Journal article 961 views 88 downloads
Polaron pair mediated triplet generation in polymer/fullerene blends
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
Nature Communications, Volume: 6, Start page: 6501
Swansea University Authors:
Stoichko Dimitrov , Jenny Nelson
, James Durrant
-
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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...
Published in: | Nature Communications |
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ISSN: | 2041-1723 2041-1723 |
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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. We find that these bound electron-hole pairs can be dissociated by electric fields.</abstract><type>Journal Article</type><journal>Nature Communications</journal><volume>6</volume><journalNumber/><paginationStart>6501</paginationStart><paginationEnd/><publisher/><placeOfPublication/><isbnPrint/><isbnElectronic/><issnPrint>2041-1723</issnPrint><issnElectronic>2041-1723</issnElectronic><keywords/><publishedDay>4</publishedDay><publishedMonth>3</publishedMonth><publishedYear>2015</publishedYear><publishedDate>2015-03-04</publishedDate><doi>10.1038/ncomms7501</doi><url/><notes>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.</notes><college>COLLEGE NANME</college><department>Engineering</department><CollegeCode>COLLEGE CODE</CollegeCode><DepartmentCode>EEN</DepartmentCode><institution>Swansea University</institution><apcterm/><lastEdited>2020-12-18T15:08:18.1171639</lastEdited><Created>2017-01-27T13:45:51.3783306</Created><path><level id="1">Faculty of Science and Engineering</level><level id="2">School of Engineering and Applied Sciences - Materials Science and Engineering</level></path><authors><author><firstname>Stoichko</firstname><surname>Dimitrov</surname><orcid>0000-0002-1564-7080</orcid><order>1</order></author><author><firstname>Scot</firstname><surname>Wheeler</surname><order>2</order></author><author><firstname>Dorota</firstname><surname>Niedzialek</surname><order>3</order></author><author><firstname>Bob C.</firstname><surname>Schroeder</surname><order>4</order></author><author><firstname>Hendrik</firstname><surname>Utzat</surname><order>5</order></author><author><firstname>Jarvist M.</firstname><surname>Frost</surname><order>6</order></author><author><firstname>Jizhong</firstname><surname>Yao</surname><order>7</order></author><author><firstname>Alexander</firstname><surname>Gillett</surname><order>8</order></author><author><firstname>Pabitra S.</firstname><surname>Tuladhar</surname><order>9</order></author><author><firstname>Iain</firstname><surname>McCulloch</surname><order>10</order></author><author><firstname>Jenny</firstname><surname>Nelson</surname><orcid>0000-0003-1048-1330</orcid><order>11</order></author><author><firstname>James</firstname><surname>Durrant</surname><orcid>0000-0001-8353-7345</orcid><order>12</order></author></authors><documents><document><filename>31796__4860__7003f1d7c43447a481cd1957ff03983d.pdf</filename><originalFilename>dimitrov2015.pdf</originalFilename><uploaded>2017-02-21T12:41:41.1270000</uploaded><type>Output</type><contentLength>726590</contentLength><contentType>application/pdf</contentType><version>Version of Record</version><cronfaStatus>true</cronfaStatus><embargoDate>2017-02-21T00:00:00.0000000</embargoDate><copyrightCorrect>false</copyrightCorrect><language>eng</language></document></documents><OutputDurs/></rfc1807> |
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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 |
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Journal article |
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Nature Communications |
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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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Faculty of Science and Engineering |
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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 |
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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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1763751736854446080 |
score |
11.021648 |