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Singlet and triplet to doublet energy transfer: improving organic light-emitting diodes with radicals

Feng Li Orcid Logo, Alexander J. Gillett Orcid Logo, Qinying Gu, Junshuai Ding, Zhangwu Chen, Timothy J. H. Hele Orcid Logo, William K. Myers Orcid Logo, Richard H. Friend Orcid Logo, Emrys Evans Orcid Logo

Nature Communications, Volume: 13, Issue: 1

Swansea University Author: Emrys Evans Orcid Logo

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Abstract

Organic light-emitting diodes (OLEDs) must be engineered to circumvent the efficiency limit imposed by the 3:1 ratio of triplet to singlet exciton formation following electron-hole capture. Here we show the spin nature of luminescent radicals such as TTM-3PCz allows direct energy harvesting from bot...

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Published in: Nature Communications
ISSN: 2041-1723
Published: Springer Science and Business Media LLC 2022
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URI: https://cronfa.swan.ac.uk/Record/cronfa60723
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Here we show the spin nature of luminescent radicals such as TTM-3PCz allows direct energy harvesting from both singlet and triplet excitons through energy transfer, with subsequent rapid and efficient light emission from the doublet excitons. This is demonstrated with a model Thermally-Activated Delayed Fluorescence (TADF) organic semiconductor, 4CzIPN, where reverse intersystem crossing from triplets is characteristically slow (50% emission by 1 &#xB5;s). The radical:TADF combination shows much faster emission via the doublet channel (80% emission by 100&#x2009;ns) than the comparable TADF-only system, and sustains higher electroluminescent efficiency with increasing current density than a radical-only device. 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E.W.E. is grateful to the Leverhulme Trust for an Early Career Fellowship; and the Royal Society for a University Research Fellowship (grant no. URF\R1\201300). TJHH thanks the Royal Society for a University Research Fellowship (grant no. URF\R1\201502). WKM and the Centre for Advanced Electron Spin Resonance is supported by EPSRC (EP/L011972/1). F.L. is an academic visitor at the Cavendish Laboratory, Cambridge, and is supported by the Talents Cultivation Programme (Jilin University, China). A.J.G. and RHF acknowledge support from the Simons Foundation (grant no. 601946) and the EPSRC (EP/M01083X/1 and EP/M005143/1). 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spelling 2022-10-27T14:53:53.6080494 v2 60723 2022-08-03 Singlet and triplet to doublet energy transfer: improving organic light-emitting diodes with radicals 538e217307dac24c9642ef1b03b41485 0000-0002-9092-3938 Emrys Evans Emrys Evans true false 2022-08-03 CHEM Organic light-emitting diodes (OLEDs) must be engineered to circumvent the efficiency limit imposed by the 3:1 ratio of triplet to singlet exciton formation following electron-hole capture. Here we show the spin nature of luminescent radicals such as TTM-3PCz allows direct energy harvesting from both singlet and triplet excitons through energy transfer, with subsequent rapid and efficient light emission from the doublet excitons. This is demonstrated with a model Thermally-Activated Delayed Fluorescence (TADF) organic semiconductor, 4CzIPN, where reverse intersystem crossing from triplets is characteristically slow (50% emission by 1 µs). The radical:TADF combination shows much faster emission via the doublet channel (80% emission by 100 ns) than the comparable TADF-only system, and sustains higher electroluminescent efficiency with increasing current density than a radical-only device. By unlocking energy transfer channels between singlet, triplet and doublet excitons, further technology opportunities are enabled for optoelectronics using organic radicals. Journal Article Nature Communications 13 1 Springer Science and Business Media LLC 2041-1723 18 5 2022 2022-05-18 10.1038/s41467-022-29759-7 COLLEGE NANME Chemistry COLLEGE CODE CHEM Swansea University J.D., Z.C. and F.L. are grateful for financial support from the National Natural Science Foundation of China (grant no. 51925303). E.W.E. is grateful to the Leverhulme Trust for an Early Career Fellowship; and the Royal Society for a University Research Fellowship (grant no. URF\R1\201300). TJHH thanks the Royal Society for a University Research Fellowship (grant no. URF\R1\201502). WKM and the Centre for Advanced Electron Spin Resonance is supported by EPSRC (EP/L011972/1). F.L. is an academic visitor at the Cavendish Laboratory, Cambridge, and is supported by the Talents Cultivation Programme (Jilin University, China). A.J.G. and RHF acknowledge support from the Simons Foundation (grant no. 601946) and the EPSRC (EP/M01083X/1 and EP/M005143/1). This project has received funding from the ERC under the European Union’s Horizon 2020 research and innovation programme (grant agreement no. 670405 and 101020167). 2022-10-27T14:53:53.6080494 2022-08-03T16:28:37.0700214 Faculty of Science and Engineering School of Engineering and Applied Sciences - Chemistry Feng Li 0000-0001-5236-3709 1 Alexander J. Gillett 0000-0001-7572-7333 2 Qinying Gu 3 Junshuai Ding 4 Zhangwu Chen 5 Timothy J. H. Hele 0000-0003-2367-3825 6 William K. Myers 0000-0001-5935-9112 7 Richard H. Friend 0000-0001-6565-6308 8 Emrys Evans 0000-0002-9092-3938 9 60723__25024__e5bd131668a24fd69f6709b968fb83b7.pdf 60723_VoR.pdf 2022-08-26T12:10:34.2632701 Output 2560411 application/pdf Version of Record true © The Author(s) 2022. This article is licensed under a Creative Commons Attribution 4.0 International License true eng http://creativecommons.org/licenses/by/4.0/
title Singlet and triplet to doublet energy transfer: improving organic light-emitting diodes with radicals
spellingShingle Singlet and triplet to doublet energy transfer: improving organic light-emitting diodes with radicals
Emrys Evans
title_short Singlet and triplet to doublet energy transfer: improving organic light-emitting diodes with radicals
title_full Singlet and triplet to doublet energy transfer: improving organic light-emitting diodes with radicals
title_fullStr Singlet and triplet to doublet energy transfer: improving organic light-emitting diodes with radicals
title_full_unstemmed Singlet and triplet to doublet energy transfer: improving organic light-emitting diodes with radicals
title_sort Singlet and triplet to doublet energy transfer: improving organic light-emitting diodes with radicals
author_id_str_mv 538e217307dac24c9642ef1b03b41485
author_id_fullname_str_mv 538e217307dac24c9642ef1b03b41485_***_Emrys Evans
author Emrys Evans
author2 Feng Li
Alexander J. Gillett
Qinying Gu
Junshuai Ding
Zhangwu Chen
Timothy J. H. Hele
William K. Myers
Richard H. Friend
Emrys Evans
format Journal article
container_title Nature Communications
container_volume 13
container_issue 1
publishDate 2022
institution Swansea University
issn 2041-1723
doi_str_mv 10.1038/s41467-022-29759-7
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
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description Organic light-emitting diodes (OLEDs) must be engineered to circumvent the efficiency limit imposed by the 3:1 ratio of triplet to singlet exciton formation following electron-hole capture. Here we show the spin nature of luminescent radicals such as TTM-3PCz allows direct energy harvesting from both singlet and triplet excitons through energy transfer, with subsequent rapid and efficient light emission from the doublet excitons. This is demonstrated with a model Thermally-Activated Delayed Fluorescence (TADF) organic semiconductor, 4CzIPN, where reverse intersystem crossing from triplets is characteristically slow (50% emission by 1 µs). The radical:TADF combination shows much faster emission via the doublet channel (80% emission by 100 ns) than the comparable TADF-only system, and sustains higher electroluminescent efficiency with increasing current density than a radical-only device. By unlocking energy transfer channels between singlet, triplet and doublet excitons, further technology opportunities are enabled for optoelectronics using organic radicals.
published_date 2022-05-18T04:19:04Z
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