Origin of long lifetime of band-edge charge carriers in organic–inorganic lead iodide perovskites

Tianran Chen; Wei Liang Chen; Benjamin J. Foley; Jooseop Lee; Jacob P.C. Ruff; J. Y.Peter Ko; Craig M. Brown; Leland W. Harriger; Depei Zhang; Changwon Park; Mina Yoon; Yu Ming Chang; Joshua J. Choi; Seung Hun Lee

doi:10.1073/pnas.1704421114

Origin of long lifetime of band-edge charge carriers in organic–inorganic lead iodide perovskites

Tianran Chen, Wei Liang Chen, Benjamin J. Foley, Jooseop Lee, Jacob P.C. Ruff, J. Y.Peter Ko, Craig M. Brown, Leland W. Harriger, Depei Zhang, Changwon Park, Mina Yoon, Yu Ming Chang, Joshua J. Choi, Seung Hun Lee

Microstructural Evolution Modeling

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

147 Scopus citations

Abstract

Long carrier lifetime is what makes hybrid organic–inorganic perovskites high-performance photovoltaic materials. Several microscopic mechanisms behind the unusually long carrier lifetime have been proposed, such as formation of large polarons, Rashba effect, ferroelectric domains, and photon recycling. Here, we show that the screening of band-edge charge carriers by rotation of organic cation molecules can be a major contribution to the prolonged carrier lifetime. Our results reveal that the band-edge carrier lifetime increases when the system enters from a phase with lower rotational entropy to another phase with higher entropy. These results imply that the recombination of the photoexcited electrons and holes is suppressed by the screening, leading to the formation of polarons and thereby extending the lifetime. Thus, searching for organic–inorganic perovskites with high rotational entropy over a wide range of temperature may be a key to achieve superior solar cell performance.

Original language	English
Pages (from-to)	7519-7524
Number of pages	6
Journal	Proceedings of the National Academy of Sciences of the United States of America
Volume	114
Issue number	29
DOIs	https://doi.org/10.1073/pnas.1704421114
State	Published - Jul 18 2017

Funding

The work at the University of Virginia is supported by the US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, under Award DE-SC0016144. The work at National Taiwan University is supported by Ministry of Science and Technology of Taiwan (MOST) Grant 105-2119-M-002-046-MY3. Computational work was performed by utilizing the computational facilities at the Center for Nanophase Materials Sciences, a US DOE Office of Science user facility. This research used resources of the National Energy Research Scientific Computing Center, which is supported by the Office of Science of the US DOE (Contract DE-AC02-05CH11231). Cornell High Energy Synchrotron Source is supported by the NSF and NIH/National Institute of General Medical Sciences via NSF Award DMR-1332208.

Funders	Funder number
DOE Office of Science
NIH/National Institute of General Medical Sciences	DMR-1332208
Office of Basic Energy Sciences	DE-SC0016144
DOE Office of Science	DE-AC02-05CH11231
US Department of Energy
National Science Foundation
U.S. Department of Energy
Office of Science
University of Virginia
Ministry of Science and Technology, Taiwan	105-2119-M-002-046-MY3

Keywords

Carrier lifetime
Organic–inorganic hybrid perovskite
Photoluminescence
Polaron

UN SDGs

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

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10.1073/pnas.1704421114

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Chen, T., Chen, W. L., Foley, B. J., Lee, J., Ruff, J. P. C., Ko, J. Y. P., Brown, C. M., Harriger, L. W., Zhang, D., Park, C., Yoon, M., Chang, Y. M., Choi, J. J., & Lee, S. H. (2017). Origin of long lifetime of band-edge charge carriers in organic–inorganic lead iodide perovskites. Proceedings of the National Academy of Sciences of the United States of America, 114(29), 7519-7524. https://doi.org/10.1073/pnas.1704421114

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abstract = "Long carrier lifetime is what makes hybrid organic–inorganic perovskites high-performance photovoltaic materials. Several microscopic mechanisms behind the unusually long carrier lifetime have been proposed, such as formation of large polarons, Rashba effect, ferroelectric domains, and photon recycling. Here, we show that the screening of band-edge charge carriers by rotation of organic cation molecules can be a major contribution to the prolonged carrier lifetime. Our results reveal that the band-edge carrier lifetime increases when the system enters from a phase with lower rotational entropy to another phase with higher entropy. These results imply that the recombination of the photoexcited electrons and holes is suppressed by the screening, leading to the formation of polarons and thereby extending the lifetime. Thus, searching for organic–inorganic perovskites with high rotational entropy over a wide range of temperature may be a key to achieve superior solar cell performance.",

keywords = "Carrier lifetime, Organic–inorganic hybrid perovskite, Photoluminescence, Polaron",

author = "Tianran Chen and Chen, {Wei Liang} and Foley, {Benjamin J.} and Jooseop Lee and Ruff, {Jacob P.C.} and Ko, {J. Y.Peter} and Brown, {Craig M.} and Harriger, {Leland W.} and Depei Zhang and Changwon Park and Mina Yoon and Chang, {Yu Ming} and Choi, {Joshua J.} and Lee, {Seung Hun}",

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Chen, T, Chen, WL, Foley, BJ, Lee, J, Ruff, JPC, Ko, JYP, Brown, CM, Harriger, LW, Zhang, D, Park, C, Yoon, M, Chang, YM, Choi, JJ & Lee, SH 2017, 'Origin of long lifetime of band-edge charge carriers in organic–inorganic lead iodide perovskites', Proceedings of the National Academy of Sciences of the United States of America, vol. 114, no. 29, pp. 7519-7524. https://doi.org/10.1073/pnas.1704421114

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AU - Chen, Tianran

AU - Chen, Wei Liang

AU - Foley, Benjamin J.

AU - Lee, Jooseop

AU - Ruff, Jacob P.C.

AU - Ko, J. Y.Peter

AU - Brown, Craig M.

AU - Harriger, Leland W.

AU - Zhang, Depei

AU - Park, Changwon

AU - Yoon, Mina

AU - Chang, Yu Ming

AU - Choi, Joshua J.

AU - Lee, Seung Hun

PY - 2017/7/18

Y1 - 2017/7/18

N2 - Long carrier lifetime is what makes hybrid organic–inorganic perovskites high-performance photovoltaic materials. Several microscopic mechanisms behind the unusually long carrier lifetime have been proposed, such as formation of large polarons, Rashba effect, ferroelectric domains, and photon recycling. Here, we show that the screening of band-edge charge carriers by rotation of organic cation molecules can be a major contribution to the prolonged carrier lifetime. Our results reveal that the band-edge carrier lifetime increases when the system enters from a phase with lower rotational entropy to another phase with higher entropy. These results imply that the recombination of the photoexcited electrons and holes is suppressed by the screening, leading to the formation of polarons and thereby extending the lifetime. Thus, searching for organic–inorganic perovskites with high rotational entropy over a wide range of temperature may be a key to achieve superior solar cell performance.

AB - Long carrier lifetime is what makes hybrid organic–inorganic perovskites high-performance photovoltaic materials. Several microscopic mechanisms behind the unusually long carrier lifetime have been proposed, such as formation of large polarons, Rashba effect, ferroelectric domains, and photon recycling. Here, we show that the screening of band-edge charge carriers by rotation of organic cation molecules can be a major contribution to the prolonged carrier lifetime. Our results reveal that the band-edge carrier lifetime increases when the system enters from a phase with lower rotational entropy to another phase with higher entropy. These results imply that the recombination of the photoexcited electrons and holes is suppressed by the screening, leading to the formation of polarons and thereby extending the lifetime. Thus, searching for organic–inorganic perovskites with high rotational entropy over a wide range of temperature may be a key to achieve superior solar cell performance.

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Origin of long lifetime of band-edge charge carriers in organic–inorganic lead iodide perovskites

Abstract

Funding

Keywords

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