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Activationless Charge Transfer Drives Photocurrent Generation in Organic Photovoltaic Blends Independent of Energetic Offset

Yifan Dong Orcid Logo, Rui Zheng, Deping Qian, Tack Ho Lee Orcid Logo, Helen L. Bristow, Pabitra Shakya Tuladhar, Hyojung Cha, James Durrant Orcid Logo

Journal of the American Chemical Society

Swansea University Author: James Durrant Orcid Logo

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DOI (Published version): 10.1021/jacs.4c11114

Abstract

Organic photovoltaics (OPVs) have recently shown substantial progress in enhancing device efficiency, driven in particular by advances in the design of nonfullerene acceptors and the reduction of the energy offset driving exciton separation at the donor/acceptor interface. Herein, we employ temperat...

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Published in: Journal of the American Chemical Society
ISSN: 0002-7863 1520-5126
Published: American Chemical Society (ACS) 2024
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URI: https://cronfa.swan.ac.uk/Record/cronfa68474
first_indexed 2024-12-06T13:48:58Z
last_indexed 2024-12-06T13:48:58Z
id cronfa68474
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spelling 2024-12-06T10:11:14.5425561 v2 68474 2024-12-06 Activationless Charge Transfer Drives Photocurrent Generation in Organic Photovoltaic Blends Independent of Energetic Offset f3dd64bc260e5c07adfa916c27dbd58a 0000-0001-8353-7345 James Durrant James Durrant true false 2024-12-06 EAAS Organic photovoltaics (OPVs) have recently shown substantial progress in enhancing device efficiency, driven in particular by advances in the design of nonfullerene acceptors and the reduction of the energy offset driving exciton separation at the donor/acceptor interface. Herein, we employ temperature-dependent transient absorption spectroscopy to investigate the activation energy for charge generation and recombination in a range of bulk heterojunction blends with nonfullerene acceptors. Remarkably, we find that in all cases charge generation is almost activationless, in the range of 11–21 meV, independent of energetic offset. Geminate recombination is also observed to be almost activationless, with only the kinetics of bimolecular charge recombination being strongly temperature-dependent, with an activation energy >400 meV. Our observation of essentially activationless charge generation, independent of energy offset, strongly indicates that charge generation in such blends does not follow Marcus theory but can rather be considered an adiabatic process associated with the motion of thermally unrelaxed carriers. Journal Article Journal of the American Chemical Society 0 American Chemical Society (ACS) 0002-7863 1520-5126 27 11 2024 2024-11-27 10.1021/jacs.4c11114 COLLEGE NANME Engineering and Applied Sciences School COLLEGE CODE EAAS Swansea University Another institution paid the OA fee The authors gratefully acknowledge financial support from the UKRI GCRF Project SUNRISE (EP/P032591/1) and EPSRC Project ATIP (EP/TO28513/1) and KAUST (OSR-2015-CRG4-2572 and OSR-2018-CRG7-3749.2). H.C. acknowledges financial support from the National Research Foundation of Korea (NRF) Grant funded by the Korea government (MSIT) (RS-2023-00213920). 2024-12-06T10:11:14.5425561 2024-12-06T09:57:05.7651862 Faculty of Science and Engineering School of Engineering and Applied Sciences - Materials Science and Engineering Yifan Dong 0000-0003-2912-3322 1 Rui Zheng 2 Deping Qian 3 Tack Ho Lee 0000-0003-2201-0165 4 Helen L. Bristow 5 Pabitra Shakya Tuladhar 6 Hyojung Cha 7 James Durrant 0000-0001-8353-7345 8
title Activationless Charge Transfer Drives Photocurrent Generation in Organic Photovoltaic Blends Independent of Energetic Offset
spellingShingle Activationless Charge Transfer Drives Photocurrent Generation in Organic Photovoltaic Blends Independent of Energetic Offset
James Durrant
title_short Activationless Charge Transfer Drives Photocurrent Generation in Organic Photovoltaic Blends Independent of Energetic Offset
title_full Activationless Charge Transfer Drives Photocurrent Generation in Organic Photovoltaic Blends Independent of Energetic Offset
title_fullStr Activationless Charge Transfer Drives Photocurrent Generation in Organic Photovoltaic Blends Independent of Energetic Offset
title_full_unstemmed Activationless Charge Transfer Drives Photocurrent Generation in Organic Photovoltaic Blends Independent of Energetic Offset
title_sort Activationless Charge Transfer Drives Photocurrent Generation in Organic Photovoltaic Blends Independent of Energetic Offset
author_id_str_mv f3dd64bc260e5c07adfa916c27dbd58a
author_id_fullname_str_mv f3dd64bc260e5c07adfa916c27dbd58a_***_James Durrant
author James Durrant
author2 Yifan Dong
Rui Zheng
Deping Qian
Tack Ho Lee
Helen L. Bristow
Pabitra Shakya Tuladhar
Hyojung Cha
James Durrant
format Journal article
container_title Journal of the American Chemical Society
container_volume 0
publishDate 2024
institution Swansea University
issn 0002-7863
1520-5126
doi_str_mv 10.1021/jacs.4c11114
publisher American Chemical Society (ACS)
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 0
active_str 0
description Organic photovoltaics (OPVs) have recently shown substantial progress in enhancing device efficiency, driven in particular by advances in the design of nonfullerene acceptors and the reduction of the energy offset driving exciton separation at the donor/acceptor interface. Herein, we employ temperature-dependent transient absorption spectroscopy to investigate the activation energy for charge generation and recombination in a range of bulk heterojunction blends with nonfullerene acceptors. Remarkably, we find that in all cases charge generation is almost activationless, in the range of 11–21 meV, independent of energetic offset. Geminate recombination is also observed to be almost activationless, with only the kinetics of bimolecular charge recombination being strongly temperature-dependent, with an activation energy >400 meV. Our observation of essentially activationless charge generation, independent of energy offset, strongly indicates that charge generation in such blends does not follow Marcus theory but can rather be considered an adiabatic process associated with the motion of thermally unrelaxed carriers.
published_date 2024-11-27T08:36:58Z
_version_ 1821393937393254400
score 11.048149

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