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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
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 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.
College: Faculty of Science and Engineering
Funders: 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).

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