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Breaking Crystallinity for Optimal Dark Current: Nonfullerene Acceptor Dilution as a Strategy for High‐Performance Organic Photodetectors

Chiara Labanti Orcid Logo, Ying Sun, Joel Luke Orcid Logo, Yifan Dong Orcid Logo, Song Yi Park, Yi‐Chun Chin Orcid Logo, Tianhao Lan, Emily J. Yang Orcid Logo, Lei Zhang Orcid Logo, Soranyel Gonzalez‐Carrero Orcid Logo, James Durrant, Ji‐Seon Kim Orcid Logo

Advanced Optical Materials, Volume: 13, Issue: 19, Start page: 2500255

Swansea University Author: James Durrant

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DOI (Published version): 10.1002/adom.202500255

Abstract

Organic photodetectors (OPDs) based on polymer donor:non‐fullerene‐acceptor (NFA) bulk heterojunction (BHJ) blends demonstrate great potential for light‐sensing applications, thanks to optoelectronic tunability and strong absorption. However, state‐of‐the‐art organic photoconversion devices lag behi...

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Published in: Advanced Optical Materials
ISSN: 2195-1071 2195-1071
Published: Wiley 2025
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URI: https://cronfa.swan.ac.uk/Record/cronfa69550
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spelling 2025-07-30T14:40:52.2476627 v2 69550 2025-05-22 Breaking Crystallinity for Optimal Dark Current: Nonfullerene Acceptor Dilution as a Strategy for High‐Performance Organic Photodetectors f3dd64bc260e5c07adfa916c27dbd58a James Durrant James Durrant true false 2025-05-22 Organic photodetectors (OPDs) based on polymer donor:non‐fullerene‐acceptor (NFA) bulk heterojunction (BHJ) blends demonstrate great potential for light‐sensing applications, thanks to optoelectronic tunability and strong absorption. However, state‐of‐the‐art organic photoconversion devices lag behind silicon counterparts due to the laborious dark current, Jd, and photodetection speed optimization required in OPDs. Herein, the donor/acceptor blend ratio is controlled to optimize PM6:Y6‐based OPDs, with diluted Y6 blends (1:0.1 D/A weight ratio) strongly suppressing Jd to 6.5 × 10−9 A cm−2 (−4 V). Diluted OPDs exhibit faster photoresponse and poor short‐circuit photocurrent generation is dramatically improved under reverse bias. In‐depth photophysical and energetic analysis reveal the origin of high performance. In diluted blends, dissociation of emissive strongly bound excitonic charge‐transfer states within Y6 require electric field assistance, while the polymer matrix provides a continuous charge‐transport pathway. The generality of this strategy is tested with various NFAs, with NFA dilution being most effective for highly crystalline acceptors. It is determined that the reduction in dark current is predominantly driven by disruption of NFA crystallinity and intermolecular interactions. Polymer‐rich BHJ devices, therefore, provide an effective optimization method for reducing dark current in OPDs and are highly promising for industrial scalability due to facile processability, robust mechanical properties, and superior thermal stability. Journal Article Advanced Optical Materials 13 19 2500255 Wiley 2195-1071 2195-1071 charge generation, dark current, organic photoconversion, organic photodetectors, organic semiconductors 4 7 2025 2025-07-04 10.1002/adom.202500255 COLLEGE NANME COLLEGE CODE Swansea University Another institution paid the OA fee The authors acknowledge the UK Engineering and Physical Sciences Research Council for funding through both the Application Targeted and Integrated Photovoltaics programme grant (EP/T028513/1) and the Centre for Doctoral Training in Plastic Electronic Materials (EP/L016702/1). 2025-07-30T14:40:52.2476627 2025-05-22T11:15:09.4544161 Faculty of Science and Engineering School of Engineering and Applied Sciences - Materials Science and Engineering Chiara Labanti 0000-0002-9732-388x 1 Ying Sun 2 Joel Luke 0000-0003-3208-8572 3 Yifan Dong 0000-0003-2912-3322 4 Song Yi Park 5 Yi‐Chun Chin 0000-0002-4434-7271 6 Tianhao Lan 7 Emily J. Yang 0000-0002-2418-4161 8 Lei Zhang 0009-0005-7024-2691 9 Soranyel Gonzalez‐Carrero 0000-0003-2430-4458 10 James Durrant 11 Ji‐Seon Kim 0000-0003-4715-3656 12 69550__34328__9fbf6a05ad454d89a159c568cc84f69a.pdf adom.202500255.pdf 2025-05-22T11:15:09.4180613 Output 3273206 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 (CC BY). true eng http://creativecommons.org/licenses/by/4.0/
title Breaking Crystallinity for Optimal Dark Current: Nonfullerene Acceptor Dilution as a Strategy for High‐Performance Organic Photodetectors
spellingShingle Breaking Crystallinity for Optimal Dark Current: Nonfullerene Acceptor Dilution as a Strategy for High‐Performance Organic Photodetectors
James Durrant
title_short Breaking Crystallinity for Optimal Dark Current: Nonfullerene Acceptor Dilution as a Strategy for High‐Performance Organic Photodetectors
title_full Breaking Crystallinity for Optimal Dark Current: Nonfullerene Acceptor Dilution as a Strategy for High‐Performance Organic Photodetectors
title_fullStr Breaking Crystallinity for Optimal Dark Current: Nonfullerene Acceptor Dilution as a Strategy for High‐Performance Organic Photodetectors
title_full_unstemmed Breaking Crystallinity for Optimal Dark Current: Nonfullerene Acceptor Dilution as a Strategy for High‐Performance Organic Photodetectors
title_sort Breaking Crystallinity for Optimal Dark Current: Nonfullerene Acceptor Dilution as a Strategy for High‐Performance Organic Photodetectors
author_id_str_mv f3dd64bc260e5c07adfa916c27dbd58a
author_id_fullname_str_mv f3dd64bc260e5c07adfa916c27dbd58a_***_James Durrant
author James Durrant
author2 Chiara Labanti
Ying Sun
Joel Luke
Yifan Dong
Song Yi Park
Yi‐Chun Chin
Tianhao Lan
Emily J. Yang
Lei Zhang
Soranyel Gonzalez‐Carrero
James Durrant
Ji‐Seon Kim
format Journal article
container_title Advanced Optical Materials
container_volume 13
container_issue 19
container_start_page 2500255
publishDate 2025
institution Swansea University
issn 2195-1071
2195-1071
doi_str_mv 10.1002/adom.202500255
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
document_store_str 1
active_str 0
description Organic photodetectors (OPDs) based on polymer donor:non‐fullerene‐acceptor (NFA) bulk heterojunction (BHJ) blends demonstrate great potential for light‐sensing applications, thanks to optoelectronic tunability and strong absorption. However, state‐of‐the‐art organic photoconversion devices lag behind silicon counterparts due to the laborious dark current, Jd, and photodetection speed optimization required in OPDs. Herein, the donor/acceptor blend ratio is controlled to optimize PM6:Y6‐based OPDs, with diluted Y6 blends (1:0.1 D/A weight ratio) strongly suppressing Jd to 6.5 × 10−9 A cm−2 (−4 V). Diluted OPDs exhibit faster photoresponse and poor short‐circuit photocurrent generation is dramatically improved under reverse bias. In‐depth photophysical and energetic analysis reveal the origin of high performance. In diluted blends, dissociation of emissive strongly bound excitonic charge‐transfer states within Y6 require electric field assistance, while the polymer matrix provides a continuous charge‐transport pathway. The generality of this strategy is tested with various NFAs, with NFA dilution being most effective for highly crystalline acceptors. It is determined that the reduction in dark current is predominantly driven by disruption of NFA crystallinity and intermolecular interactions. Polymer‐rich BHJ devices, therefore, provide an effective optimization method for reducing dark current in OPDs and are highly promising for industrial scalability due to facile processability, robust mechanical properties, and superior thermal stability.
published_date 2025-07-04T05:24:58Z
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