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Fast Transfer of Triplet to Doublet Excitons from Organometallic Host to Organic Radical Semiconductors

Qinying Gu, Sebastian Gorgon, Alexander S. Romanov, Feng Li, Richard H. Friend, Emrys Evans Orcid Logo

Advanced Materials, Volume: 36, Issue: 30, Start page: 2402790

Swansea University Author: Emrys Evans Orcid Logo

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DOI (Published version): 10.1002/adma.202402790

Abstract

Spin triplet exciton formation sets limits on technologies using organic semiconductors that are confined to singlet-triplet photophysics. In contrast, excitations in the spin doublet manifold in organic radical semiconductors can show efficient luminescence. Here we explore the dynamics of the spin...

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Published in: Advanced Materials
ISSN: 0935-9648 1521-4095
Published: Wiley 2024
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URI: https://cronfa.swan.ac.uk/Record/cronfa66573
first_indexed 2024-06-03T11:33:31Z
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spelling 2024-11-01T14:06:59.6426721 v2 66573 2024-06-03 Fast Transfer of Triplet to Doublet Excitons from Organometallic Host to Organic Radical Semiconductors 538e217307dac24c9642ef1b03b41485 0000-0002-9092-3938 Emrys Evans Emrys Evans true false 2024-06-03 EAAS Spin triplet exciton formation sets limits on technologies using organic semiconductors that are confined to singlet-triplet photophysics. In contrast, excitations in the spin doublet manifold in organic radical semiconductors can show efficient luminescence. Here we explore the dynamics of the spin allowed process of intermolecular energy transfer from triplet to doublet excitons. We employ a carbene-metal-amide (CMA-CF3) as a model triplet donor host, since following photoexcitation it undergoes extremely fast intersystem crossing to set up a population of triplet excitons within 4 ps. This enables a foundational study for tracking energy transfer from triplets to a model radical semiconductor, TTM-3PCz. Over 74% of all radical luminescence originates from the triplet channel in this system under photoexcitation. We find that intermolecular triplet-to-doublet energy transfer can occur directly and rapidly, with 12% of triplet excitons transferring already on sub-ns timescales. This enhanced triplet harvesting mechanism is utilised in efficient near-infrared organic light-emitting diodes, which can be extended to other opto-electronic and -spintronic technologies by radical-based spin control in molecular semiconductors. Journal Article Advanced Materials 36 30 2402790 Wiley 0935-9648 1521-4095 Doublet emission; exciton management; organic light-emitting diodes; photophysics; radical materials 25 7 2024 2024-07-25 10.1002/adma.202402790 COLLEGE NANME Engineering and Applied Sciences School COLLEGE CODE EAAS Swansea University SU Library paid the OA fee (TA Institutional Deal) Cambridge Trust; China Scholarship Council - 201808060075; Engineering and Physical Sciences Research Council - EP/M005143/1; Engineering and Physical Sciences Research Council - EP/W018519/1; Engineering and Physical Sciences Research Council - EP/S022953/1; H2020 European Research Council - 101020167; National Natural Science Foundation of China - 2019TD-33; National Natural Science Foundation of China - 51925303; Royal Society - URF\R1\201300; Simons Foundation - 601946 2024-11-01T14:06:59.6426721 2024-06-03T12:31:22.5695707 Faculty of Science and Engineering School of Engineering and Applied Sciences - Chemistry Qinying Gu 1 Sebastian Gorgon 2 Alexander S. Romanov 3 Feng Li 4 Richard H. Friend 5 Emrys Evans 0000-0002-9092-3938 6 66573__30685__81a9192eabb34bb5a8ac40c9fa841952.pdf 66573.VOR.pdf 2024-06-19T16:14:56.7356239 Output 2110836 application/pdf Version of Record true true eng http://creativecommons.org/licenses/by/4.0/
title Fast Transfer of Triplet to Doublet Excitons from Organometallic Host to Organic Radical Semiconductors
spellingShingle Fast Transfer of Triplet to Doublet Excitons from Organometallic Host to Organic Radical Semiconductors
Emrys Evans
title_short Fast Transfer of Triplet to Doublet Excitons from Organometallic Host to Organic Radical Semiconductors
title_full Fast Transfer of Triplet to Doublet Excitons from Organometallic Host to Organic Radical Semiconductors
title_fullStr Fast Transfer of Triplet to Doublet Excitons from Organometallic Host to Organic Radical Semiconductors
title_full_unstemmed Fast Transfer of Triplet to Doublet Excitons from Organometallic Host to Organic Radical Semiconductors
title_sort Fast Transfer of Triplet to Doublet Excitons from Organometallic Host to Organic Radical Semiconductors
author_id_str_mv 538e217307dac24c9642ef1b03b41485
author_id_fullname_str_mv 538e217307dac24c9642ef1b03b41485_***_Emrys Evans
author Emrys Evans
author2 Qinying Gu
Sebastian Gorgon
Alexander S. Romanov
Feng Li
Richard H. Friend
Emrys Evans
format Journal article
container_title Advanced Materials
container_volume 36
container_issue 30
container_start_page 2402790
publishDate 2024
institution Swansea University
issn 0935-9648
1521-4095
doi_str_mv 10.1002/adma.202402790
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 - Chemistry{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Chemistry
document_store_str 1
active_str 0
description Spin triplet exciton formation sets limits on technologies using organic semiconductors that are confined to singlet-triplet photophysics. In contrast, excitations in the spin doublet manifold in organic radical semiconductors can show efficient luminescence. Here we explore the dynamics of the spin allowed process of intermolecular energy transfer from triplet to doublet excitons. We employ a carbene-metal-amide (CMA-CF3) as a model triplet donor host, since following photoexcitation it undergoes extremely fast intersystem crossing to set up a population of triplet excitons within 4 ps. This enables a foundational study for tracking energy transfer from triplets to a model radical semiconductor, TTM-3PCz. Over 74% of all radical luminescence originates from the triplet channel in this system under photoexcitation. We find that intermolecular triplet-to-doublet energy transfer can occur directly and rapidly, with 12% of triplet excitons transferring already on sub-ns timescales. This enhanced triplet harvesting mechanism is utilised in efficient near-infrared organic light-emitting diodes, which can be extended to other opto-electronic and -spintronic technologies by radical-based spin control in molecular semiconductors.
published_date 2024-07-25T08:31:05Z
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