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Exact Solution of Kinetic Analysis for Thermally Activated Delayed Fluorescence Materials

  • Youichi Tsuchiya*
    Youichi Tsuchiya
    Center for Organic Photonics and Electronics Research (OPERA), Kyushu University, 744, Motooka, Nishi-ku, Fukuoka 819-0395, Japan
    *Email: [email protected]
  • Stefan Diesing
    Stefan Diesing
    Organic Semiconductor Centre, EaStCHEM School of Chemistry, University of St Andrews, Fife, St Andrews KY16 9ST, U.K.
    Organic Semiconductor Centre, SUPA School of Physics and Astronomy, University of St Andrews, Fife, St Andrews KY16 9ST, U.K.
  • Fatima Bencheikh
    Fatima Bencheikh
    Center for Organic Photonics and Electronics Research (OPERA), Kyushu University, 744, Motooka, Nishi-ku, Fukuoka 819-0395, Japan
  • Yoshimasa Wada
    Yoshimasa Wada
    Institute for Chemical Research, Kyoto University, Uji, Kyoto 611-0011, Japan
  • Paloma L. dos Santos
    Paloma L. dos Santos
    Organic Semiconductor Centre, SUPA School of Physics and Astronomy, University of St Andrews, Fife, St Andrews KY16 9ST, U.K.
  • Hironori Kaji
    Hironori Kaji
    Institute for Chemical Research, Kyoto University, Uji, Kyoto 611-0011, Japan
  • Eli Zysman-Colman*
    Eli Zysman-Colman
    Organic Semiconductor Centre, EaStCHEM School of Chemistry, University of St Andrews, Fife, St Andrews KY16 9ST, U.K.
    *Email: [email protected]
  • Ifor D. W. Samuel*
    Ifor D. W. Samuel
    Organic Semiconductor Centre, SUPA School of Physics and Astronomy, University of St Andrews, Fife, St Andrews KY16 9ST, U.K.
    *Email: [email protected]
  • , and 
  • Chihaya Adachi*
    Chihaya Adachi
    Center for Organic Photonics and Electronics Research (OPERA), Kyushu University, 744, Motooka, Nishi-ku, Fukuoka 819-0395, Japan
    International Institute for Carbon Neutral Energy Research (WPI-ICNER), Kyushu University, 744, Motooka, Nishi-ku, Fukuoka 819-0395, Japan
    *Email: [email protected]
Cite this: J. Phys. Chem. A 2021, 125, 36, 8074–8089
Publication Date (Web):September 2, 2021
https://doi.org/10.1021/acs.jpca.1c04056
Copyright © 2021 American Chemical Society

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    Abstract

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    The photophysical analysis of thermally activated delayed fluorescence (TADF) materials has become instrumental for providing insights into their stability and performance, which is not only relevant for organic light-emitting diodes but also for other applications such as sensing, imaging, and photocatalysis. Thus, a deeper understanding of the photophysics underpinning the TADF mechanism is required to push materials design further. Previously reported analyses in the literature of the kinetics of the various processes occurring in a TADF material rely on several a priori assumptions to estimate the rate constants for forward and reverse intersystem crossing. In this report, we demonstrate a method to determine these rate constants using a three-state model together with a steady-state approximation and, importantly, no additional assumptions. Further, we derive the exact rate equations, greatly facilitating a comparison of the TADF properties of structurally diverse emitters and providing a comprehensive understanding of the photophysics of these systems.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpca.1c04056.

    • Typical estimation methods in the literature for kRISC and kISC, several conversion equations from reported to corrected ones, validity of the approximation of kSkp by assuming kSkRISC, relationships of efficiencies between the element and overall ones, several equations for derivation omitted in the main text, detailed exciton distribution, and derivation of rate equations standing on four-state photophysics with the minimum assumptions related to El-Sayed’s and Kasha’s rules (PDF)

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