Constructive molecular configurations for surface-defect passivation of perovskite photovoltaics
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. Howeve...
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| Published in | Science (American Association for the Advancement of Science) Vol. 366; no. 6472; pp. 1509 - 1513 |
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| Main Authors | , , , , , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
American Association for the Advancement of Science
20.12.2019
The American Association for the Advancement of Science AAAS |
| Subjects | |
| Online Access | Get full text |
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| 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. Here, 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. |
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| AbstractList | 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. Unproductive charge recombination at surface defects can limit the efficiency of hybrid perovskite solar cells, but these defects can be passivated by the binding of small molecules. Wang et al. studied three such small molecules—theophylline, caffeine, and theobromine—that bear both carbonyl and amino groups. For theophylline, hydrogen bonding of the amino hydrogen to surface iodide optimized the carbonyl interaction with a lead antisite defect and improved the efficiency of a perovskite cell from 21 to 22.6%. Science , this issue p. 1509 Molecules that bring N-H and C=O groups into an optimal configuration passivate antisite lead defects on perovskite surfaces. 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. Here, 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. 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. Here, 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. Optimizing surface passivationUnproductive charge recombination at surface defects can limit the efficiency of hybrid perovskite solar cells, but these defects can be passivated by the binding of small molecules. Wang et al. studied three such small molecules—theophylline, caffeine, and theobromine—that bear both carbonyl and amino groups. For theophylline, hydrogen bonding of the amino hydrogen to surface iodide optimized the carbonyl interaction with a lead antisite defect and improved the efficiency of a perovskite cell from 21 to 22.6%.Science, this issue p. 1509Surface 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. Here, 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. 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. Here, 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.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. Here, 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. |
| Author | Huang, Tianyi Lee Yang, Jonathan Houk, Kendall N. Tan, Shaun Zhao, Yepin Wang, Minhuan Nuryyeva, Selbi Yang, Yang Wang, Rui Zhu, Jiahui Wang, Zhao-Kui Wang, Kai-Li Luo, Yanqi Yavuz, Ilhan Xu, Guangwei Xue, Jingjing Fenning, David |
| Author_xml | – sequence: 1 givenname: Rui surname: Wang fullname: Wang, Rui – sequence: 2 givenname: Jingjing surname: Xue fullname: Xue, Jingjing – sequence: 3 givenname: Kai-Li surname: Wang fullname: Wang, Kai-Li – sequence: 4 givenname: Zhao-Kui surname: Wang fullname: Wang, Zhao-Kui – sequence: 5 givenname: Yanqi surname: Luo fullname: Luo, Yanqi – sequence: 6 givenname: David surname: Fenning fullname: Fenning, David – sequence: 7 givenname: Guangwei surname: Xu fullname: Xu, Guangwei – sequence: 8 givenname: Selbi surname: Nuryyeva fullname: Nuryyeva, Selbi – sequence: 9 givenname: Tianyi surname: Huang fullname: Huang, Tianyi – sequence: 10 givenname: Yepin surname: Zhao fullname: Zhao, Yepin – sequence: 11 givenname: Jonathan surname: Lee Yang fullname: Lee Yang, Jonathan – sequence: 12 givenname: Jiahui surname: Zhu fullname: Zhu, Jiahui – sequence: 13 givenname: Minhuan surname: Wang fullname: Wang, Minhuan – sequence: 14 givenname: Shaun surname: Tan fullname: Tan, Shaun – sequence: 15 givenname: Ilhan surname: Yavuz fullname: Yavuz, Ilhan – sequence: 16 givenname: Kendall N. surname: Houk fullname: Houk, Kendall N. – sequence: 17 givenname: Yang surname: Yang fullname: Yang, Yang |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/31857483$$D View this record in MEDLINE/PubMed https://www.osti.gov/servlets/purl/1574274$$D View this record in Osti.gov |
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| ContentType | Journal Article |
| Copyright | Copyright © 2019 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Copyright © 2019 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works |
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| CorporateAuthor | Univ. of California, Los Angeles, CA (United States) |
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| DOI | 10.1126/science.aay9698 |
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| Snippet | Surface trap–mediated nonradiative charge recombination is a major limit to achieving high-efficiency metal-halide perovskite photovoltaics. The ionic... Unproductive charge recombination at surface defects can limit the efficiency of hybrid perovskite solar cells, but these defects can be passivated by the... Surface trap-mediated nonradiative charge recombination is a major limit to achieving high-efficiency metal-halide perovskite photovoltaics. The ionic... Optimizing surface passivationUnproductive charge recombination at surface defects can limit the efficiency of hybrid perovskite solar cells, but these defects... |
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| SubjectTerms | Amino groups Binding Caffeine Carbonyl compounds Carbonyls Configurations Defects Efficiency Energy conversion efficiency Functional groups Hydrogen Hydrogen bonding Hydrogen bonds Iodides Iodine Lead Metal halides Optimization Organic chemistry Passivity Perovskites Photovoltaic cells Photovoltaics Recombination Solar cells SOLAR ENERGY Surface charge Surface defects Theophylline |
| Title | Constructive molecular configurations for surface-defect passivation of perovskite photovoltaics |
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