No Cover Image

E-Thesis 421 views 875 downloads

Design of Radical Materials and Systems Towards Opto-Spintronics / JOHN HUDSON

Swansea University Author: JOHN HUDSON

  • 2024_Hudson_J.final.69268.pdf

    PDF | E-Thesis – open access

    Copyright: The Author, John Hudson, 2024 Distributed under the terms of a Creative Commons Attribution 4.0 License (CC BY 4.0).

    Download (27.44MB)

DOI (Published version): 10.23889/SUThesis.69268

Abstract

Luminescent organic radicals can exploit optical transitions between doublet-spinground and excited states for which potential applications are being explored in more efficient organic light-emitting diodes (OLEDs). In this thesis we investigate how the unpaired electron in radicals enable fundamental...

Full description

Published: Swansea University, Wales, UK 2025
Institution: Swansea University
Degree level: Doctoral
Degree name: Ph.D
Supervisor: Evans, E.W., and Meredith, P.
URI: https://cronfa.swan.ac.uk/Record/cronfa69268
first_indexed 2025-04-10T14:02:25Z
last_indexed 2025-04-11T05:22:36Z
id cronfa69268
recordtype RisThesis
fullrecord <?xml version="1.0"?><rfc1807><datestamp>2025-04-10T15:05:47.7070204</datestamp><bib-version>v2</bib-version><id>69268</id><entry>2025-04-10</entry><title>Design of Radical Materials and Systems Towards Opto-Spintronics</title><swanseaauthors><author><sid>e6ac8b633e4b6759a04f23ef5c7940af</sid><firstname>JOHN</firstname><surname>HUDSON</surname><name>JOHN HUDSON</name><active>true</active><ethesisStudent>false</ethesisStudent></author></swanseaauthors><date>2025-04-10</date><abstract>Luminescent organic radicals can exploit optical transitions between doublet-spinground and excited states for which potential applications are being explored in more e&#xFB03;cient organic light-emitting diodes (OLEDs). In this thesis we investigate how the unpaired electron in radicals enable fundamental mechanisms for energy and spin control that could be used in future optoelectronic and opto-spintronic technologies. The design of photon- spin mechanisms towards target functions requires understanding of how the &#x2018;extra spin&#x2019; of radicals a&#xFB00;ects their optical, spin and magnetic properties. Here we study the emergent photo- and spin physics from pairing known closed-shell organic molecules with luminescent open-shell radicals. Following a description of the photophysical mechanisms and magnetic interactions of closed-shell and open-shell molecular species, we set out a re- view on the use of radicals as emissive components in optoelectronics. We then explore the potential of exploiting reversible energy transfer between triplet and doublet states to establish magnetosensitive luminescence and spin polarisation. This is followed by experimental work combining the organometallic deep-blue phosphor FIr6 with the &#x2018;fruit-&#xFB02;y&#x2019; TTM-1Cz radical. F&#xF6;rster-mediated triplet-doublet energy transfer with nanosecond life-time ( = 3.1 &#xD7; 107 s&#x2212;1), high e&#xFB03;ciency (85 &#xB1; 25%), and without the need for tripletdi&#xFB00;usion in &#xFB01;lm blends is demonstrated. Finally, we explore the magnetosensitivity of systems involving energy transfer between radical doublet and acene triplet species. From photophysical and spin-resonance analysis, we focus on the interaction of doublet states with paramagnetic triplet species towards establishing design rules for applications that span from OLEDs to &#x2018;spin sensitisers&#x2019; and magnetic-&#xFB01;eld inclination sensors.</abstract><type>E-Thesis</type><journal/><volume/><journalNumber/><paginationStart/><paginationEnd/><publisher/><placeOfPublication>Swansea University, Wales, UK</placeOfPublication><isbnPrint/><isbnElectronic/><issnPrint/><issnElectronic/><keywords>Photophysics and Spin Physics of Organic Semiconductors, Spin Chemistry, Quantum Information Science, Spintronics, Functional Materials, Molecular Design</keywords><publishedDay>6</publishedDay><publishedMonth>2</publishedMonth><publishedYear>2025</publishedYear><publishedDate>2025-02-06</publishedDate><doi>10.23889/SUThesis.69268</doi><url/><notes/><college>COLLEGE NANME</college><CollegeCode>COLLEGE CODE</CollegeCode><institution>Swansea University</institution><supervisor>Evans, E.W., and Meredith, P.</supervisor><degreelevel>Doctoral</degreelevel><degreename>Ph.D</degreename><apcterm/><funders/><projectreference/><lastEdited>2025-04-10T15:05:47.7070204</lastEdited><Created>2025-04-10T14:56:37.2279262</Created><path><level id="1">Faculty of Science and Engineering</level><level id="2">School of Engineering and Applied Sciences - Chemistry</level></path><authors><author><firstname>JOHN</firstname><surname>HUDSON</surname><order>1</order></author></authors><documents><document><filename>69268__34005__d731c1c1a30444cca060150764657daa.pdf</filename><originalFilename>2024_Hudson_J.final.69268.pdf</originalFilename><uploaded>2025-04-10T15:01:37.1070871</uploaded><type>Output</type><contentLength>28769563</contentLength><contentType>application/pdf</contentType><version>E-Thesis &#x2013; open access</version><cronfaStatus>true</cronfaStatus><documentNotes>Copyright: The Author, John Hudson, 2024 Distributed under the terms of a Creative Commons Attribution 4.0 License (CC BY 4.0).</documentNotes><copyrightCorrect>true</copyrightCorrect><language>eng</language><licence>https://creativecommons.org/licenses/by/4.0/</licence></document></documents><OutputDurs/></rfc1807>
spelling 2025-04-10T15:05:47.7070204 v2 69268 2025-04-10 Design of Radical Materials and Systems Towards Opto-Spintronics e6ac8b633e4b6759a04f23ef5c7940af JOHN HUDSON JOHN HUDSON true false 2025-04-10 Luminescent organic radicals can exploit optical transitions between doublet-spinground and excited states for which potential applications are being explored in more efficient organic light-emitting diodes (OLEDs). In this thesis we investigate how the unpaired electron in radicals enable fundamental mechanisms for energy and spin control that could be used in future optoelectronic and opto-spintronic technologies. The design of photon- spin mechanisms towards target functions requires understanding of how the ‘extra spin’ of radicals affects their optical, spin and magnetic properties. Here we study the emergent photo- and spin physics from pairing known closed-shell organic molecules with luminescent open-shell radicals. Following a description of the photophysical mechanisms and magnetic interactions of closed-shell and open-shell molecular species, we set out a re- view on the use of radicals as emissive components in optoelectronics. We then explore the potential of exploiting reversible energy transfer between triplet and doublet states to establish magnetosensitive luminescence and spin polarisation. This is followed by experimental work combining the organometallic deep-blue phosphor FIr6 with the ‘fruit-fly’ TTM-1Cz radical. Förster-mediated triplet-doublet energy transfer with nanosecond life-time ( = 3.1 × 107 s−1), high efficiency (85 ± 25%), and without the need for tripletdiffusion in film blends is demonstrated. Finally, we explore the magnetosensitivity of systems involving energy transfer between radical doublet and acene triplet species. From photophysical and spin-resonance analysis, we focus on the interaction of doublet states with paramagnetic triplet species towards establishing design rules for applications that span from OLEDs to ‘spin sensitisers’ and magnetic-field inclination sensors. E-Thesis Swansea University, Wales, UK Photophysics and Spin Physics of Organic Semiconductors, Spin Chemistry, Quantum Information Science, Spintronics, Functional Materials, Molecular Design 6 2 2025 2025-02-06 10.23889/SUThesis.69268 COLLEGE NANME COLLEGE CODE Swansea University Evans, E.W., and Meredith, P. Doctoral Ph.D 2025-04-10T15:05:47.7070204 2025-04-10T14:56:37.2279262 Faculty of Science and Engineering School of Engineering and Applied Sciences - Chemistry JOHN HUDSON 1 69268__34005__d731c1c1a30444cca060150764657daa.pdf 2024_Hudson_J.final.69268.pdf 2025-04-10T15:01:37.1070871 Output 28769563 application/pdf E-Thesis – open access true Copyright: The Author, John Hudson, 2024 Distributed under the terms of a Creative Commons Attribution 4.0 License (CC BY 4.0). true eng https://creativecommons.org/licenses/by/4.0/
title Design of Radical Materials and Systems Towards Opto-Spintronics
spellingShingle Design of Radical Materials and Systems Towards Opto-Spintronics
JOHN HUDSON
title_short Design of Radical Materials and Systems Towards Opto-Spintronics
title_full Design of Radical Materials and Systems Towards Opto-Spintronics
title_fullStr Design of Radical Materials and Systems Towards Opto-Spintronics
title_full_unstemmed Design of Radical Materials and Systems Towards Opto-Spintronics
title_sort Design of Radical Materials and Systems Towards Opto-Spintronics
author_id_str_mv e6ac8b633e4b6759a04f23ef5c7940af
author_id_fullname_str_mv e6ac8b633e4b6759a04f23ef5c7940af_***_JOHN HUDSON
author JOHN HUDSON
author2 JOHN HUDSON
format E-Thesis
publishDate 2025
institution Swansea University
doi_str_mv 10.23889/SUThesis.69268
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 Luminescent organic radicals can exploit optical transitions between doublet-spinground and excited states for which potential applications are being explored in more efficient organic light-emitting diodes (OLEDs). In this thesis we investigate how the unpaired electron in radicals enable fundamental mechanisms for energy and spin control that could be used in future optoelectronic and opto-spintronic technologies. The design of photon- spin mechanisms towards target functions requires understanding of how the ‘extra spin’ of radicals affects their optical, spin and magnetic properties. Here we study the emergent photo- and spin physics from pairing known closed-shell organic molecules with luminescent open-shell radicals. Following a description of the photophysical mechanisms and magnetic interactions of closed-shell and open-shell molecular species, we set out a re- view on the use of radicals as emissive components in optoelectronics. We then explore the potential of exploiting reversible energy transfer between triplet and doublet states to establish magnetosensitive luminescence and spin polarisation. This is followed by experimental work combining the organometallic deep-blue phosphor FIr6 with the ‘fruit-fly’ TTM-1Cz radical. Förster-mediated triplet-doublet energy transfer with nanosecond life-time ( = 3.1 × 107 s−1), high efficiency (85 ± 25%), and without the need for tripletdiffusion in film blends is demonstrated. Finally, we explore the magnetosensitivity of systems involving energy transfer between radical doublet and acene triplet species. From photophysical and spin-resonance analysis, we focus on the interaction of doublet states with paramagnetic triplet species towards establishing design rules for applications that span from OLEDs to ‘spin sensitisers’ and magnetic-field inclination sensors.
published_date 2025-02-06T05:26:30Z
_version_ 1851369550201749504
score 11.089572