Pressure-Induced Bandgap Optimization in Lead-Based Perovskites with Prolonged Carrier Lifetime and Ambient Retainability

Gang Liu; Lingping Kong; Jue Gong; Wenge Yang; Ho Kwang Mao; Qingyang Hu; Zhenxian Liu; Richard D. Schaller; Dongzhou Zhang; Tao Xu

doi:10.1002/adfm.201604208

Pressure-Induced Bandgap Optimization in Lead-Based Perovskites with Prolonged Carrier Lifetime and Ambient Retainability

Gang Liu^*, Lingping Kong, Jue Gong, Wenge Yang, Ho Kwang Mao, Qingyang Hu, Zhenxian Liu, Richard D. Schaller, Dongzhou Zhang, Tao Xu

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

200 Scopus citations

Abstract

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, for 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.

Original language	English (US)
Article number	1604208
Journal	Advanced Functional Materials
Volume	27
Issue number	3
DOIs	https://doi.org/10.1002/adfm.201604208
State	Published - Jan 19 2017

Funding

This project was supported by NSAF (Grant No. U1530402) and National Science Foundation (Grant No. CBET-1150617). High pressure powder structure characterizations were performed at beamline 16-BM-D at HPCAT, APS, ANL. HPCAT operations were supported by DOE-NNSA under Award No. DE-NA0001974 and DOE-BES under Award No. DE-FG02- 99ER45775, with partial instrumentation funding by the National Science Foundation (NSF). Part of this work was also performed at the Center for Nanoscale Materials (CNM), ANL, and the Infrared Lab of the National Synchrotron Light Source (NSLS II), Brookhaven National Laboratory (BNL). The use of APS and CNM facilities was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (DE-AC02-06CH11357). The Infrared Lab was supported by National Science Foundation (EAR 1606856, COMPRES) and DOE/NNSA (DE-NA-0002006, CDAC). The authors also thank Dr. Victor V. Ryzhov for his experimental support and Dr. H. Sheng for useful discussions. The computational work was conducted on the SR10000-K1/52 supercomputing facilities of the Institute for Materials Research, Tohoku University.

Keywords

bandgap
carrier lifetime
high pressure
perovskite

ASJC Scopus subject areas

General Chemistry
General Materials Science
Condensed Matter Physics

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This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1002/adfm.201604208

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title = "Pressure-Induced Bandgap Optimization in Lead-Based Perovskites with Prolonged Carrier Lifetime and Ambient Retainability",

abstract = "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, for 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.",

keywords = "bandgap, carrier lifetime, high pressure, perovskite",

author = "Gang Liu and Lingping Kong and Jue Gong and Wenge Yang and Mao, \{Ho Kwang\} and Qingyang Hu and Zhenxian Liu and Schaller, \{Richard D.\} and Dongzhou Zhang and Tao Xu",

note = "Funding Information: This project was supported by NSAF (Grant No. U1530402) and National Science Foundation (Grant No. CBET-1150617). High pressure powder structure characterizations were performed at beamline 16-BM-D at HPCAT, APS, ANL. HPCAT operations were supported by DOE-NNSA under Award No. DE-NA0001974 and DOE-BES under Award No. DE-FG02- 99ER45775, with partial instrumentation funding by the National Science Foundation (NSF). Part of this work was also performed at the Center for Nanoscale Materials (CNM), ANL, and the Infrared Lab of the National Synchrotron Light Source (NSLS II), Brookhaven National Laboratory (BNL). The use of APS and CNM facilities was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (DE-AC02-06CH11357). The Infrared Lab was supported by National Science Foundation (EAR 1606856, COMPRES) and DOE/NNSA (DE-NA-0002006, CDAC). The authors also thank Dr. Victor V. Ryzhov for his experimental support and Dr. H. Sheng for useful discussions. The computational work was conducted on the SR10000-K1/52 supercomputing facilities of the Institute for Materials Research, Tohoku University. Publisher Copyright: {\textcopyright} 2016 WILEY-VCH Verlag GmbH \& Co. KGaA, Weinheim",

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AU - Gong, Jue

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AU - Mao, Ho Kwang

AU - Hu, Qingyang

AU - Liu, Zhenxian

AU - Schaller, Richard D.

AU - Zhang, Dongzhou

AU - Xu, Tao

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N2 - 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, for 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.

AB - 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, for 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.

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Pressure-Induced Bandgap Optimization in Lead-Based Perovskites with Prolonged Carrier Lifetime and Ambient Retainability

Abstract

Funding

Keywords

ASJC Scopus subject areas

UN SDGs

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