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Title: Constructive molecular configurations for surface-defect passivation of perovskite photovoltaics

Abstract

Surface trap-mediated nonradiative charge recombination is a major limit to achieving high-efficiency metal-halide perovskite photovoltaics. The ionic character of perovskite lattice has enabled molecular defect passivation approaches through interaction between functional groups and defects. However, a lack of in-depth understanding of how the molecular configuration influences the passivation effectiveness is a challenge to rational molecule design. In this work, the chemical environment of a functional group that is activated for defect passivation was systematically investigated with theophylline, caffeine, and theobromine. When N-H and C=O were in an optimal configuration in the molecule, hydrogen-bond formation between N-H and I (iodine) assisted the primary C=O binding with the antisite Pb (lead) defect to maximize surface-defect binding. A stabilized power conversion efficiency of 22.6% of photovoltaic device was demonstrated with theophylline treatment.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [4];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [5];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [6]; ORCiD logo [1]; ORCiD logo [7]
  1. Univ. of California, Los Angeles, CA (United States)
  2. Soochow Univ., Suzhou (China)
  3. Univ. of California, Los Angeles, CA (United States); Soochow Univ., Suzhou (China)
  4. Univ. of California, San Diego, La Jolla, CA (United States)
  5. Univ. of California, Berkeley, CA (United States)
  6. Marmara Univ., Istanbul (Turkey)
  7. Univ. of California, Los Angeles, CA (United States) ; Westlake Univ., Hangzhou (China)
Publication Date:
Research Org.:
Univ. of California, Los Angeles, CA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office; US Department of the Navy, Office of Naval Research (ONR); National Natural Science Foundation of China (NNSFC); Collaborative Innovation Center of Suzhou Nano Science and Technology; California Energy Commission; National Science Foundation (NSF)
OSTI Identifier:
1574274
Grant/Contract Number:  
EE0008751; EPC-16-050; ECCS-1542148
Resource Type:
Accepted Manuscript
Journal Name:
Science
Additional Journal Information:
Journal Volume: 366; Journal Issue: 6472; Journal ID: ISSN 0036-8075
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY

Citation Formats

Wang, Rui, Xue, Jingjing, Wang, Kai-Li, Wang, Zhao-Kui, Luo, Yanqi, Fenning, David, Xu, Guangwei, Nuryyeva, Selbi, Huang, Tianyi, Zhao, Yepin, Yang, Jonathan Lee, Zhu, Jiahui, Wang, Minhuan, Tan, Shaun, Yavuz, Ilhan, Houk, Kendall N., and Yang, Yang. Constructive molecular configurations for surface-defect passivation of perovskite photovoltaics. United States: N. p., 2019. Web. doi:10.1126/science.aay9698.
Wang, Rui, Xue, Jingjing, Wang, Kai-Li, Wang, Zhao-Kui, Luo, Yanqi, Fenning, David, Xu, Guangwei, Nuryyeva, Selbi, Huang, Tianyi, Zhao, Yepin, Yang, Jonathan Lee, Zhu, Jiahui, Wang, Minhuan, Tan, Shaun, Yavuz, Ilhan, Houk, Kendall N., & Yang, Yang. Constructive molecular configurations for surface-defect passivation of perovskite photovoltaics. United States. doi:https://doi.org/10.1126/science.aay9698
Wang, Rui, Xue, Jingjing, Wang, Kai-Li, Wang, Zhao-Kui, Luo, Yanqi, Fenning, David, Xu, Guangwei, Nuryyeva, Selbi, Huang, Tianyi, Zhao, Yepin, Yang, Jonathan Lee, Zhu, Jiahui, Wang, Minhuan, Tan, Shaun, Yavuz, Ilhan, Houk, Kendall N., and Yang, Yang. Fri . "Constructive molecular configurations for surface-defect passivation of perovskite photovoltaics". United States. doi:https://doi.org/10.1126/science.aay9698. https://www.osti.gov/servlets/purl/1574274.
@article{osti_1574274,
title = {Constructive molecular configurations for surface-defect passivation of perovskite photovoltaics},
author = {Wang, Rui and Xue, Jingjing and Wang, Kai-Li and Wang, Zhao-Kui and Luo, Yanqi and Fenning, David and Xu, Guangwei and Nuryyeva, Selbi and Huang, Tianyi and Zhao, Yepin and Yang, Jonathan Lee and Zhu, Jiahui and Wang, Minhuan and Tan, Shaun and Yavuz, Ilhan and Houk, Kendall N. and Yang, Yang},
abstractNote = {Surface trap-mediated nonradiative charge recombination is a major limit to achieving high-efficiency metal-halide perovskite photovoltaics. The ionic character of perovskite lattice has enabled molecular defect passivation approaches through interaction between functional groups and defects. However, a lack of in-depth understanding of how the molecular configuration influences the passivation effectiveness is a challenge to rational molecule design. In this work, the chemical environment of a functional group that is activated for defect passivation was systematically investigated with theophylline, caffeine, and theobromine. When N-H and C=O were in an optimal configuration in the molecule, hydrogen-bond formation between N-H and I (iodine) assisted the primary C=O binding with the antisite Pb (lead) defect to maximize surface-defect binding. A stabilized power conversion efficiency of 22.6% of photovoltaic device was demonstrated with theophylline treatment.},
doi = {10.1126/science.aay9698},
journal = {Science},
number = 6472,
volume = 366,
place = {United States},
year = {2019},
month = {12}
}

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