Mechanism of intersystem crossing of thermally activated delayed fluorescence molecules

The Journal of Physical Chemistry. a
Toshinari OgiwaraTadaaki Ikoma

Abstract

The spin sublevel dynamics of the excited triplet state in thermally activated delayed fluorescence (TADF) molecules have not been investigated for high-intensity organic light-emitting diode materials. Understanding the mechanism for intersystem crossing (ISC) is thus important for designing novel TADF materials. We report the first study on the ISC dynamics of the lowest excited triplet state from the lowest excited singlet state with charge-transfer (CT) character of TADF molecules with different external quantum efficiencies (EQEs) using time-resolved electron paramagnetic resonance methods. Analysis of the observed spin polarization indicates a strong correlation of the EQE with the population rate due to ISC induced by hyperfine coupling with the magnetic nuclei. It is concluded that molecules with high EQE have an extremely small energy gap between the (1)CT and (3)CT states, which allows an additional ISC channel due to the hyperfine interactions.

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Citations

Jun 25, 2016·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Jamie GibsonThomas J Penfold
Mar 14, 2017·Physical Chemistry Chemical Physics : PCCP·J Gibson, T J Penfold
Apr 9, 2020·Chemical Record : an Official Publication of the Chemical Society of Japan ... [et Al.]·Julien Eng, Thomas J Penfold
Mar 10, 2017·Methods and Applications in Fluorescence·Fernando B DiasAndrew P Monkman
Dec 3, 2016·Nature Communications·Marc K EtheringtonAndrew P Monkman
Nov 25, 2020·Chemical Society Reviews·Yuwei XuYuguang Ma
Dec 19, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Xue ZhangJianzhang Zhao
Feb 21, 2021·Annual Review of Physical Chemistry·Christel M Marian
Jul 28, 2021·Nature Communications·Bluebell H DrummondEmrys W Evans
Aug 4, 2021·The Journal of Physical Chemistry. a·Bidhan Chandra GarainSwapan K Pati
Jun 30, 2018·The Journal of Physical Chemistry Letters·Emrys W EvansNeil C Greenham
Jul 10, 2019·The Journal of Physical Chemistry Letters·Yuri E KandrashkinJianzhang Zhao
Sep 21, 2021·The Journal of Physical Chemistry. B·Mushraf HussainOmar F Mohammed

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