Vibrationally Assisted Intersystem Crossing in Benchmark Thermally Activated Delayed Fluorescence Molecules

Evans, Emrys; Olivier, Yoann; Puttisong, Yuttapoom; Myers, William K.; H., Timothy J.; Menke, S. Matthew; Thomas, Tudor H.; Credgington, Dan; Beljonne, David; Friend, Richard H.; Greenham, Neil C.

doi:10.1021/acs.jpclett.8b01556

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Vibrationally Assisted Intersystem Crossing in Benchmark Thermally Activated Delayed Fluorescence Molecules

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

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...

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Published in:	The Journal of Physical Chemistry Letters
ISSN:	1948-7185 1948-7185
Published:	American Chemical Society (ACS) 2018
Online Access:	Check full text
URI:	https://cronfa.swan.ac.uk/Record/cronfa57572
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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 ́ under Grant Agreement No. 1117545.</funders><lastEdited>2021-09-08T15:44:35.7907723</lastEdited><Created>2021-08-10T09:28:46.7665047</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>Emrys</firstname><surname>Evans</surname><orcid>0000-0002-9092-3938</orcid><order>1</order></author><author><firstname>Yoann</firstname><surname>Olivier</surname><order>2</order></author><author><firstname>Yuttapoom</firstname><surname>Puttisong</surname><order>3</order></author><author><firstname>William K.</firstname><surname>Myers</surname><order>4</order></author><author><firstname>Timothy J. 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spelling	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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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
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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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score	11.013148

Vibrationally Assisted Intersystem Crossing in Benchmark Thermally Activated Delayed Fluorescence Molecules

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