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Impact of Interface Energetic Alignment and Mobile Ions on Charge Carrier Accumulation and Extraction in p‐i‐n Perovskite Solar Cells

Weidong Xu Orcid Logo, Lucy J. F. Hart Orcid Logo, Benjamin Moss, Pietro Caprioglio, Thomas J. Macdonald, Francesco Furlan, Julianna Panidi, Robert D. J. Oliver, Richard A. Pacalaj, Martin Heeney, Nicola Gasparini, Henry J. Snaith, Piers R. F. Barnes, James Durrant Orcid Logo

Advanced Energy Materials

Swansea University Author: James Durrant Orcid Logo

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DOI (Published version): 10.1002/aenm.202301102

Abstract

Understanding the kinetic competition between charge extraction and recombination, and how this is impacted by mobile ions, remains a key challenge in perovskite solar cells (PSCs). Here, this issue is addressed by combining operando photoluminescence (PL) measurements, which allow the measurement o...

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Published in: Advanced Energy Materials
ISSN: 1614-6832 1614-6840
Published: Wiley
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URI: https://cronfa.swan.ac.uk/Record/cronfa64065
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Here, this issue is addressed by combining operando photoluminescence (PL) measurements, which allow the measurement of real-time PL spectra during current–voltage (J–V) scans under 1-sun equivalent illumination, with the results of drift-diffusion simulations. This operando PL analysis allows direct comparison between the internal performance (recombination currents and quasi-Fermi-level-splitting (QFLS)) and the external performance (J–V) of a PSC during operation. Analyses of four PSCs with different electron transport materials (ETMs) quantify how a deeper ETM LUMO induces greater interfacial recombination, while a shallower LUMO impedes charge extraction. Furthermore, it is found that a low ETM mobility leads to charge accumulation in the perovskite under short-circuit conditions. However, thisalone cannot explain the remarkably high short-circuit QFLS of over 1 eV which is observed in all devices. 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spelling v2 64065 2023-08-09 Impact of Interface Energetic Alignment and Mobile Ions on Charge Carrier Accumulation and Extraction in p‐i‐n Perovskite Solar Cells f3dd64bc260e5c07adfa916c27dbd58a 0000-0001-8353-7345 James Durrant James Durrant true false 2023-08-09 MTLS Understanding the kinetic competition between charge extraction and recombination, and how this is impacted by mobile ions, remains a key challenge in perovskite solar cells (PSCs). Here, this issue is addressed by combining operando photoluminescence (PL) measurements, which allow the measurement of real-time PL spectra during current–voltage (J–V) scans under 1-sun equivalent illumination, with the results of drift-diffusion simulations. This operando PL analysis allows direct comparison between the internal performance (recombination currents and quasi-Fermi-level-splitting (QFLS)) and the external performance (J–V) of a PSC during operation. Analyses of four PSCs with different electron transport materials (ETMs) quantify how a deeper ETM LUMO induces greater interfacial recombination, while a shallower LUMO impedes charge extraction. Furthermore, it is found that a low ETM mobility leads to charge accumulation in the perovskite under short-circuit conditions. However, thisalone cannot explain the remarkably high short-circuit QFLS of over 1 eV which is observed in all devices. Instead, drift-diffusion simulations allow this effect to be assigned to the presence of mobile ions which screen the internal electric field at short-circuit and lead to a reduction in the short-circuit current density by over 2 mA cm−2 in the best device. Journal Article Advanced Energy Materials Wiley 1614-6832 1614-6840 Charge accumulation, charge extraction, drift-diffusion simulation, ion migration, operando photoluminescence spectroscopy, perovskite solar cells, quasi-Fermi level splitting 0 0 0 0001-01-01 10.1002/aenm.202301102 http://dx.doi.org/10.1002/aenm.202301102 COLLEGE NANME Materials Science and Engineering COLLEGE CODE MTLS Swansea University EPSRC, Korean NRF GRL, European Commission Research Executive Agency, Royal Society University Research Fellowship, Royal Society Research Fellows Enhanced Research Expenses EP/T028513/1, EP/L016702/1, EP/V057839/1, EP/T012455/1, 2017K1A1A2013153, 859752 HEL4CHIR-OLED H2020-MSCA-ITN-2019, URF/R1/221834, RF/ERE/221066 2023-09-08T12:15:50.8061181 2023-08-09T10:02:14.9913453 Faculty of Science and Engineering School of Engineering and Applied Sciences - Materials Science and Engineering Weidong Xu 0000-0002-3934-8579 1 Lucy J. F. Hart 0000-0002-6269-4672 2 Benjamin Moss 3 Pietro Caprioglio 4 Thomas J. Macdonald 5 Francesco Furlan 6 Julianna Panidi 7 Robert D. J. Oliver 8 Richard A. Pacalaj 9 Martin Heeney 10 Nicola Gasparini 11 Henry J. Snaith 12 Piers R. F. Barnes 13 James Durrant 0000-0001-8353-7345 14 64065__28278__576fc709fa16420a920151d497fe9f0e.pdf 64065.pdf 2023-08-09T10:13:37.4653248 Output 2479362 application/pdf Version of Record true © 2023 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH. Distributed under the terms of a Creative Commons Attribution 4.0 License (CC BY 4.0). true eng http://creativecommons.org/licenses/by/4.0/
title Impact of Interface Energetic Alignment and Mobile Ions on Charge Carrier Accumulation and Extraction in p‐i‐n Perovskite Solar Cells
spellingShingle Impact of Interface Energetic Alignment and Mobile Ions on Charge Carrier Accumulation and Extraction in p‐i‐n Perovskite Solar Cells
James Durrant
title_short Impact of Interface Energetic Alignment and Mobile Ions on Charge Carrier Accumulation and Extraction in p‐i‐n Perovskite Solar Cells
title_full Impact of Interface Energetic Alignment and Mobile Ions on Charge Carrier Accumulation and Extraction in p‐i‐n Perovskite Solar Cells
title_fullStr Impact of Interface Energetic Alignment and Mobile Ions on Charge Carrier Accumulation and Extraction in p‐i‐n Perovskite Solar Cells
title_full_unstemmed Impact of Interface Energetic Alignment and Mobile Ions on Charge Carrier Accumulation and Extraction in p‐i‐n Perovskite Solar Cells
title_sort Impact of Interface Energetic Alignment and Mobile Ions on Charge Carrier Accumulation and Extraction in p‐i‐n Perovskite Solar Cells
author_id_str_mv f3dd64bc260e5c07adfa916c27dbd58a
author_id_fullname_str_mv f3dd64bc260e5c07adfa916c27dbd58a_***_James Durrant
author James Durrant
author2 Weidong Xu
Lucy J. F. Hart
Benjamin Moss
Pietro Caprioglio
Thomas J. Macdonald
Francesco Furlan
Julianna Panidi
Robert D. J. Oliver
Richard A. Pacalaj
Martin Heeney
Nicola Gasparini
Henry J. Snaith
Piers R. F. Barnes
James Durrant
format Journal article
container_title Advanced Energy Materials
institution Swansea University
issn 1614-6832
1614-6840
doi_str_mv 10.1002/aenm.202301102
publisher Wiley
college_str Faculty of Science and Engineering
hierarchytype
hierarchy_top_id facultyofscienceandengineering
hierarchy_top_title Faculty of Science and Engineering
hierarchy_parent_id facultyofscienceandengineering
hierarchy_parent_title Faculty of Science and Engineering
department_str School of Engineering and Applied Sciences - Materials Science and Engineering{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Materials Science and Engineering
url http://dx.doi.org/10.1002/aenm.202301102
document_store_str 1
active_str 0
description Understanding the kinetic competition between charge extraction and recombination, and how this is impacted by mobile ions, remains a key challenge in perovskite solar cells (PSCs). Here, this issue is addressed by combining operando photoluminescence (PL) measurements, which allow the measurement of real-time PL spectra during current–voltage (J–V) scans under 1-sun equivalent illumination, with the results of drift-diffusion simulations. This operando PL analysis allows direct comparison between the internal performance (recombination currents and quasi-Fermi-level-splitting (QFLS)) and the external performance (J–V) of a PSC during operation. Analyses of four PSCs with different electron transport materials (ETMs) quantify how a deeper ETM LUMO induces greater interfacial recombination, while a shallower LUMO impedes charge extraction. Furthermore, it is found that a low ETM mobility leads to charge accumulation in the perovskite under short-circuit conditions. However, thisalone cannot explain the remarkably high short-circuit QFLS of over 1 eV which is observed in all devices. Instead, drift-diffusion simulations allow this effect to be assigned to the presence of mobile ions which screen the internal electric field at short-circuit and lead to a reduction in the short-circuit current density by over 2 mA cm−2 in the best device.
published_date 0001-01-01T12:15:52Z
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score 11.01628

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