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Polaron pair mediated triplet generation in polymer/fullerene blends

Stoichko Dimitrov Orcid Logo, Scot Wheeler, Dorota Niedzialek, Bob C. Schroeder, Hendrik Utzat, Jarvist M. Frost, Jizhong Yao, Alexander Gillett, Pabitra S. Tuladhar, Iain McCulloch, Jenny Nelson Orcid Logo, James Durrant Orcid Logo

Nature Communications, Volume: 6, Start page: 6501

Swansea University Authors: Stoichko Dimitrov Orcid Logo, Jenny Nelson Orcid Logo, James Durrant Orcid Logo

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DOI (Published version): 10.1038/ncomms7501

Abstract

Electron spin is a key consideration for the function of organic semiconductors in light-emitting diodes and solar cells, as well as spintronic applications relying on organic magnetoresistance. A mechanism for triplet excited state generation in such systems is by recombination of electron-hole pai...

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Published in: Nature Communications
ISSN: 2041-1723 2041-1723
Published: 2015
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URI: https://cronfa.swan.ac.uk/Record/cronfa31796
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A mechanism for triplet excited state generation in such systems is by recombination of electron-hole pairs. However, the exact charge recombination mechanism, whether geminate or nongeminate and whether it involves spin-state mixing is not well understood. In this work, the dynamics of free charge separation competing with recombination to polymer triplet states is studied in two closely related polymer-fullerene blends with differing polymer fluorination and photovoltaic performance. Using time-resolved laser spectroscopic techniques and quantum chemical calculations, we show that lower charge separation in the fluorinated system is associated with the formation of bound electron-hole pairs, which undergo spin-state mixing on the nanosecond timescale and subsequent geminate recombination to triplet excitons. 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spelling 2020-12-18T15:08:18.1171639 v2 31796 2017-01-27 Polaron pair mediated triplet generation in polymer/fullerene blends 9fc26ec1b8655cd0d66f7196a924fe14 0000-0002-1564-7080 Stoichko Dimitrov Stoichko Dimitrov true false e0e41c0bb2b9cae677f7fbbf88abe590 0000-0003-1048-1330 Jenny Nelson Jenny Nelson true false f3dd64bc260e5c07adfa916c27dbd58a 0000-0001-8353-7345 James Durrant James Durrant true false 2017-01-27 EEN Electron spin is a key consideration for the function of organic semiconductors in light-emitting diodes and solar cells, as well as spintronic applications relying on organic magnetoresistance. A mechanism for triplet excited state generation in such systems is by recombination of electron-hole pairs. However, the exact charge recombination mechanism, whether geminate or nongeminate and whether it involves spin-state mixing is not well understood. In this work, the dynamics of free charge separation competing with recombination to polymer triplet states is studied in two closely related polymer-fullerene blends with differing polymer fluorination and photovoltaic performance. Using time-resolved laser spectroscopic techniques and quantum chemical calculations, we show that lower charge separation in the fluorinated system is associated with the formation of bound electron-hole pairs, which undergo spin-state mixing on the nanosecond timescale and subsequent geminate recombination to triplet excitons. We find that these bound electron-hole pairs can be dissociated by electric fields. Journal Article Nature Communications 6 6501 2041-1723 2041-1723 4 3 2015 2015-03-04 10.1038/ncomms7501 The author made a substantial contribution to the conception and design of the study; to the organisation of the conduct of the study; to carrying out the study (including acquisition of study data); to analysis and interpretation of study data. The author helped draft the output. COLLEGE NANME Engineering COLLEGE CODE EEN Swansea University 2020-12-18T15:08:18.1171639 2017-01-27T13:45:51.3783306 Faculty of Science and Engineering School of Engineering and Applied Sciences - Materials Science and Engineering Stoichko Dimitrov 0000-0002-1564-7080 1 Scot Wheeler 2 Dorota Niedzialek 3 Bob C. Schroeder 4 Hendrik Utzat 5 Jarvist M. Frost 6 Jizhong Yao 7 Alexander Gillett 8 Pabitra S. Tuladhar 9 Iain McCulloch 10 Jenny Nelson 0000-0003-1048-1330 11 James Durrant 0000-0001-8353-7345 12 31796__4860__7003f1d7c43447a481cd1957ff03983d.pdf dimitrov2015.pdf 2017-02-21T12:41:41.1270000 Output 726590 application/pdf Version of Record true 2017-02-21T00:00:00.0000000 false eng
title Polaron pair mediated triplet generation in polymer/fullerene blends
spellingShingle Polaron pair mediated triplet generation in polymer/fullerene blends
Stoichko Dimitrov
Jenny Nelson
James Durrant
title_short Polaron pair mediated triplet generation in polymer/fullerene blends
title_full Polaron pair mediated triplet generation in polymer/fullerene blends
title_fullStr Polaron pair mediated triplet generation in polymer/fullerene blends
title_full_unstemmed Polaron pair mediated triplet generation in polymer/fullerene blends
title_sort Polaron pair mediated triplet generation in polymer/fullerene blends
author_id_str_mv 9fc26ec1b8655cd0d66f7196a924fe14
e0e41c0bb2b9cae677f7fbbf88abe590
f3dd64bc260e5c07adfa916c27dbd58a
author_id_fullname_str_mv 9fc26ec1b8655cd0d66f7196a924fe14_***_Stoichko Dimitrov
e0e41c0bb2b9cae677f7fbbf88abe590_***_Jenny Nelson
f3dd64bc260e5c07adfa916c27dbd58a_***_James Durrant
author Stoichko Dimitrov
Jenny Nelson
James Durrant
author2 Stoichko Dimitrov
Scot Wheeler
Dorota Niedzialek
Bob C. Schroeder
Hendrik Utzat
Jarvist M. Frost
Jizhong Yao
Alexander Gillett
Pabitra S. Tuladhar
Iain McCulloch
Jenny Nelson
James Durrant
format Journal article
container_title Nature Communications
container_volume 6
container_start_page 6501
publishDate 2015
institution Swansea University
issn 2041-1723
2041-1723
doi_str_mv 10.1038/ncomms7501
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 - Materials Science and Engineering{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Materials Science and Engineering
document_store_str 1
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description Electron spin is a key consideration for the function of organic semiconductors in light-emitting diodes and solar cells, as well as spintronic applications relying on organic magnetoresistance. A mechanism for triplet excited state generation in such systems is by recombination of electron-hole pairs. However, the exact charge recombination mechanism, whether geminate or nongeminate and whether it involves spin-state mixing is not well understood. In this work, the dynamics of free charge separation competing with recombination to polymer triplet states is studied in two closely related polymer-fullerene blends with differing polymer fluorination and photovoltaic performance. Using time-resolved laser spectroscopic techniques and quantum chemical calculations, we show that lower charge separation in the fluorinated system is associated with the formation of bound electron-hole pairs, which undergo spin-state mixing on the nanosecond timescale and subsequent geminate recombination to triplet excitons. We find that these bound electron-hole pairs can be dissociated by electric fields.
published_date 2015-03-04T03:38:51Z
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