021/acs.chemmater.7b01184
McCall, Kyle M., Stoumpos, Constantinos C., Kostina, Svetlana S., Kanatzidis, Mercouri G., and Wessels, Bruce W. Thu .
"Strong Electron–Phonon Coupling and Self-Trapped Excitons in the Defect Halide Perovskites A3M2I9 (A = Cs, Rb; M = Bi, Sb)". United States. https://doi.org/10.1021/acs.chemmater.7b01184. https://www.osti.gov/servlets/purl/1494819.
@article{osti_1494819,
title = {Strong Electron–Phonon Coupling and Self-Trapped Excitons in the Defect Halide Perovskites A3M2I9 (A = Cs, Rb; M = Bi, Sb)},
author = {McCall, Kyle M. and Stoumpos, Constantinos C. and Kostina, Svetlana S. and Kanatzidis, Mercouri G. and Wessels, Bruce W.},
abstractNote = {The optical and electronic properties of Bridgman grown single crystals of the wide-bandgap semiconducting defect halide perovskites A3M2I9 (A = Cs, Rb; M = Bi, Sb) have been investigated. Intense Raman scattering was observed at room temperature for each compound, indicating high polarizability and strong electron–phonon coupling. Both low-temperature and room-temperature photoluminescence (PL) were measured for each compound. Cs3Sb2I9 and Rb3Sb2I9 have broad PL emission bands between 1.75 and 2.05 eV with peaks at 1.96 and 1.92 eV, respectively. The Cs3Bi2I9 PL spectra showed broad emission consisting of several overlapping bands in the 1.65–2.2 eV range. Evidence of strong electron–phonon coupling comparable to that of the alkali halides was observed in phonon broadening of the PL emission. Effective phonon energies obtained from temperature-dependent PL measurements were in agreement with the Raman peak energies. A model is proposed whereby electron–phonon interactions in Cs3Sb2I9, Rb3Sb2I9, and Cs3Bi2I9 induce small polarons, resulting in trapping of excitons by the lattice. The recombination of these self-trapped excitons is responsible for the broad PL emission. Finally, Rb3Bi2I9, Rb3Sb2I9, and Cs3Bi2I9 exhibit high resistivity and photoconductivity response under laser photoexcitation, indicating that these compounds possess potential as semiconductor hard radiation detector materials.},
doi = {10.1021/acs.chemmater.7b01184},
journal = {Chemistry of Materials},
number = 9,
volume = 29,
place = {United States},
year = {Thu Apr 20 00:00:00 EDT 2017},
month = {Thu Apr 20 00:00:00 EDT 2017}
}
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Tin Halide Perovskite (ASnX 3 ) Solar Cells: A Comprehensive Guide toward the Highest Power Conversion Efficiency
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Transformation of Perovskite BaBiO 3 into Layered BaBiO 2.5 Crystals Featuring Unusual Chemical Bonding and Luminescence
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Surprising discoveries on the way to an old compound: four transient iodido antimonates
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Distinct green electroluminescence from lead-free CsCuBr 2 halide micro-crosses
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Enhanced On–Off Ratio Photodetectors Based on Lead‐Free Cs 3 Bi 2 I 9 Single Crystal Thin Films
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“Unleaded” Perovskites: Status Quo and Future Prospects of Tin‐Based Perovskite Solar Cells
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Colloidal Synthesis and Optical Properties of All‐Inorganic Low‐Dimensional Cesium Copper Halide Nanocrystals
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Rational design of a triiodide-intercalated dielectric-switching hybrid for visible-light absorption
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