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

Author

Listed:
  • Marc K. Etherington

    (Durham University)

  • Jamie Gibson

    (School of Chemistry, Newcastle University)

  • Heather F. Higginbotham

    (Durham University)

  • Thomas J. Penfold

    (School of Chemistry, Newcastle University)

  • Andrew P. Monkman

    (Durham University)

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.

Suggested Citation

  • Marc K. Etherington & Jamie Gibson & Heather F. Higginbotham & Thomas J. Penfold & Andrew P. Monkman, 2016. "Revealing the spin–vibronic coupling mechanism of thermally activated delayed fluorescence," Nature Communications, Nature, vol. 7(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:7:y:2016:i:1:d:10.1038_ncomms13680
    DOI: 10.1038/ncomms13680
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    Cited by:

    1. Hyung Suk Kim & Sang Hoon Lee & Seunghyup Yoo & Chihaya Adachi, 2024. "Understanding of complex spin up-conversion processes in charge-transfer-type organic molecules," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    2. Alexander J. Gillett & Claire Tonnelé & Giacomo Londi & Gaetano Ricci & Manon Catherin & Darcy M. L. Unson & David Casanova & Frédéric Castet & Yoann Olivier & Weimin M. Chen & Elena Zaborova & Emrys , 2021. "Spontaneous exciton dissociation enables spin state interconversion in delayed fluorescence organic semiconductors," Nature Communications, Nature, vol. 12(1), pages 1-10, December.

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