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Research Article

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, and Seung-Hun Lee
  1. aDepartment of Physics, University of Virginia, Charlottesville, VA 22904;
  2. bCenter for Condensed Matter Sciences, National Taiwan University, Taipei 10617, Taiwan;
  3. cDepartment of Chemical Engineering, University of Virginia, Charlottesville, VA 22904;
  4. dCornell High Energy Synchrotron Source, Cornell University, Ithaca, NY 14853;
  5. eNIST Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, MD 20899;
  6. fCenter for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN 37831

See allHide authors and affiliations

PNAS first published July 3, 2017; https://doi.org/10.1073/pnas.1704421114
Tianran Chen
aDepartment of Physics, University of Virginia, Charlottesville, VA 22904;
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Wei-Liang Chen
bCenter for Condensed Matter Sciences, National Taiwan University, Taipei 10617, Taiwan;
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Benjamin J. Foley
cDepartment of Chemical Engineering, University of Virginia, Charlottesville, VA 22904;
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Jooseop Lee
dCornell High Energy Synchrotron Source, Cornell University, Ithaca, NY 14853;
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Jacob P. C. Ruff
dCornell High Energy Synchrotron Source, Cornell University, Ithaca, NY 14853;
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J. Y. Peter Ko
dCornell High Energy Synchrotron Source, Cornell University, Ithaca, NY 14853;
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Craig M. Brown
eNIST Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, MD 20899;
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Leland W. Harriger
eNIST Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, MD 20899;
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Depei Zhang
aDepartment of Physics, University of Virginia, Charlottesville, VA 22904;
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Changwon Park
fCenter for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN 37831
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Mina Yoon
fCenter for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN 37831
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Yu-Ming Chang
bCenter for Condensed Matter Sciences, National Taiwan University, Taipei 10617, Taiwan;
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Joshua J. Choi
cDepartment of Chemical Engineering, University of Virginia, Charlottesville, VA 22904;
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  • For correspondence: shlee@virginia.edu jjc6z@virginia.edu
Seung-Hun Lee
aDepartment of Physics, University of Virginia, Charlottesville, VA 22904;
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  • For correspondence: shlee@virginia.edu jjc6z@virginia.edu
  1. Edited by Peidong Yang, University of California, Berkeley, CA, and approved May 26, 2017 (received for review March 16, 2017)

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Significance

Hybrid organic–inorganic perovskites (HOIPs) are among the most promising materials for next-generation solar cells that combine high efficiency and low cost. The record efficiency of HOIP-based solar cells has reached above 22%, which is comparable to that of silicon solar cells. HOIP solar cells can be manufactured using simple solution processing methods that can be drastically cheaper than the current commercial solar cell technologies. Despite the progress so far, the microscopic mechanism for the high solar cell efficiency in HOIPs is yet to be understood. Our study shows that rotation of organic molecules in HOIPs extends the lifetime of photoexcited charge carriers, leading to the high efficiency. This insight can guide the progress toward improved solar cell performance.

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.

  • organic–inorganic hybrid perovskite
  • carrier lifetime
  • photoluminescence
  • polaron

Footnotes

  • ↵1T.C. and W.-L.C. contributed equally to this work.

  • ↵2To whom correspondence may be addressed. Email: shlee{at}virginia.edu or jjc6z{at}virginia.edu.
  • Author contributions: S.-H.L. designed research; T.C., W.-L.C., B.J.F., J.L., J.P.C.R., J.Y.P.K., C.M.B., L.W.H., D.Z., C.P., M.Y., Y.-M.C., J.J.C., and S.-H.L. performed research; T.C. and W.-L.C. analyzed data; and J.J.C. and S.-H.L. wrote the paper.

  • The authors declare no conflict of interest.

  • This article is a PNAS Direct Submission.

  • This article contains supporting information online at www.pnas.org/lookup/suppl/doi:10.1073/pnas.1704421114/-/DCSupplemental.

Freely available online through the PNAS open access option.

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Origin of long lifetime of charge carriers in HOIP
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
Proceedings of the National Academy of Sciences Jul 2017, 201704421; DOI: 10.1073/pnas.1704421114

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Origin of long lifetime of charge carriers in HOIP
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
Proceedings of the National Academy of Sciences Jul 2017, 201704421; DOI: 10.1073/pnas.1704421114
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    • Abstract
    • Temperature-History Dependent PL Spectra of HC(NH2)2PbI3 and CH3NH3PbI3
    • Structural Phase Transitions in HC(NH2)2PbI3 and CH3NH3PbI3
    • First-Principles Electronic Structures of HC(NH2)2PbI3 and CH3NH3PbI3
    • TRPL of HC(NH2)2PbI3 and CH3NH3PbI3
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