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Electron spin resonance resolves intermediate triplet states in delayed fluorescence

Author

Listed:
  • Bluebell H. Drummond

    (University of Cambridge
    University of Oxford, Inorganic Chemistry Laboratory)

  • Naoya Aizawa

    (RIKEN Center for Emergent Matter Science (CEMS))

  • Yadong Zhang

    (Georgia Institute of Technology)

  • William K. Myers

    (University of Oxford, Inorganic Chemistry Laboratory)

  • Yao Xiong

    (Georgia Institute of Technology)

  • Matthew W. Cooper

    (Georgia Institute of Technology)

  • Stephen Barlow

    (Georgia Institute of Technology)

  • Qinying Gu

    (University of Cambridge)

  • Leah R. Weiss

    (University of Cambridge
    University of Chicago)

  • Alexander J. Gillett

    (University of Cambridge)

  • Dan Credgington

    (University of Cambridge)

  • Yong-Jin Pu

    (RIKEN Center for Emergent Matter Science (CEMS))

  • Seth R. Marder

    (Georgia Institute of Technology)

  • Emrys W. Evans

    (University of Cambridge
    Swansea University)

Abstract

Molecular organic fluorophores are currently used in organic light-emitting diodes, though non-emissive triplet excitons generated in devices incorporating conventional fluorophores limit the efficiency. This limit can be overcome in materials that have intramolecular charge-transfer excitonic states and associated small singlet-triplet energy separations; triplets can then be converted to emissive singlet excitons resulting in efficient delayed fluorescence. However, the mechanistic details of the spin interconversion have not yet been fully resolved. We report transient electron spin resonance studies that allow direct probing of the spin conversion in a series of delayed fluorescence fluorophores with varying energy gaps between local excitation and charge-transfer triplet states. The observation of distinct triplet signals, unusual in transient electron spin resonance, suggests that multiple triplet states mediate the photophysics for efficient light emission in delayed fluorescence emitters. We reveal that as the energy separation between local excitation and charge-transfer triplet states decreases, spin interconversion changes from a direct, singlet-triplet mechanism to an indirect mechanism involving intermediate states.

Suggested Citation

  • 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.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-24612-9
    DOI: 10.1038/s41467-021-24612-9
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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. Sinyeong Jung & Wai-Lung Cheung & Si-jie Li & Min Wang & Wansi Li & Cangyu Wang & Xiaoge Song & Guodan Wei & Qinghua Song & Season Si Chen & Wanqing Cai & Maggie Ng & Wai Kit Tang & Man-Chung Tang, 2023. "Enhancing operational stability of OLEDs based on subatomic modified thermally activated delayed fluorescence compounds," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    3. Lei Hua & Yuchao Liu & Binbin Liu & Zhennan Zhao & Lei Zhang & Shouke Yan & Zhongjie Ren, 2022. "Constructing high-efficiency orange-red thermally activated delayed fluorescence emitters by three-dimension molecular engineering," Nature Communications, Nature, vol. 13(1), pages 1-11, December.

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