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Elucidating the Origins of Subgap Tail States and Open-Circuit Voltage in Methylammonium Lead Triiodide Perovskite Solar Cells

Tian Du, Jinhyun Kim, Jonathan Ngiam, Shengda Xu, Piers R. F. Barnes, James Durrant Orcid Logo, Martyn A. McLachlan

Advanced Functional Materials, Volume: 28, Issue: 32, Start page: 1801808

Swansea University Author: James Durrant Orcid Logo

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DOI (Published version): 10.1002/adfm.201801808

Abstract

Recombination via subgap trap states is considered a limiting factor in the development of organometal halide perovskite solar cells. Here, the impact of active layer crystallinity on the accumulated charge and open‐circuit voltage (Voc) in solar cells based on methylammonium lead triiodide (CH3NH3P...

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Published in: Advanced Functional Materials
ISSN: 1616-301X
Published: 2018
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URI: https://cronfa.swan.ac.uk/Record/cronfa43500
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first_indexed 2018-08-17T11:56:58Z
last_indexed 2018-10-09T19:34:47Z
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spelling 2018-10-09T14:45:33.1670133 v2 43500 2018-08-17 Elucidating the Origins of Subgap Tail States and Open-Circuit Voltage in Methylammonium Lead Triiodide Perovskite Solar Cells f3dd64bc260e5c07adfa916c27dbd58a 0000-0001-8353-7345 James Durrant James Durrant true false 2018-08-17 MTLS Recombination via subgap trap states is considered a limiting factor in the development of organometal halide perovskite solar cells. Here, the impact of active layer crystallinity on the accumulated charge and open‐circuit voltage (Voc) in solar cells based on methylammonium lead triiodide (CH3NH3PbI3, MAPI) is demonstrated. It is shown that MAPI crystallinity can be systematically tailored by modulating the stoichiometry of the precursor mix, where small quantities of excess methylammonium iodide (MAI) improve crystallinity, increasing device Voc by ≈200 mV. Using in situ differential charging and transient photovoltage measurements, charge density and charge carrier recombination lifetime are determined under operational conditions. Increased Voc is correlated to improved active layer crystallinity and a reduction in the density of trap states in MAPI. Photoluminescence spectroscopy shows that an increase in trap state density correlates with faster carrier trapping and more nonradiative recombination pathways. Fundamental insights into the origin of Voc in perovskite photovoltaics are provided and it is demonstrated why highly crystalline perovskite films are paramount for high‐performance devices. Journal Article Advanced Functional Materials 28 32 1801808 1616-301X crystallinity, open‐circuit voltage, perovskite solar cells, tail states 6 8 2018 2018-08-06 10.1002/adfm.201801808 COLLEGE NANME Materials Science and Engineering COLLEGE CODE MTLS Swansea University 2018-10-09T14:45:33.1670133 2018-08-17T08:52:26.4550762 Faculty of Science and Engineering School of Engineering and Applied Sciences - Materials Science and Engineering Tian Du 1 Jinhyun Kim 2 Jonathan Ngiam 3 Shengda Xu 4 Piers R. F. Barnes 5 James Durrant 0000-0001-8353-7345 6 Martyn A. McLachlan 7 0043500-17082018085606.pdf du2018.pdf 2018-08-17T08:56:06.2300000 Output 2525236 application/pdf Version of Record true 2018-08-17T00:00:00.0000000 true eng
title Elucidating the Origins of Subgap Tail States and Open-Circuit Voltage in Methylammonium Lead Triiodide Perovskite Solar Cells
spellingShingle Elucidating the Origins of Subgap Tail States and Open-Circuit Voltage in Methylammonium Lead Triiodide Perovskite Solar Cells
James Durrant
title_short Elucidating the Origins of Subgap Tail States and Open-Circuit Voltage in Methylammonium Lead Triiodide Perovskite Solar Cells
title_full Elucidating the Origins of Subgap Tail States and Open-Circuit Voltage in Methylammonium Lead Triiodide Perovskite Solar Cells
title_fullStr Elucidating the Origins of Subgap Tail States and Open-Circuit Voltage in Methylammonium Lead Triiodide Perovskite Solar Cells
title_full_unstemmed Elucidating the Origins of Subgap Tail States and Open-Circuit Voltage in Methylammonium Lead Triiodide Perovskite Solar Cells
title_sort Elucidating the Origins of Subgap Tail States and Open-Circuit Voltage in Methylammonium Lead Triiodide Perovskite Solar Cells
author_id_str_mv f3dd64bc260e5c07adfa916c27dbd58a
author_id_fullname_str_mv f3dd64bc260e5c07adfa916c27dbd58a_***_James Durrant
author James Durrant
author2 Tian Du
Jinhyun Kim
Jonathan Ngiam
Shengda Xu
Piers R. F. Barnes
James Durrant
Martyn A. McLachlan
format Journal article
container_title Advanced Functional Materials
container_volume 28
container_issue 32
container_start_page 1801808
publishDate 2018
institution Swansea University
issn 1616-301X
doi_str_mv 10.1002/adfm.201801808
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
document_store_str 1
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description Recombination via subgap trap states is considered a limiting factor in the development of organometal halide perovskite solar cells. Here, the impact of active layer crystallinity on the accumulated charge and open‐circuit voltage (Voc) in solar cells based on methylammonium lead triiodide (CH3NH3PbI3, MAPI) is demonstrated. It is shown that MAPI crystallinity can be systematically tailored by modulating the stoichiometry of the precursor mix, where small quantities of excess methylammonium iodide (MAI) improve crystallinity, increasing device Voc by ≈200 mV. Using in situ differential charging and transient photovoltage measurements, charge density and charge carrier recombination lifetime are determined under operational conditions. Increased Voc is correlated to improved active layer crystallinity and a reduction in the density of trap states in MAPI. Photoluminescence spectroscopy shows that an increase in trap state density correlates with faster carrier trapping and more nonradiative recombination pathways. Fundamental insights into the origin of Voc in perovskite photovoltaics are provided and it is demonstrated why highly crystalline perovskite films are paramount for high‐performance devices.
published_date 2018-08-06T03:54:42Z
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