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Title: Simultaneous band-gap narrowing and carrier-lifetime prolongation of organic–inorganic trihalide perovskites

Authors:
; ; ; ; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1354526
Report Number(s):
BNL-113043-2016-JA
Journal ID: ISSN 0027-8424
DOE Contract Number:
SC00112704
Resource Type:
Journal Article
Resource Relation:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America; Journal Volume: 113; Journal Issue: 32
Country of Publication:
United States
Language:
English

Citation Formats

Kong, Lingping, Liu, Gang, Gong, Jue, Hu, Qingyang, Schaller, Richard D., Dera, Przemyslaw, Zhang, Dongzhou, Liu, Zhenxian, Yang, Wenge, Zhu, Kai, Tang, Yuzhao, Wang, Chuanyi, Wei, Su-Huai, Xu, Tao, and Mao, Ho-kwang. Simultaneous band-gap narrowing and carrier-lifetime prolongation of organic–inorganic trihalide perovskites. United States: N. p., 2016. Web. doi:10.1073/pnas.1609030113.
Kong, Lingping, Liu, Gang, Gong, Jue, Hu, Qingyang, Schaller, Richard D., Dera, Przemyslaw, Zhang, Dongzhou, Liu, Zhenxian, Yang, Wenge, Zhu, Kai, Tang, Yuzhao, Wang, Chuanyi, Wei, Su-Huai, Xu, Tao, & Mao, Ho-kwang. Simultaneous band-gap narrowing and carrier-lifetime prolongation of organic–inorganic trihalide perovskites. United States. doi:10.1073/pnas.1609030113.
Kong, Lingping, Liu, Gang, Gong, Jue, Hu, Qingyang, Schaller, Richard D., Dera, Przemyslaw, Zhang, Dongzhou, Liu, Zhenxian, Yang, Wenge, Zhu, Kai, Tang, Yuzhao, Wang, Chuanyi, Wei, Su-Huai, Xu, Tao, and Mao, Ho-kwang. 2016. "Simultaneous band-gap narrowing and carrier-lifetime prolongation of organic–inorganic trihalide perovskites". United States. doi:10.1073/pnas.1609030113.
@article{osti_1354526,
title = {Simultaneous band-gap narrowing and carrier-lifetime prolongation of organic–inorganic trihalide perovskites},
author = {Kong, Lingping and Liu, Gang and Gong, Jue and Hu, Qingyang and Schaller, Richard D. and Dera, Przemyslaw and Zhang, Dongzhou and Liu, Zhenxian and Yang, Wenge and Zhu, Kai and Tang, Yuzhao and Wang, Chuanyi and Wei, Su-Huai and Xu, Tao and Mao, Ho-kwang},
abstractNote = {},
doi = {10.1073/pnas.1609030113},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 32,
volume = 113,
place = {United States},
year = 2016,
month = 7
}
  • The organic-inorganic hybrid lead trihalide perovskites have been emerging as the most attractive photovoltaic materials. As regulated by Shockley-Queisser theory, a formidable materials science challenge for improvement to the next level requires further band-gap narrowing for broader absorption in solar spectrum, while retaining or even synergistically prolonging the carrier lifetime, a critical factor responsible for attaining the near-band-gap photovoltage. Herein, by applying controllable hydrostatic pressure, we have achieved unprecedented simultaneous enhancement in both band-gap narrowing and carrier-lifetime prolongation (up to 70% to -100% increase) under mild pressures at -0.3 GPa. The pressure-induced modulation on pure hybrid perovskites without introducing anymore » adverse chemical or thermal effect clearly demonstrates the importance of band edges on the photon-electron interaction and maps a pioneering route toward a further increase in their photovoltaic performance.« less
  • Organic-inorganic perovskite solar cells have attracted tremendous attention because of their remarkably high power conversion efficiencies. To further improve device performance, it is imperative to obtain fundamental understandings on the photo-response and long-term stability down to the microscopic level. Here, we report the quantitative nanoscale photoconductivity imaging on two methylammonium lead triiodide thin films with different efficiencies by light-stimulated microwave impedance microscopy. The microwave signals are largely uniform across grains and grain boundaries, suggesting that microstructures do not lead to strong spatial variations of the intrinsic photo-response. In contrast, the measured photoconductivity and lifetime are strongly affected by bulk propertiesmore » such as the sample crystallinity. As visualized by the spatial evolution of local photoconductivity, the degradation process begins with the disintegration of grains rather than nucleation and propagation from visible boundaries between grains. In conclusion, our findings provide insights to improve the electro-optical properties of perovskite thin films towards large-scale commercialization.« less
  • Bond length and bond angle exhibited by valence electrons is essential to the core of chemistry. Using lead-based organic–inorganic perovskite compounds as an exploratory platform, it is demonstrated that the modulation of valence electrons by compression can lead to discovery of new properties of known compounds. Yet, despite its unprecedented progress, further efficiency boost of lead-based organic–inorganic perovskite solar cells is hampered by their wider bandgap than the optimum value according to the Shockley–Queisser limit. By modulating the valence electron wavefunction with modest hydraulic pressure up to 2.1 GPa, the optimized bandgap for single-junction solar cells in lead-based perovskites, formore » the first time, is achieved by narrowing the bandgap of formamidinium lead triiodide (HC(NH2)2PbI3) from 1.489 to 1.337 eV. Strikingly, such bandgap narrowing is partially retained after the release of pressure to ambient, and the bandgap narrowing is also accompanied with double-prolonged carrier lifetime. With First-principles simulation, this work opens a new dimension in basic chemical understanding of structural photonics and electronics and paves an alternative pathway toward better photovoltaic materials-by-design.« less
  • Bond length and bond angle exhibited by valence electrons is essential to the core of chemistry. Using lead-based organic–inorganic perovskite compounds as an exploratory platform, it is demonstrated that the modulation of valence electrons by compression can lead to discovery of new properties of known compounds. Yet, despite its unprecedented progress, further efficiency boost of lead-based organic–inorganic perovskite solar cells is hampered by their wider bandgap than the optimum value according to the Shockley–Queisser limit. By modulating the valence electron wavefunction with modest hydraulic pressure up to 2.1 GPa, the optimized bandgap for single-junction solar cells in lead-based perovskites, formore » the first time, is achieved by narrowing the bandgap of formamidinium lead triiodide (HC(NH 2) 2PbI 3) from 1.489 to 1.337 eV. Strikingly, such bandgap narrowing is partially retained after the release of pressure to ambient, and the bandgap narrowing is also accompanied with double-prolonged carrier lifetime. With First-principles simulation, this work opens a new dimension in basic chemical understanding of structural photonics and electronics and paves an alternative pathway toward better photovoltaic materials-by-design.« less