Inhomogeneous Defect Distribution in Mixed-Polytype Metal Halide Perovskites

Young Won Woo; Zhenzhu Li; Young Kwang Jung; Ji Sang Park; Aron Walsh

doi:10.1021/acsenergylett.2c02306

Inhomogeneous Defect Distribution in Mixed-Polytype Metal Halide Perovskites

Young Won Woo, Zhenzhu Li, Young Kwang Jung, Ji Sang Park, Aron Walsh

Department of Materials Science and Engineering

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

1 Citation (Scopus)

Abstract

The competition between corner-, edge-, and face-sharing octahedral networks is a cause of phase inhomogeneity in metal halide perovskite thin-films. Here we probe the charged iodine vacancy distribution and transport at the junction between cubic and hexagonal polytypes of CsPbI₃ from first-principles materials modeling. We predict a lower defect formation energy in the face-sharing regions, which correlates with a longer Pb-I bond length and causes a million-fold increase in local defect concentration. These defects are predicted to be more mobile in the face-sharing regions with a reduced activation energy for vacancy-mediated diffusion. We conclude that hexagonal phase inclusions or interfaces will act as defect sinks that could influence carrier dynamics in perovskite-based solar cells and electrical devices.

Original language	English
Pages (from-to)	356-360
Number of pages	5
Journal	ACS Energy Letters
Volume	8
Issue number	1
DOIs	https://doi.org/10.1021/acsenergylett.2c02306
Publication status	Published - 2023 Jan 13

Bibliographical note

Funding Information:
This research was supported by a grant of the Korea Health Technology R&D Project through the Korea Health Industry Development Institute (KHIDI), funded by the Ministry of Health & Welfare, Republic of Korea (grant number: HI19C1344). Computational resources have been provided by the KISTI Supercomputing Center (KSC-2021-CRE-0510). We are also grateful to the UK Materials and Molecular Modelling Hub for computational resources, which is partially funded by EPSRC (EP/P020194/1 and EP/T022213/1).

Publisher Copyright:
© 2022 The Authors. Published by American Chemical Society.

All Science Journal Classification (ASJC) codes

Chemistry (miscellaneous)
Renewable Energy, Sustainability and the Environment
Fuel Technology
Energy Engineering and Power Technology
Materials Chemistry

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10.1021/acsenergylett.2c02306

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title = "Inhomogeneous Defect Distribution in Mixed-Polytype Metal Halide Perovskites",

abstract = "The competition between corner-, edge-, and face-sharing octahedral networks is a cause of phase inhomogeneity in metal halide perovskite thin-films. Here we probe the charged iodine vacancy distribution and transport at the junction between cubic and hexagonal polytypes of CsPbI3 from first-principles materials modeling. We predict a lower defect formation energy in the face-sharing regions, which correlates with a longer Pb-I bond length and causes a million-fold increase in local defect concentration. These defects are predicted to be more mobile in the face-sharing regions with a reduced activation energy for vacancy-mediated diffusion. We conclude that hexagonal phase inclusions or interfaces will act as defect sinks that could influence carrier dynamics in perovskite-based solar cells and electrical devices.",

author = "Woo, {Young Won} and Zhenzhu Li and Jung, {Young Kwang} and Park, {Ji Sang} and Aron Walsh",

note = "Funding Information: This research was supported by a grant of the Korea Health Technology R&D Project through the Korea Health Industry Development Institute (KHIDI), funded by the Ministry of Health & Welfare, Republic of Korea (grant number: HI19C1344). Computational resources have been provided by the KISTI Supercomputing Center (KSC-2021-CRE-0510). We are also grateful to the UK Materials and Molecular Modelling Hub for computational resources, which is partially funded by EPSRC (EP/P020194/1 and EP/T022213/1). Publisher Copyright: {\textcopyright} 2022 The Authors. Published by American Chemical Society.",

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doi = "10.1021/acsenergylett.2c02306",

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AU - Woo, Young Won

AU - Li, Zhenzhu

AU - Jung, Young Kwang

AU - Park, Ji Sang

AU - Walsh, Aron

N1 - Funding Information: This research was supported by a grant of the Korea Health Technology R&D Project through the Korea Health Industry Development Institute (KHIDI), funded by the Ministry of Health & Welfare, Republic of Korea (grant number: HI19C1344). Computational resources have been provided by the KISTI Supercomputing Center (KSC-2021-CRE-0510). We are also grateful to the UK Materials and Molecular Modelling Hub for computational resources, which is partially funded by EPSRC (EP/P020194/1 and EP/T022213/1). Publisher Copyright: © 2022 The Authors. Published by American Chemical Society.

PY - 2023/1/13

Y1 - 2023/1/13

N2 - The competition between corner-, edge-, and face-sharing octahedral networks is a cause of phase inhomogeneity in metal halide perovskite thin-films. Here we probe the charged iodine vacancy distribution and transport at the junction between cubic and hexagonal polytypes of CsPbI3 from first-principles materials modeling. We predict a lower defect formation energy in the face-sharing regions, which correlates with a longer Pb-I bond length and causes a million-fold increase in local defect concentration. These defects are predicted to be more mobile in the face-sharing regions with a reduced activation energy for vacancy-mediated diffusion. We conclude that hexagonal phase inclusions or interfaces will act as defect sinks that could influence carrier dynamics in perovskite-based solar cells and electrical devices.

AB - The competition between corner-, edge-, and face-sharing octahedral networks is a cause of phase inhomogeneity in metal halide perovskite thin-films. Here we probe the charged iodine vacancy distribution and transport at the junction between cubic and hexagonal polytypes of CsPbI3 from first-principles materials modeling. We predict a lower defect formation energy in the face-sharing regions, which correlates with a longer Pb-I bond length and causes a million-fold increase in local defect concentration. These defects are predicted to be more mobile in the face-sharing regions with a reduced activation energy for vacancy-mediated diffusion. We conclude that hexagonal phase inclusions or interfaces will act as defect sinks that could influence carrier dynamics in perovskite-based solar cells and electrical devices.

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Inhomogeneous Defect Distribution in Mixed-Polytype Metal Halide Perovskites

Abstract

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All Science Journal Classification (ASJC) codes

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