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Electron spin resonance resolves intermediate triplet states in delayed fluorescence

Bluebell H. Drummond, Naoya Aizawa, Yadong Zhang, William K. Myers, Yao Xiong, Matthew W. Cooper, Stephen Barlow, Qinying Gu, Leah R. Weiss, Alexander J. Gillett, Dan Credgington, Yong-Jin Pu, Seth R. Marder, Emrys Evans Orcid Logo

Nature Communications, Volume: 12, Issue: 1

Swansea University Author: Emrys Evans Orcid Logo

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DOI (Published version): 10.1038/s41467-021-24612-9

Abstract

Molecular organic fluorophores are currently used in organic light-emitting diodes, though non-emissive triplet excitons generated in devices incorporating conventional fluorophores limit the efficiency. This limit can be overcome in materials that have intramolecular charge-transfer excitonic state...

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Published in: Nature Communications
ISSN: 2041-1723
Published: Springer Science and Business Media LLC 2021
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URI: https://cronfa.swan.ac.uk/Record/cronfa57410
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last_indexed 2023-01-11T14:37:18Z
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spelling 2022-10-27T14:41:14.4128774 v2 57410 2021-07-16 Electron spin resonance resolves intermediate triplet states in delayed fluorescence 538e217307dac24c9642ef1b03b41485 0000-0002-9092-3938 Emrys Evans Emrys Evans true false 2021-07-16 EAAS Molecular organic fluorophores are currently used in organic light-emitting diodes, though non-emissive triplet excitons generated in devices incorporating conventional fluorophores limit the efficiency. This limit can be overcome in materials that have intramolecular charge-transfer excitonic states and associated small singlet-triplet energy separations; triplets can then be converted to emissive singlet excitons resulting in efficient delayed fluorescence. However, the mechanistic details of the spin interconversion have not yet been fully resolved. We report transient electron spin resonance studies that allow direct probing of the spin conversion in a series of delayed fluorescence fluorophores with varying energy gaps between local excitation and charge-transfer triplet states. The observation of distinct triplet signals, unusual in transient electron spin resonance, suggests that multiple triplet states mediate the photophysics for efficient light emission in delayed fluorescence emitters. We reveal that as the energy separation between local excitation and charge-transfer triplet states decreases, spin interconversion changes from a direct, singlet-triplet mechanism to an indirect mechanism involving intermediate states. Journal Article Nature Communications 12 1 Springer Science and Business Media LLC 2041-1723 26 7 2021 2021-07-26 10.1038/s41467-021-24612-9 COLLEGE NANME Engineering and Applied Sciences School COLLEGE CODE EAAS Swansea University External research funder(s) paid the OA fee (includes OA grants disbursed by the Library) Engineering and Physical Sciences Research Council EP/M005143/1; EP/L015978/1; EP/L011972/1 2022-10-27T14:41:14.4128774 2021-07-16T14:41:06.6111576 Faculty of Science and Engineering School of Engineering and Applied Sciences - Chemistry Bluebell H. Drummond 1 Naoya Aizawa 2 Yadong Zhang 3 William K. Myers 4 Yao Xiong 5 Matthew W. Cooper 6 Stephen Barlow 7 Qinying Gu 8 Leah R. Weiss 9 Alexander J. Gillett 10 Dan Credgington 11 Yong-Jin Pu 12 Seth R. Marder 13 Emrys Evans 0000-0002-9092-3938 14 57410__20688__93c994a879864b119cdfc90e91f74e58.pdf 57410.pdf 2021-08-19T17:28:42.8188978 Output 1827064 application/pdf Version of Record true © The Author(s) 2021. This article is licensed under a Creative Commons Attribution 4.0 International License true eng http://creativecommons.org/licenses/by/4.0/
title Electron spin resonance resolves intermediate triplet states in delayed fluorescence
spellingShingle Electron spin resonance resolves intermediate triplet states in delayed fluorescence
Emrys Evans
title_short Electron spin resonance resolves intermediate triplet states in delayed fluorescence
title_full Electron spin resonance resolves intermediate triplet states in delayed fluorescence
title_fullStr Electron spin resonance resolves intermediate triplet states in delayed fluorescence
title_full_unstemmed Electron spin resonance resolves intermediate triplet states in delayed fluorescence
title_sort Electron spin resonance resolves intermediate triplet states in delayed fluorescence
author_id_str_mv 538e217307dac24c9642ef1b03b41485
author_id_fullname_str_mv 538e217307dac24c9642ef1b03b41485_***_Emrys Evans
author Emrys Evans
author2 Bluebell H. Drummond
Naoya Aizawa
Yadong Zhang
William K. Myers
Yao Xiong
Matthew W. Cooper
Stephen Barlow
Qinying Gu
Leah R. Weiss
Alexander J. Gillett
Dan Credgington
Yong-Jin Pu
Seth R. Marder
Emrys Evans
format Journal article
container_title Nature Communications
container_volume 12
container_issue 1
publishDate 2021
institution Swansea University
issn 2041-1723
doi_str_mv 10.1038/s41467-021-24612-9
publisher Springer Science and Business Media LLC
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 - Chemistry{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Chemistry
document_store_str 1
active_str 0
description Molecular organic fluorophores are currently used in organic light-emitting diodes, though non-emissive triplet excitons generated in devices incorporating conventional fluorophores limit the efficiency. This limit can be overcome in materials that have intramolecular charge-transfer excitonic states and associated small singlet-triplet energy separations; triplets can then be converted to emissive singlet excitons resulting in efficient delayed fluorescence. However, the mechanistic details of the spin interconversion have not yet been fully resolved. We report transient electron spin resonance studies that allow direct probing of the spin conversion in a series of delayed fluorescence fluorophores with varying energy gaps between local excitation and charge-transfer triplet states. The observation of distinct triplet signals, unusual in transient electron spin resonance, suggests that multiple triplet states mediate the photophysics for efficient light emission in delayed fluorescence emitters. We reveal that as the energy separation between local excitation and charge-transfer triplet states decreases, spin interconversion changes from a direct, singlet-triplet mechanism to an indirect mechanism involving intermediate states.
published_date 2021-07-26T20:15:38Z
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