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Multiphoton excited singlet/triplet mixed self-trapped exciton emission

Author

Listed:
  • Rui Zhou

    (Zhengzhou University)

  • Laizhi Sui

    (Chinese Academy of Sciences)

  • Xinbao Liu

    (Chinese Academy of Sciences)

  • Kaikai Liu

    (Zhengzhou University)

  • Dengyang Guo

    (Zhengzhou University
    University of Cambridge)

  • Wenbo Zhao

    (Zhengzhou University)

  • Shiyu Song

    (Zhengzhou University)

  • Chaofan Lv

    (Zhengzhou University)

  • Shu Chen

    (Zhengzhou University)

  • Tianci Jiang

    (The First Affiliated Hospital of Zhengzhou University
    Henan Key Laboratory for Pharmacology of Liver Diseases)

  • Zhe Cheng

    (The First Affiliated Hospital of Zhengzhou University
    Henan Key Laboratory for Pharmacology of Liver Diseases)

  • Sheng Meng

    (Chinese Academy of Sciences)

  • Chongxin Shan

    (Zhengzhou University)

Abstract

Multiphoton excited luminescence is of paramount importance in the field of optical detection and biological photonics. Self-trapped exciton (STE) emission with self-absorption-free advantages provide a choice for multiphoton excited luminescence. Herein, multiphoton excited singlet/triplet mixed STE emission with a large full width at half-maximum (617 meV) and Stokes shift (1.29 eV) has been demonstrated in single-crystalline ZnO nanocrystals. Temperature dependent steady state, transient state and time-resolved electron spin resonance spectra demonstrate a mixture of singlet (63%) and triplet (37%) mixed STE emission, which contributes to a high photoluminescence quantum yield (60.5%). First-principles calculations suggest 48.34 meV energy per exciton stored by phonons in the distorted lattice of excited states, and 58 meV singlet-triplet splitting energy for the nanocrystals being consistent with the experimental measurements. The model clarifies long and controversial debates on ZnO emission in visible region, and the multiphoton excited singlet/triplet mixed STE emission is also observed.

Suggested Citation

  • Rui Zhou & Laizhi Sui & Xinbao Liu & Kaikai Liu & Dengyang Guo & Wenbo Zhao & Shiyu Song & Chaofan Lv & Shu Chen & Tianci Jiang & Zhe Cheng & Sheng Meng & Chongxin Shan, 2023. "Multiphoton excited singlet/triplet mixed self-trapped exciton emission," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-36958-3
    DOI: 10.1038/s41467-023-36958-3
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