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Title: Atomic Structure and Electrical Activity of Grain Boundaries and Ruddlesden-Popper Faults in Cesium Lead Bromide Perovskite

Abstract

To evaluate the role of planar defects in lead-halide perovskites—cheap, versatile semiconducting materials—it is critical to examine their structure, including defects, at the atomic scale and develop a detailed understanding of their impact on electronic properties. In this study, postsynthesis nanocrystal fusion, aberration-corrected scanning transmission electron microscopy, and first-principles calculations are combined to study the nature of different planar defects formed in CsPbBr3 nanocrystals. Two types of prevalent planar defects from atomic resolution imaging are observed: previously unreported Br-rich [001](210)Σ5 grain boundaries (GBs) and Ruddlesden–Popper (RP) planar faults. The first-principles calculations reveal that neither of these planar faults induce deep defect levels, but their Br-deficient counterparts do. It is found that the Σ5 GB repels electrons and attracts holes, similar to an n–p–n junction, and the RP planar defects repel both electrons and holes, similar to a semiconductor–insulator–semiconductor junction. Finally, the potential applications of these findings and their implications to understand the planar defects in organic–inorganic lead-halide perovskites that have led to solar cells with extremely high photoconversion efficiencies are discussed.

Authors:
 [1];  [1]; ORCiD logo [2];  [3];  [1]; ORCiD logo [2];  [2];  [3]; ORCiD logo [1]
  1. Washington Univ., St. Louis, MO (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Univ. of Missouri, Columbia, MO (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1493984
Alternate Identifier(s):
OSTI ID: 1484312
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 31; Journal Issue: 4; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Thind, Arashdeep Singh, Luo, Guangfu, Hachtel, Jordan A., Morrell, Maria V., Cho, Sung Beom, Borisevich, Albina Y., Idrobo, Juan-Carlos, Xing, Yangchuan, and Mishra, Rohan. Atomic Structure and Electrical Activity of Grain Boundaries and Ruddlesden-Popper Faults in Cesium Lead Bromide Perovskite. United States: N. p., 2018. Web. doi:10.1002/adma.201805047.
Thind, Arashdeep Singh, Luo, Guangfu, Hachtel, Jordan A., Morrell, Maria V., Cho, Sung Beom, Borisevich, Albina Y., Idrobo, Juan-Carlos, Xing, Yangchuan, & Mishra, Rohan. Atomic Structure and Electrical Activity of Grain Boundaries and Ruddlesden-Popper Faults in Cesium Lead Bromide Perovskite. United States. doi:10.1002/adma.201805047.
Thind, Arashdeep Singh, Luo, Guangfu, Hachtel, Jordan A., Morrell, Maria V., Cho, Sung Beom, Borisevich, Albina Y., Idrobo, Juan-Carlos, Xing, Yangchuan, and Mishra, Rohan. Mon . "Atomic Structure and Electrical Activity of Grain Boundaries and Ruddlesden-Popper Faults in Cesium Lead Bromide Perovskite". United States. doi:10.1002/adma.201805047.
@article{osti_1493984,
title = {Atomic Structure and Electrical Activity of Grain Boundaries and Ruddlesden-Popper Faults in Cesium Lead Bromide Perovskite},
author = {Thind, Arashdeep Singh and Luo, Guangfu and Hachtel, Jordan A. and Morrell, Maria V. and Cho, Sung Beom and Borisevich, Albina Y. and Idrobo, Juan-Carlos and Xing, Yangchuan and Mishra, Rohan},
abstractNote = {To evaluate the role of planar defects in lead-halide perovskites—cheap, versatile semiconducting materials—it is critical to examine their structure, including defects, at the atomic scale and develop a detailed understanding of their impact on electronic properties. In this study, postsynthesis nanocrystal fusion, aberration-corrected scanning transmission electron microscopy, and first-principles calculations are combined to study the nature of different planar defects formed in CsPbBr3 nanocrystals. Two types of prevalent planar defects from atomic resolution imaging are observed: previously unreported Br-rich [001](210)Σ5 grain boundaries (GBs) and Ruddlesden–Popper (RP) planar faults. The first-principles calculations reveal that neither of these planar faults induce deep defect levels, but their Br-deficient counterparts do. It is found that the Σ5 GB repels electrons and attracts holes, similar to an n–p–n junction, and the RP planar defects repel both electrons and holes, similar to a semiconductor–insulator–semiconductor junction. Finally, the potential applications of these findings and their implications to understand the planar defects in organic–inorganic lead-halide perovskites that have led to solar cells with extremely high photoconversion efficiencies are discussed.},
doi = {10.1002/adma.201805047},
journal = {Advanced Materials},
issn = {0935-9648},
number = 4,
volume = 31,
place = {United States},
year = {2018},
month = {12}
}

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Works referenced in this record:

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Projector augmented-wave method
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Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
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