Giant Huang–Rhys Factor for Electron Capture by the Iodine Intersitial in Perovskite Solar Cells

Lucy Whalley; Puck van gerwen; Jarvist M. Frost; Sunghyun Kim; Samantha N. Hood; Aron Walsh

doi:https://arxiv.org/abs/2105.02097

Giant Huang–Rhys Factor for Electron Capture by the Iodine Intersitial in Perovskite Solar Cells

Lucy Whalley^*, Puck van gerwen, Jarvist M. Frost, Sunghyun Kim, Samantha N. Hood, Aron Walsh

^*Corresponding author for this work

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Abstract

Improvement in the optoelectronic performance of halide perovskite semiconductors requires the identification and suppression of nonradiative carrier trapping processes. The iodine interstitial has been established as a deep level defect and implicated as an active recombination center. We analyze the quantum mechanics of carrier trapping. Fast and irreversible electron capture by the neutral iodine interstitial is found. The effective Huang–Rhys factor exceeds 300, indicative of the strong electron–phonon coupling that is possible in soft semiconductors. The accepting phonon mode has a frequency of 53 cm–1 and has an associated electron capture coefficient of 1 × 10–10 cm3 s–1. The inverse participation ratio is used to quantify the localization of phonon modes associated with the transition. We infer that suppression of octahedral rotations is an important factor to enhance defect tolerance.

Original language	English
Pages (from-to)	9123-9128
Number of pages	6
Journal	Journal of the American Chemical Society
Volume	143
Issue number	24
Early online date	8 Jun 2021
DOIs	https://doi.org/https://arxiv.org/abs/2105.02097 https://doi.org/10.1021/jacs.1c03064
Publication status	Published - 23 Jun 2021

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https://arxiv.org/abs/2105.02097Licence: CC BY
10.1021/jacs.1c03064Licence: CC BY

2105.02097Accepted author manuscript, 1.87 MBLicence: CC BY
Final published versionFinal published version, 1.48 MBLicence: CC BY
Advance online versionFinal published version, 1.26 MBLicence: CC BY

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title = "Giant Huang–Rhys Factor for Electron Capture by the Iodine Intersitial in Perovskite Solar Cells",

abstract = "Improvement in the optoelectronic performance of halide perovskite semiconductors requires the identification and suppression of nonradiative carrier trapping processes. The iodine interstitial has been established as a deep level defect and implicated as an active recombination center. We analyze the quantum mechanics of carrier trapping. Fast and irreversible electron capture by the neutral iodine interstitial is found. The effective Huang–Rhys factor exceeds 300, indicative of the strong electron–phonon coupling that is possible in soft semiconductors. The accepting phonon mode has a frequency of 53 cm–1 and has an associated electron capture coefficient of 1 × 10–10 cm3 s–1. The inverse participation ratio is used to quantify the localization of phonon modes associated with the transition. We infer that suppression of octahedral rotations is an important factor to enhance defect tolerance.",

author = "Lucy Whalley and \{van gerwen\}, Puck and Frost, \{Jarvist M.\} and Sunghyun Kim and Hood, \{Samantha N.\} and Aron Walsh",

note = "Funding information: Calculations were performed on the Piz Daint supercomputer at the Swiss National Supercomputing Centre (CSCS) via the Partnership for Advanced Computing in Europe (PRACE) project pr51. Via our membership of the UK's HPC Materials Chemistry Consortium, which is funded by EPSRC (EP/L000202, EP/R029431), this work also used the ARCHER Supercomputing Service (http://www.archer.ac.uk). This work was supported by a National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT) (No. 2018R1C1B6008728) and the H2020 Programme under the project STARCELL (H2020-NMBP-03-2016-720907). J.M.F. is supported by a Royal Society University Research Fellowship (URF-R1-191292).",

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doi = "https://arxiv.org/abs/2105.02097",

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AU - Whalley, Lucy

AU - van gerwen, Puck

AU - Frost, Jarvist M.

AU - Kim, Sunghyun

AU - Hood, Samantha N.

AU - Walsh, Aron

N1 - Funding information: Calculations were performed on the Piz Daint supercomputer at the Swiss National Supercomputing Centre (CSCS) via the Partnership for Advanced Computing in Europe (PRACE) project pr51. Via our membership of the UK's HPC Materials Chemistry Consortium, which is funded by EPSRC (EP/L000202, EP/R029431), this work also used the ARCHER Supercomputing Service (http://www.archer.ac.uk). This work was supported by a National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT) (No. 2018R1C1B6008728) and the H2020 Programme under the project STARCELL (H2020-NMBP-03-2016-720907). J.M.F. is supported by a Royal Society University Research Fellowship (URF-R1-191292).

PY - 2021/6/23

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N2 - Improvement in the optoelectronic performance of halide perovskite semiconductors requires the identification and suppression of nonradiative carrier trapping processes. The iodine interstitial has been established as a deep level defect and implicated as an active recombination center. We analyze the quantum mechanics of carrier trapping. Fast and irreversible electron capture by the neutral iodine interstitial is found. The effective Huang–Rhys factor exceeds 300, indicative of the strong electron–phonon coupling that is possible in soft semiconductors. The accepting phonon mode has a frequency of 53 cm–1 and has an associated electron capture coefficient of 1 × 10–10 cm3 s–1. The inverse participation ratio is used to quantify the localization of phonon modes associated with the transition. We infer that suppression of octahedral rotations is an important factor to enhance defect tolerance.

AB - Improvement in the optoelectronic performance of halide perovskite semiconductors requires the identification and suppression of nonradiative carrier trapping processes. The iodine interstitial has been established as a deep level defect and implicated as an active recombination center. We analyze the quantum mechanics of carrier trapping. Fast and irreversible electron capture by the neutral iodine interstitial is found. The effective Huang–Rhys factor exceeds 300, indicative of the strong electron–phonon coupling that is possible in soft semiconductors. The accepting phonon mode has a frequency of 53 cm–1 and has an associated electron capture coefficient of 1 × 10–10 cm3 s–1. The inverse participation ratio is used to quantify the localization of phonon modes associated with the transition. We infer that suppression of octahedral rotations is an important factor to enhance defect tolerance.

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JO - Journal of the American Chemical Society

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IS - 24

ER -

Giant Huang–Rhys Factor for Electron Capture by the Iodine Intersitial in Perovskite Solar Cells

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