Correctly Assessing Defect Tolerance in Halide Perovskites

Zhang, Xie; Turiansky, Mark E.; Van de Walle, Chris G.

doi:10.1021/acs.jpcc.0c01324

Title: Correctly Assessing Defect Tolerance in Halide Perovskites

Abstract

The notion of “defect tolerance” has often been invoked to explain the excellent performance of halide perovskites in optoelectronic applications. However, this concept has not been rigorously defined or assessed. A common interpretation is that all of the energetically favorable intrinsic defects are shallow. On the basis of examples in the prototypical halide perovskite CsPbI₃, we show that this is not the case. The antisite defects Pb_I and I_Pb are energetically favorable, but also have levels deep in the band gap. Still, because of strong anharmonicity, they are not efficient nonradiative recombination centers. Here, our study demonstrates how to correctly evaluate the “defect tolerance” of halide perovskites.

Authors:

^[1]; Turiansky, Mark E. ^[1];

^[1]

Univ. of California, Santa Barbara, CA (United States)

Publication Date:: Tue Feb 25 00:00:00 EST 2020

Research Org.:: Univ. of California, Santa Barbara, CA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1601528

Grant/Contract Number:: SC0010689; AC02-05CH11231

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Physical Chemistry. C

Additional Journal Information:: Journal Volume: 124; Journal Issue: 11; Journal ID: ISSN 1932-7447

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Halide perovskites; Defect tolerance; Nonradiative recombination; First-principles calculations; Defects; Energy levels; Recombination; Potential energy; Perovskites

Citation Formats


                    Zhang, Xie, Turiansky, Mark E., and Van de Walle, Chris G. Correctly Assessing Defect Tolerance in Halide Perovskites.  United States: N. p., 2020. 
Web.  doi:10.1021/acs.jpcc.0c01324.

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                    Zhang, Xie, Turiansky, Mark E., & Van de Walle, Chris G. Correctly Assessing Defect Tolerance in Halide Perovskites.  United States.  https://doi.org/10.1021/acs.jpcc.0c01324

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                    Zhang, Xie, Turiansky, Mark E., and Van de Walle, Chris G. Tue .  
"Correctly Assessing Defect Tolerance in Halide Perovskites".  United States.  https://doi.org/10.1021/acs.jpcc.0c01324.  https://www.osti.gov/servlets/purl/1601528.

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@article{osti_1601528,

  title        = {Correctly Assessing Defect Tolerance in Halide Perovskites},

  author       = {Zhang, Xie and Turiansky, Mark E. and Van de Walle, Chris G.},

  abstractNote = {The notion of “defect tolerance” has often been invoked to explain the excellent performance of halide perovskites in optoelectronic applications. However, this concept has not been rigorously defined or assessed. A common interpretation is that all of the energetically favorable intrinsic defects are shallow. On the basis of examples in the prototypical halide perovskite CsPbI3, we show that this is not the case. The antisite defects PbI and IPb are energetically favorable, but also have levels deep in the band gap. Still, because of strong anharmonicity, they are not efficient nonradiative recombination centers. Here, our study demonstrates how to correctly evaluate the “defect tolerance” of halide perovskites.},

  doi          = {10.1021/acs.jpcc.0c01324},

  journal      = {Journal of Physical Chemistry. C},

  number       = 11,

  volume       = 124,

  place        = {United States},

  year         = {Tue Feb 25 00:00:00 EST 2020},

  month        = {Tue Feb 25 00:00:00 EST 2020}

}

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Title: Correctly Assessing Defect Tolerance in Halide Perovskites

Abstract

Citation Formats

Iodide management in formamidinium-lead-halide–based perovskite layers for efficient solar cells journal, June 2017

Methylammonium Chloride Induces Intermediate Phase Stabilization for Efficient Perovskite Solar Cells journal, September 2019

Efficient perovskite light-emitting diodes featuring nanometre-sized crystallites journal, January 2017

Defect Tolerance in Methylammonium Lead Triiodide Perovskite journal, July 2016

High Defect Tolerance in Lead Halide Perovskite CsPbBr 3 journal, January 2017

Tutorial: Defects in semiconductors—Combining experiment and theory journal, May 2016

Nonradiative capture and recombination by multiphonon emission in GaAs and GaP journal, January 1977

Unusual defect physics in CH 3 NH 3 PbI 3 perovskite solar cell absorber journal, February 2014

Density Functional Calculations of Native Defects in CH 3 NH 3 PbI 3 : Effects of Spin–Orbit Coupling and Self-Interaction Error journal, April 2015

Identification of Trap States in Perovskite Solar Cells journal, June 2015

Hole Trapping by Iodine Interstitial Defects Decreases Free Carrier Losses in Perovskite Solar Cells: A Time-Domain Ab Initio Study journal, May 2017

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal, October 1996

Projector augmented-wave method journal, December 1994

Special points for Brillouin-zone integrations journal, June 1976

Hybrid functionals based on a screened Coulomb potential journal, May 2003

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First-principles calculations for point defects in solids journal, March 2014

Fully Ab Initio Finite-Size Corrections for Charged-Defect Supercell Calculations journal, January 2009

First-principles theory of nonradiative carrier capture via multiphonon emission journal, August 2014

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Anharmonicity Extends Carrier Lifetimes in Lead Halide Perovskites at Elevated Temperatures journal, September 2019

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Methylammonium Chloride Induces Intermediate Phase Stabilization for Efficient Perovskite Solar Cells
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journal, July 2016

High Defect Tolerance in Lead Halide Perovskite CsPbBr ₃
journal, January 2017

Tutorial: Defects in semiconductors—Combining experiment and theory
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Nonradiative capture and recombination by multiphonon emission in GaAs and GaP
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Unusual defect physics in CH ₃ NH ₃ PbI ₃ perovskite solar cell absorber
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Density Functional Calculations of Native Defects in CH ₃ NH ₃ PbI ₃ : Effects of Spin–Orbit Coupling and Self-Interaction Error
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journal, December 1994

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journal, June 1976

Hybrid functionals based on a screened Coulomb potential
journal, May 2003

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