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Understanding of complex spin up-conversion processes in charge-transfer-type organic molecules

Author

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  • Hyung Suk Kim

    (Kyushu University
    Kyushu University)

  • Sang Hoon Lee

    (Kyushu University)

  • Seunghyup Yoo

    (Korea Advanced Institute of Science and Technology (KAIST))

  • Chihaya Adachi

    (Kyushu University
    Kyushu University
    Kyushu University)

Abstract

Despite significant progress made over the past decade in thermally activated delayed fluorescence (TADF) molecules as a material paradigm for enhancing the performance of organic light-emitting diodes, the underlying spin-flip mechanism in these charge-transfer (CT)-type molecular systems remains an enigma, even since its initial report in 2012. While the initial and final electronic states involved in spin-flip between the lowest singlet and lowest triplet excited states are well understood, the exact dynamic processes and the role of intermediate high-lying triplet (T) states are still not fully comprehended. In this context, we propose a comprehensive model to describe the spin-flip processes applicable for a typical CT-type molecule, revealing the origin of the high-lying T state in a partial molecular framework in CT-type molecules. This work provides experimental and theoretical insights into the understanding of intersystem crossing for CT-type molecules, facilitating more precise control over spin-flip rates and thus advancing toward developing the next-generation platform for purely organic luminescent candidates.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-46406-5
    DOI: 10.1038/s41467-024-46406-5
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    References listed on IDEAS

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    1. Bluebell H. Drummond & Naoya Aizawa & Yadong Zhang & William K. Myers & Yao Xiong & Matthew W. Cooper & Stephen Barlow & Qinying Gu & Leah R. Weiss & Alexander J. Gillett & Dan Credgington & Yong-Jin , 2021. "Electron spin resonance resolves intermediate triplet states in delayed fluorescence," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    2. Naoya Aizawa & Yu Harabuchi & Satoshi Maeda & Yong-Jin Pu, 2020. "Kinetic prediction of reverse intersystem crossing in organic donor–acceptor molecules," Nature Communications, Nature, vol. 11(1), pages 1-6, December.
    3. 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.
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    Cited by:

    1. Suman Kuila & Hector Miranda-Salinas & Julien Eng & Chunyong Li & Martin R. Bryce & Thomas J. Penfold & Andrew P. Monkman, 2024. "Rigid and planar π-conjugated molecules leading to long-lived intramolecular charge-transfer states exhibiting thermally activated delayed fluorescence," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

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