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Vibrationally Assisted Intersystem Crossing in Benchmark Thermally Activated Delayed Fluorescence Molecules
The Journal of Physical Chemistry Letters, Volume: 9, Issue: 14, Pages: 4053 - 4058
Swansea University Author:
Emrys Evans
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DOI (Published version): 10.1021/acs.jpclett.8b01556
Abstract
Electrically injected charge carriers in organic light-emitting devices (OLEDs) undergo recombination events to form singlet and triplet states in a 1:3 ratio, representing a fundamental hurdle for achieving high quantum efficiency. Dopants based on thermally activated delayed fluorescence (TADF) ha...
Published in: | The Journal of Physical Chemistry Letters |
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ISSN: | 1948-7185 1948-7185 |
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American Chemical Society (ACS)
2018
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URI: | https://cronfa.swan.ac.uk/Record/cronfa57572 |
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<?xml version="1.0"?><rfc1807><datestamp>2021-09-08T15:44:35.7907723</datestamp><bib-version>v2</bib-version><id>57572</id><entry>2021-08-10</entry><title>Vibrationally Assisted Intersystem Crossing in Benchmark Thermally Activated Delayed Fluorescence Molecules</title><swanseaauthors><author><sid>538e217307dac24c9642ef1b03b41485</sid><ORCID>0000-0002-9092-3938</ORCID><firstname>Emrys</firstname><surname>Evans</surname><name>Emrys Evans</name><active>true</active><ethesisStudent>false</ethesisStudent></author></swanseaauthors><date>2021-08-10</date><deptcode>CHEM</deptcode><abstract>Electrically injected charge carriers in organic light-emitting devices (OLEDs) undergo recombination events to form singlet and triplet states in a 1:3 ratio, representing a fundamental hurdle for achieving high quantum efficiency. Dopants based on thermally activated delayed fluorescence (TADF) have emerged as promising candidates for addressing the spin statistics issue in OLEDs. In these materials, reverse singlet–triplet intersystem crossing (rISC) becomes efficient, thereby activating luminescence pathways for weakly emissive triplet states. However, despite a growing consensus that torsional vibrations facilitate spin–orbit-coupling- (SOC-) driven ISC in these molecules, there is a shortage of experimental evidence. We use transient electron spin resonance and theory to show unambiguously that SOC interactions drive spin conversion and that ISC is a dynamic process gated by conformational fluctuations for benchmark carbazolyl–dicyanobenzene TADF emitters.</abstract><type>Journal Article</type><journal>The Journal of Physical Chemistry Letters</journal><volume>9</volume><journalNumber>14</journalNumber><paginationStart>4053</paginationStart><paginationEnd>4058</paginationEnd><publisher>American Chemical Society (ACS)</publisher><placeOfPublication/><isbnPrint/><isbnElectronic/><issnPrint>1948-7185</issnPrint><issnElectronic>1948-7185</issnElectronic><keywords/><publishedDay>19</publishedDay><publishedMonth>7</publishedMonth><publishedYear>2018</publishedYear><publishedDate>2018-07-19</publishedDate><doi>10.1021/acs.jpclett.8b01556</doi><url/><notes/><college>COLLEGE NANME</college><department>Chemistry</department><CollegeCode>COLLEGE CODE</CollegeCode><DepartmentCode>CHEM</DepartmentCode><institution>Swansea University</institution><apcterm>Other</apcterm><funders>E.W.E., N.C.G. and R.H.F. would like to thank the EPSRC for funding (EP/M01083X/1, EP/M005143/1). Y.P. is grateful to The Swedish Research Council VR2015-00436 for a postdoc grant. W.K.M. is supported by the EPSRC grant EP/L011972/ 1 for CAESR (Centre for Advanced Electron Spin Resonance). T.J.H.H. thanks Jesus College, Cambridge, for a Research Fellowship. DJNC acknowledges the Royal Society for a University Research Fellowship. The work in Mons was supported by the European Union’s Horizon 2020 research and innovation program under Grant Agreement No. 646176 (EXTMOS project) and by Belgian National Fund for Scientific Research (FNRS/F.R.S.). Computational resources have been provided by the Consortium des É quipements de Calcul Intensif (CÉ CI), funded by F.R.S.-FNRS under Grant No. 2.5020.11 as well as the Tier-1 supercomputer of the Fedé ration Wallonie-Bruxelles, funded by the Walloon Region ́
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2021-09-08T15:44:35.7907723 v2 57572 2021-08-10 Vibrationally Assisted Intersystem Crossing in Benchmark Thermally Activated Delayed Fluorescence Molecules 538e217307dac24c9642ef1b03b41485 0000-0002-9092-3938 Emrys Evans Emrys Evans true false 2021-08-10 CHEM Electrically injected charge carriers in organic light-emitting devices (OLEDs) undergo recombination events to form singlet and triplet states in a 1:3 ratio, representing a fundamental hurdle for achieving high quantum efficiency. Dopants based on thermally activated delayed fluorescence (TADF) have emerged as promising candidates for addressing the spin statistics issue in OLEDs. In these materials, reverse singlet–triplet intersystem crossing (rISC) becomes efficient, thereby activating luminescence pathways for weakly emissive triplet states. However, despite a growing consensus that torsional vibrations facilitate spin–orbit-coupling- (SOC-) driven ISC in these molecules, there is a shortage of experimental evidence. We use transient electron spin resonance and theory to show unambiguously that SOC interactions drive spin conversion and that ISC is a dynamic process gated by conformational fluctuations for benchmark carbazolyl–dicyanobenzene TADF emitters. Journal Article The Journal of Physical Chemistry Letters 9 14 4053 4058 American Chemical Society (ACS) 1948-7185 1948-7185 19 7 2018 2018-07-19 10.1021/acs.jpclett.8b01556 COLLEGE NANME Chemistry COLLEGE CODE CHEM Swansea University Other E.W.E., N.C.G. and R.H.F. would like to thank the EPSRC for funding (EP/M01083X/1, EP/M005143/1). Y.P. is grateful to The Swedish Research Council VR2015-00436 for a postdoc grant. W.K.M. is supported by the EPSRC grant EP/L011972/ 1 for CAESR (Centre for Advanced Electron Spin Resonance). T.J.H.H. thanks Jesus College, Cambridge, for a Research Fellowship. DJNC acknowledges the Royal Society for a University Research Fellowship. The work in Mons was supported by the European Union’s Horizon 2020 research and innovation program under Grant Agreement No. 646176 (EXTMOS project) and by Belgian National Fund for Scientific Research (FNRS/F.R.S.). Computational resources have been provided by the Consortium des É quipements de Calcul Intensif (CÉ CI), funded by F.R.S.-FNRS under Grant No. 2.5020.11 as well as the Tier-1 supercomputer of the Fedé ration Wallonie-Bruxelles, funded by the Walloon Region ́ under Grant Agreement No. 1117545. 2021-09-08T15:44:35.7907723 2021-08-10T09:28:46.7665047 Faculty of Science and Engineering School of Engineering and Applied Sciences - Chemistry Emrys Evans 0000-0002-9092-3938 1 Yoann Olivier 2 Yuttapoom Puttisong 3 William K. Myers 4 Timothy J. H. Hele 5 S. Matthew Menke 6 Tudor H. Thomas 7 Dan Credgington 8 David Beljonne 9 Richard H. Friend 10 Neil C. Greenham 11 57572__20786__3e3bf66cbbd64b89a6b4279613e25976.pdf 57572.pdf 2021-09-08T15:43:57.0440728 Output 1598175 application/pdf Version of Record true This is an open access article published under a Creative Commons Attribution (CC-BY) License true eng http://pubs.acs.org/page/policy/authorchoice_ccby_termsofuse.html |
title |
Vibrationally Assisted Intersystem Crossing in Benchmark Thermally Activated Delayed Fluorescence Molecules |
spellingShingle |
Vibrationally Assisted Intersystem Crossing in Benchmark Thermally Activated Delayed Fluorescence Molecules Emrys Evans |
title_short |
Vibrationally Assisted Intersystem Crossing in Benchmark Thermally Activated Delayed Fluorescence Molecules |
title_full |
Vibrationally Assisted Intersystem Crossing in Benchmark Thermally Activated Delayed Fluorescence Molecules |
title_fullStr |
Vibrationally Assisted Intersystem Crossing in Benchmark Thermally Activated Delayed Fluorescence Molecules |
title_full_unstemmed |
Vibrationally Assisted Intersystem Crossing in Benchmark Thermally Activated Delayed Fluorescence Molecules |
title_sort |
Vibrationally Assisted Intersystem Crossing in Benchmark Thermally Activated Delayed Fluorescence Molecules |
author_id_str_mv |
538e217307dac24c9642ef1b03b41485 |
author_id_fullname_str_mv |
538e217307dac24c9642ef1b03b41485_***_Emrys Evans |
author |
Emrys Evans |
author2 |
Emrys Evans Yoann Olivier Yuttapoom Puttisong William K. Myers Timothy J. H. Hele S. Matthew Menke Tudor H. Thomas Dan Credgington David Beljonne Richard H. Friend Neil C. Greenham |
format |
Journal article |
container_title |
The Journal of Physical Chemistry Letters |
container_volume |
9 |
container_issue |
14 |
container_start_page |
4053 |
publishDate |
2018 |
institution |
Swansea University |
issn |
1948-7185 1948-7185 |
doi_str_mv |
10.1021/acs.jpclett.8b01556 |
publisher |
American Chemical Society (ACS) |
college_str |
Faculty of Science and Engineering |
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facultyofscienceandengineering |
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Faculty of Science and Engineering |
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facultyofscienceandengineering |
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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 |
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description |
Electrically injected charge carriers in organic light-emitting devices (OLEDs) undergo recombination events to form singlet and triplet states in a 1:3 ratio, representing a fundamental hurdle for achieving high quantum efficiency. Dopants based on thermally activated delayed fluorescence (TADF) have emerged as promising candidates for addressing the spin statistics issue in OLEDs. In these materials, reverse singlet–triplet intersystem crossing (rISC) becomes efficient, thereby activating luminescence pathways for weakly emissive triplet states. However, despite a growing consensus that torsional vibrations facilitate spin–orbit-coupling- (SOC-) driven ISC in these molecules, there is a shortage of experimental evidence. We use transient electron spin resonance and theory to show unambiguously that SOC interactions drive spin conversion and that ISC is a dynamic process gated by conformational fluctuations for benchmark carbazolyl–dicyanobenzene TADF emitters. |
published_date |
2018-07-19T04:13:25Z |
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1763753911166959616 |
score |
11.021648 |