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Revealing the spin–vibronic coupling mechanism of thermally activated delayed fluorescence

Etherington, Marc K.; Gibson, Jamie; Higginbotham, Heather F.; Penfold, Thomas J.; Monkman, Andrew P.

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Authors

Marc K. Etherington

Jamie Gibson

Heather F. Higginbotham

Thomas J. Penfold



Contributors

Heather Cole dpcq23@durham.ac.uk
Other

Abstract

Knowing the underlying photophysics of thermally activated delayed fluorescence (TADF) allows proper design of high efficiency organic light-emitting diodes. We have proposed a model to describe reverse intersystem crossing (rISC) in donor–acceptor charge transfer molecules, where spin–orbit coupling between singlet and triplet states is mediated by one of the local triplet states of the donor (or acceptor). This second order, vibronically coupled mechanism describes the basic photophysics of TADF. Through a series of measurements, whereby the energy ordering of the charge transfer (CT) excited states and the local triplet are tuned in and out of resonance, we show that TADF reaches a maximum at the resonance point, substantiating our model of rISC. Moreover, using photoinduced absorption, we show how the populations of both singlet and triplet CT states and the local triplet state change in and out of resonance. Our vibronic coupling rISC model is used to predict this behaviour and describes how rISC and TADF are affected by external perturbation.

Citation

Etherington, M. K., Gibson, J., Higginbotham, H. F., Penfold, T. J., & Monkman, A. P. (2016). Revealing the spin–vibronic coupling mechanism of thermally activated delayed fluorescence. Nature Communications, 7, Article 13680. https://doi.org/10.1038/ncomms13680

Journal Article Type Article
Acceptance Date Oct 25, 2016
Online Publication Date Nov 30, 2016
Publication Date Nov 30, 2016
Deposit Date Dec 1, 2016
Publicly Available Date Dec 2, 2016
Journal Nature Communications
Publisher Nature Research
Peer Reviewed Peer Reviewed
Volume 7
Article Number 13680
DOI https://doi.org/10.1038/ncomms13680

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Publisher Licence URL
http://creativecommons.org/licenses/by/4.0/

Copyright Statement
This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/





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