E-Thesis 421 views 875 downloads
Design of Radical Materials and Systems Towards Opto-Spintronics / JOHN HUDSON
Swansea University Author: JOHN HUDSON
-
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...
| 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 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.</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 – 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 |

