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Title: Dipolar cations confer defect tolerance in wide-bandgap metal halide perovskites

Efficient wide-bandgap perovskite solar cells (PSCs) enable high-efficiency tandem photovoltaics when combined with crystalline silicon and other low-bandgap absorbers. However, wide-bandgap PSCs today exhibit performance far inferior to that of sub-1.6-eV bandgap PSCs due to their tendency to form a high density of deep traps. Here, we show that healing the deep traps in wide-bandgap perovskites—in effect, increasing the defect tolerance via cation engineering—enables further performance improvements in PSCs. We achieve a stabilized power conversion efficiency of 20.7% for 1.65-eV bandgap PSCs by incorporating dipolar cations, with a high open-circuit voltage of 1.22 V and a fill factor exceeding 80%. We also obtain a stabilized efficiency of 19.1% for 1.74-eV bandgap PSCs with a high open-circuit voltage of 1.25 V. From density functional theory calculations, we find that the presence and reorientation of the dipolar cation in mixed cation–halide perovskites heals the defects that introduce deep trap states.
Authors:
 [1] ;  [2] ;  [2] ;  [2] ;  [2] ;  [2] ;  [3] ;  [2] ;  [4] ;  [2] ; ORCiD logo [2] ;  [2] ; ORCiD logo [5] ;  [6] ;  [2] ; ORCiD logo [2] ; ORCiD logo [2] ;  [3] ; ORCiD logo [2]
  1. Univ. of Toronto, ON (Canada). Dept. of Electrical and Computer Engineering; Nanjing Univ. (China). National Lab. of Solid State Microstructures. Collaborative Innovation Centre of Advanced Microstructures. Jiangsu Key Lab. of Artificial Functional Materials. College of Engineering and Applied Sciences
  2. Univ. of Toronto, ON (Canada). Dept. of Electrical and Computer Engineering
  3. Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  4. Univ. of Toronto, ON (Canada). Dept. of Electrical and Computer Engineering; Henan Univ., Kaifeng (China). Key Lab. of Photovoltaic Materials. Dept. of Physics and Electronics
  5. Univ. of Toronto, ON (Canada). Dept. of Electrical and Computer Engineering; KU Leuven (Belgium). Dept. of Chemistry
  6. KU Leuven (Belgium). Dept. of Chemistry
Publication Date:
Grant/Contract Number:
AC02-05CH11231; N00014-17-1-2524; OSR-2017-CPF-3321-03; 680-50-1511
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States); Univ. of Toronto, ON (Canada); Nanjing Univ. (China)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Office of Naval Research (ONR) (United States); King Abdullah Univ. of Science and Technology (KAUST) (Saudi Arabia); Ontario Research Fund Research Excellence Program (Canada); Natural Sciences and Engineering Research Council of Canada (NSERC); Netherlands Organisation for Scientific Research (NWO); Thousand Talent Program for Young Outstanding Scientists (China)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; devices for energy harvesting; solar cells
OSTI Identifier:
1477412

Tan, Hairen, Che, Fanglin, Wei, Mingyang, Zhao, Yicheng, Saidaminov, Makhsud I., Todorović, Petar, Broberg, Danny, Walters, Grant, Tan, Furui, Zhuang, Taotao, Sun, Bin, Liang, Zhiqin, Yuan, Haifeng, Fron, Eduard, Kim, Junghwan, Yang, Zhenyu, Voznyy, Oleksandr, Asta, Mark, and Sargent, Edward H.. Dipolar cations confer defect tolerance in wide-bandgap metal halide perovskites. United States: N. p., Web. doi:10.1038/s41467-018-05531-8.
Tan, Hairen, Che, Fanglin, Wei, Mingyang, Zhao, Yicheng, Saidaminov, Makhsud I., Todorović, Petar, Broberg, Danny, Walters, Grant, Tan, Furui, Zhuang, Taotao, Sun, Bin, Liang, Zhiqin, Yuan, Haifeng, Fron, Eduard, Kim, Junghwan, Yang, Zhenyu, Voznyy, Oleksandr, Asta, Mark, & Sargent, Edward H.. Dipolar cations confer defect tolerance in wide-bandgap metal halide perovskites. United States. doi:10.1038/s41467-018-05531-8.
Tan, Hairen, Che, Fanglin, Wei, Mingyang, Zhao, Yicheng, Saidaminov, Makhsud I., Todorović, Petar, Broberg, Danny, Walters, Grant, Tan, Furui, Zhuang, Taotao, Sun, Bin, Liang, Zhiqin, Yuan, Haifeng, Fron, Eduard, Kim, Junghwan, Yang, Zhenyu, Voznyy, Oleksandr, Asta, Mark, and Sargent, Edward H.. 2018. "Dipolar cations confer defect tolerance in wide-bandgap metal halide perovskites". United States. doi:10.1038/s41467-018-05531-8. https://www.osti.gov/servlets/purl/1477412.
@article{osti_1477412,
title = {Dipolar cations confer defect tolerance in wide-bandgap metal halide perovskites},
author = {Tan, Hairen and Che, Fanglin and Wei, Mingyang and Zhao, Yicheng and Saidaminov, Makhsud I. and Todorović, Petar and Broberg, Danny and Walters, Grant and Tan, Furui and Zhuang, Taotao and Sun, Bin and Liang, Zhiqin and Yuan, Haifeng and Fron, Eduard and Kim, Junghwan and Yang, Zhenyu and Voznyy, Oleksandr and Asta, Mark and Sargent, Edward H.},
abstractNote = {Efficient wide-bandgap perovskite solar cells (PSCs) enable high-efficiency tandem photovoltaics when combined with crystalline silicon and other low-bandgap absorbers. However, wide-bandgap PSCs today exhibit performance far inferior to that of sub-1.6-eV bandgap PSCs due to their tendency to form a high density of deep traps. Here, we show that healing the deep traps in wide-bandgap perovskites—in effect, increasing the defect tolerance via cation engineering—enables further performance improvements in PSCs. We achieve a stabilized power conversion efficiency of 20.7% for 1.65-eV bandgap PSCs by incorporating dipolar cations, with a high open-circuit voltage of 1.22 V and a fill factor exceeding 80%. We also obtain a stabilized efficiency of 19.1% for 1.74-eV bandgap PSCs with a high open-circuit voltage of 1.25 V. From density functional theory calculations, we find that the presence and reorientation of the dipolar cation in mixed cation–halide perovskites heals the defects that introduce deep trap states.},
doi = {10.1038/s41467-018-05531-8},
journal = {Nature Communications},
number = ,
volume = 9,
place = {United States},
year = {2018},
month = {8}
}

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