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Critical Role of Non‐Fullerene Crystalline Domains in Stabilizing Charge Separation in Bulk Heterojunction Organic Solar Cells

Soyeong Jeong, Aniket Rana, Weidong Xu, Keren Ai, Rachel Catherine Kilbride, Yiwen Wang, Damin Lee, Pabitra Shakya Tuladhar, Hyojung Cha Orcid Logo, James Durrant

Advanced Energy Materials, Volume: 15, Issue: 33, Start page: 2501633

Swansea University Author: James Durrant

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DOI (Published version): 10.1002/aenm.202501633

Abstract

This study addresses the role of energetic offsets resulting from non‐fullerene acceptor crystallization/aggregation in stabilizing charge separation in organic bulk heterojunction (BHJ) solar cells. Devices are fabricated using PM6 as electron donor and either IDIC or Y6 as acceptor, with blend rat...

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Published in: Advanced Energy Materials
ISSN: 1614-6832 1614-6840
Published: Wiley 2025
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URI: https://cronfa.swan.ac.uk/Record/cronfa69779
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Reducing acceptor content significantly lowers device performance, most notably for initially higher performing PM6:Y6 BHJ's (from 14.31% to 0.95%) compared to PM6:IDIC (from 11.28% to 3.40%). Optical, optoelectronic, and morphological characterizations reveal that lower acceptor content PM6:Y6 devices exhibit suppressed acceptor aggregation/crystallinity, correlated with increased recombination losses and lower efficiency. Charge separation in optimal (1:1) PM6:Y6 devices is found to be stabilized by a LUMO level energetic offset between intermixed and pure, more crystalline, Y6 domains, driven by strong electronic interactions between Y6 molecules. In contrast, PM6:IDIC devices show minimal changes in energetics and recombination kinetics, aligning with their smaller performance decline, and consistent with IDIC's weaker electronic interactions. 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spelling 2025-11-10T12:20:05.9038613 v2 69779 2025-06-20 Critical Role of Non‐Fullerene Crystalline Domains in Stabilizing Charge Separation in Bulk Heterojunction Organic Solar Cells f3dd64bc260e5c07adfa916c27dbd58a James Durrant James Durrant true false 2025-06-20 This study addresses the role of energetic offsets resulting from non‐fullerene acceptor crystallization/aggregation in stabilizing charge separation in organic bulk heterojunction (BHJ) solar cells. Devices are fabricated using PM6 as electron donor and either IDIC or Y6 as acceptor, with blend ratios from 5:1 to 1:1. Reducing acceptor content significantly lowers device performance, most notably for initially higher performing PM6:Y6 BHJ's (from 14.31% to 0.95%) compared to PM6:IDIC (from 11.28% to 3.40%). Optical, optoelectronic, and morphological characterizations reveal that lower acceptor content PM6:Y6 devices exhibit suppressed acceptor aggregation/crystallinity, correlated with increased recombination losses and lower efficiency. Charge separation in optimal (1:1) PM6:Y6 devices is found to be stabilized by a LUMO level energetic offset between intermixed and pure, more crystalline, Y6 domains, driven by strong electronic interactions between Y6 molecules. In contrast, PM6:IDIC devices show minimal changes in energetics and recombination kinetics, aligning with their smaller performance decline, and consistent with IDIC's weaker electronic interactions. As such strong electronic interactions between Y6 molecules are concluded to provide an energetic stabilization of electrons in more aggregated/crystalline Y6 domains, suppressing charge recombination, and analogous to that observed for the highest performing fullerene acceptor PCBM. Journal Article Advanced Energy Materials 15 33 2501633 Wiley 1614-6832 1614-6840 bulk heterojunction, charge transfer, intermixed phases, non-fullerene acceptors, photovoltaic device, recombination dynamics, solar cells 2 9 2025 2025-09-02 10.1002/aenm.202501633 COLLEGE NANME COLLEGE CODE Swansea University Another institution paid the OA fee Heeger Center for Advanced Materials; Research Institute for Solar and Sustainable Energies; Global Research Laboratory Program. Grant Number: NRF-2017K1A1A2013153; National Research Foundation; Engineering and Physical Sciences Research Council. Grant Number: ATIP EP/T028513/1; Gwangju Institute of Science and Technology; Postdoctoral Fellowship Program. Grant Number: NRF-2021R1A6A3A03045866 2025-11-10T12:20:05.9038613 2025-06-20T12:59:29.1218828 Faculty of Science and Engineering School of Engineering and Applied Sciences - Materials Science and Engineering Soyeong Jeong 1 Aniket Rana 2 Weidong Xu 3 Keren Ai 4 Rachel Catherine Kilbride 5 Yiwen Wang 6 Damin Lee 7 Pabitra Shakya Tuladhar 8 Hyojung Cha 0000-0003-0184-9471 9 James Durrant 10 69779__34533__58133abac0ca4772834fa571fcd65356.pdf aenm.202501633.pdf 2025-06-20T12:59:29.0975595 Output 2250476 application/pdf Version of Record true © 2025 The Author(s). This is an open access article under the terms of the Creative Commons Attribution License. true eng http://creativecommons.org/licenses/by/4.0/
title Critical Role of Non‐Fullerene Crystalline Domains in Stabilizing Charge Separation in Bulk Heterojunction Organic Solar Cells
spellingShingle Critical Role of Non‐Fullerene Crystalline Domains in Stabilizing Charge Separation in Bulk Heterojunction Organic Solar Cells
James Durrant
title_short Critical Role of Non‐Fullerene Crystalline Domains in Stabilizing Charge Separation in Bulk Heterojunction Organic Solar Cells
title_full Critical Role of Non‐Fullerene Crystalline Domains in Stabilizing Charge Separation in Bulk Heterojunction Organic Solar Cells
title_fullStr Critical Role of Non‐Fullerene Crystalline Domains in Stabilizing Charge Separation in Bulk Heterojunction Organic Solar Cells
title_full_unstemmed Critical Role of Non‐Fullerene Crystalline Domains in Stabilizing Charge Separation in Bulk Heterojunction Organic Solar Cells
title_sort Critical Role of Non‐Fullerene Crystalline Domains in Stabilizing Charge Separation in Bulk Heterojunction Organic Solar Cells
author_id_str_mv f3dd64bc260e5c07adfa916c27dbd58a
author_id_fullname_str_mv f3dd64bc260e5c07adfa916c27dbd58a_***_James Durrant
author James Durrant
author2 Soyeong Jeong
Aniket Rana
Weidong Xu
Keren Ai
Rachel Catherine Kilbride
Yiwen Wang
Damin Lee
Pabitra Shakya Tuladhar
Hyojung Cha
James Durrant
format Journal article
container_title Advanced Energy Materials
container_volume 15
container_issue 33
container_start_page 2501633
publishDate 2025
institution Swansea University
issn 1614-6832
1614-6840
doi_str_mv 10.1002/aenm.202501633
publisher Wiley
college_str Faculty of Science and Engineering
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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 This study addresses the role of energetic offsets resulting from non‐fullerene acceptor crystallization/aggregation in stabilizing charge separation in organic bulk heterojunction (BHJ) solar cells. Devices are fabricated using PM6 as electron donor and either IDIC or Y6 as acceptor, with blend ratios from 5:1 to 1:1. Reducing acceptor content significantly lowers device performance, most notably for initially higher performing PM6:Y6 BHJ's (from 14.31% to 0.95%) compared to PM6:IDIC (from 11.28% to 3.40%). Optical, optoelectronic, and morphological characterizations reveal that lower acceptor content PM6:Y6 devices exhibit suppressed acceptor aggregation/crystallinity, correlated with increased recombination losses and lower efficiency. Charge separation in optimal (1:1) PM6:Y6 devices is found to be stabilized by a LUMO level energetic offset between intermixed and pure, more crystalline, Y6 domains, driven by strong electronic interactions between Y6 molecules. In contrast, PM6:IDIC devices show minimal changes in energetics and recombination kinetics, aligning with their smaller performance decline, and consistent with IDIC's weaker electronic interactions. As such strong electronic interactions between Y6 molecules are concluded to provide an energetic stabilization of electrons in more aggregated/crystalline Y6 domains, suppressing charge recombination, and analogous to that observed for the highest performing fullerene acceptor PCBM.
published_date 2025-09-02T05:29:04Z
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