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Title: Do grain boundaries dominate non-radiative recombination in CH 3NH 3PbI 3 perovskite thin films?

Here, we examine GBs with respect to non-GB regions (grain surfaces (GSs) and grain interiors (GIs)) in high-quality micrometer-sized perovskite CH 3NH 3PbI 3 (or MAPbI 3) thin films using high-resolution confocal fluorescence-lifetime imaging microscopy in conjunction with kinetic modeling of charge-transport and recombination processes. We show that, contrary to previous studies, GBs in our perovskite MAPbI3 thin films do not lead to increased recombination but that recombination in these films happens primarily in the non-GB regions (i.e., GSs or GIs). We also find that GBs in these films are not transparent to photogenerated carriers, which is likely associated with a potential barrier at GBs. Lastly, even though GBs generally display lower luminescence intensities than GSs/GIs, the lifetimes at GBs are no worse than those at GSs/GIs, further suggesting that GBs do not dominate non-radiative recombination in MAPbI 3 thin films.
Authors:
 [1] ;  [2] ; ORCiD logo [1] ;  [1] ;  [3] ; ORCiD logo [1] ;  [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States). Chemistry and Nanoscience Center
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States). Biosciences Center
  3. National Renewable Energy Lab. (NREL), Golden, CO (United States). Material Science Center
Publication Date:
Report Number(s):
NREL/JA-5900-66143
Journal ID: ISSN 1463-9076; PPCPFQ; TRN: US1700984
Grant/Contract Number:
AC36-08GO28308
Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 19; Journal Issue: 7; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Research Org:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Solar Energy Technologies Office (EE-4S); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE; grain boundaries; grain surfaces; grain interiors; perovskite thin films
OSTI Identifier:
1344765

Yang, Mengjin, Zeng, Yining, Li, Zhen, Kim, Dong Hoe, Jiang, Chun-Sheng, van de Lagemaat, Jao, and Zhu, Kai. Do grain boundaries dominate non-radiative recombination in CH3NH3PbI 3 perovskite thin films?. United States: N. p., Web. doi:10.1039/C6CP08770A.
Yang, Mengjin, Zeng, Yining, Li, Zhen, Kim, Dong Hoe, Jiang, Chun-Sheng, van de Lagemaat, Jao, & Zhu, Kai. Do grain boundaries dominate non-radiative recombination in CH3NH3PbI 3 perovskite thin films?. United States. doi:10.1039/C6CP08770A.
Yang, Mengjin, Zeng, Yining, Li, Zhen, Kim, Dong Hoe, Jiang, Chun-Sheng, van de Lagemaat, Jao, and Zhu, Kai. 2017. "Do grain boundaries dominate non-radiative recombination in CH3NH3PbI 3 perovskite thin films?". United States. doi:10.1039/C6CP08770A. https://www.osti.gov/servlets/purl/1344765.
@article{osti_1344765,
title = {Do grain boundaries dominate non-radiative recombination in CH3NH3PbI 3 perovskite thin films?},
author = {Yang, Mengjin and Zeng, Yining and Li, Zhen and Kim, Dong Hoe and Jiang, Chun-Sheng and van de Lagemaat, Jao and Zhu, Kai},
abstractNote = {Here, we examine GBs with respect to non-GB regions (grain surfaces (GSs) and grain interiors (GIs)) in high-quality micrometer-sized perovskite CH3NH3PbI3 (or MAPbI3) thin films using high-resolution confocal fluorescence-lifetime imaging microscopy in conjunction with kinetic modeling of charge-transport and recombination processes. We show that, contrary to previous studies, GBs in our perovskite MAPbI3 thin films do not lead to increased recombination but that recombination in these films happens primarily in the non-GB regions (i.e., GSs or GIs). We also find that GBs in these films are not transparent to photogenerated carriers, which is likely associated with a potential barrier at GBs. Lastly, even though GBs generally display lower luminescence intensities than GSs/GIs, the lifetimes at GBs are no worse than those at GSs/GIs, further suggesting that GBs do not dominate non-radiative recombination in MAPbI3 thin films.},
doi = {10.1039/C6CP08770A},
journal = {Physical Chemistry Chemical Physics. PCCP (Print)},
number = 7,
volume = 19,
place = {United States},
year = {2017},
month = {1}
}

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