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Title: Exploring Polaronic, Excitonic Structures and Luminescence in Cs 4PbBr 6/CsPbBr 3

Abstract

Among the important family of halide perovskites, one particular case of all-inorganic, 0-D Cs 4PbBr 6 and 3-D CsPbBr 3-based nanostructures and thin films is witnessing intense activity due to ultrafast luminescence with high quantum yield. To understand their emissive behavior, we use hybrid density functional calculations to first compare the ground-state electronic structure of the two prospective compounds. The dispersive band edges of CsPbBr 3 do not support self-trapped carriers, which agrees with reports of weak exciton binding energy and high photocurrent. The larger gap 0-D material Cs 4PbBr 6, however, reveals polaronic and excitonic features. We show that those lattice-coupled carriers are likely responsible for observed ultraviolet emission around ~375 nm, reported in bulk Cs 4PbBr 6 and Cs 4PbBr 6/CsPbBr 3 composites. Ionization potential calculations and estimates of type-I band alignment support the notion of quantum confinement leading to fast, green emission from CsPbBr 3 nanostructures embedded in Cs 4PbBr 6.

Authors:
 [1]; ORCiD logo [1]
  1. Univ. of Arkansas, Fayetteville, AR (United States). Dept. of Chemistry and Physics
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1484253
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 9; Journal Issue: 4; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Kang, Byungkyun, and Biswas, Koushik. Exploring Polaronic, Excitonic Structures and Luminescence in Cs4PbBr6/CsPbBr3. United States: N. p., 2018. Web. doi:10.1021/acs.jpclett.7b03333.
Kang, Byungkyun, & Biswas, Koushik. Exploring Polaronic, Excitonic Structures and Luminescence in Cs4PbBr6/CsPbBr3. United States. doi:10.1021/acs.jpclett.7b03333.
Kang, Byungkyun, and Biswas, Koushik. Mon . "Exploring Polaronic, Excitonic Structures and Luminescence in Cs4PbBr6/CsPbBr3". United States. doi:10.1021/acs.jpclett.7b03333. https://www.osti.gov/servlets/purl/1484253.
@article{osti_1484253,
title = {Exploring Polaronic, Excitonic Structures and Luminescence in Cs4PbBr6/CsPbBr3},
author = {Kang, Byungkyun and Biswas, Koushik},
abstractNote = {Among the important family of halide perovskites, one particular case of all-inorganic, 0-D Cs4PbBr6 and 3-D CsPbBr3-based nanostructures and thin films is witnessing intense activity due to ultrafast luminescence with high quantum yield. To understand their emissive behavior, we use hybrid density functional calculations to first compare the ground-state electronic structure of the two prospective compounds. The dispersive band edges of CsPbBr3 do not support self-trapped carriers, which agrees with reports of weak exciton binding energy and high photocurrent. The larger gap 0-D material Cs4PbBr6, however, reveals polaronic and excitonic features. We show that those lattice-coupled carriers are likely responsible for observed ultraviolet emission around ~375 nm, reported in bulk Cs4PbBr6 and Cs4PbBr6/CsPbBr3 composites. Ionization potential calculations and estimates of type-I band alignment support the notion of quantum confinement leading to fast, green emission from CsPbBr3 nanostructures embedded in Cs4PbBr6.},
doi = {10.1021/acs.jpclett.7b03333},
journal = {Journal of Physical Chemistry Letters},
issn = {1948-7185},
number = 4,
volume = 9,
place = {United States},
year = {2018},
month = {2}
}

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Cited by: 48 works
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Works referencing / citing this record:

Highly Emissive Self-Trapped Excitons in Fully Inorganic Zero-Dimensional Tin Halides
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  • Su, Ying; Zeng, Qinghui; Chen, Xuejiao
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Highly efficient CsPbBr 3 perovskite nanocrystals induced by structure transformation between CsPbBr 3 and Cs 4 PbBr 6 phases
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  • Su, Ying; Zeng, Qinghui; Chen, Xuejiao
  • Journal of Materials Chemistry C, Vol. 7, Issue 25
  • DOI: 10.1039/c9tc01763a

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  • Benin, Bogdan M.; Dirin, Dmitry N.; Morad, Viktoriia
  • Angewandte Chemie International Edition, Vol. 57, Issue 35
  • DOI: 10.1002/anie.201806452

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