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Proof of crystal-field-perturbation-enhanced luminescence of lanthanide-doped nanocrystals through interstitial H+ doping

Author

Listed:
  • Guowei Li

    (Chinese Academy of Sciences
    University of the Chinese Academy of Sciences)

  • Shihui Jiang

    (Chinese Academy of Sciences
    University of the Chinese Academy of Sciences)

  • Aijun Liu

    (Chinese Academy of Sciences)

  • Lixiang Ye

    (Chinese Academy of Sciences
    University of the Chinese Academy of Sciences
    Fujian Medical University)

  • Jianxi Ke

    (Chinese Academy of Sciences
    Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China)

  • Caiping Liu

    (Chinese Academy of Sciences
    Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China
    Advanced Energy Science and Technology Guangdong Laboratory)

  • Lian Chen

    (Chinese Academy of Sciences)

  • Yongsheng Liu

    (Chinese Academy of Sciences
    University of the Chinese Academy of Sciences
    Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China
    Advanced Energy Science and Technology Guangdong Laboratory)

  • Maochun Hong

    (Chinese Academy of Sciences
    University of the Chinese Academy of Sciences
    Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China
    Advanced Energy Science and Technology Guangdong Laboratory)

Abstract

Crystal-field perturbation is theoretically the most direct and effective method of achieving highly efficient photoluminescence from trivalent lanthanide (Ln3+) ions through breaking the parity-forbidden nature of their 4f-transitions. However, exerting such crystal-field perturbation remains an arduous task even in well-developed Ln3+-doped luminescent nanocrystals (NCs). Herein, we report crystal-field perturbation through interstitial H+-doping in orthorhombic-phase NaMgF3:Ln3+ NCs and achieve a three-orders-of-magnitude emission amplification without a distinct lattice distortion. Mechanistic studies reveal that the interstitial H+ ions perturb the local charge density distribution, leading to anisotropic polarization of the F− ligand, which affects the highly symmetric Ln3+-substituted [MgF6]4− octahedral clusters. This effectively alleviates the parity-forbidden selective rule to enhance the 4f–4 f radiative transition rate of the Ln3+ emitter and is directly corroborated by the apparent shortening of the radiative recombination lifetime. The interstitially H+-doped NaMgF3:Yb/Er NCs are successfully used as bioimaging agents for real-time vascular imaging. These findings provide concrete evidence for crystal-field perturbation effects and promote the design of Ln3+-doped luminescent NCs with high brightness.

Suggested Citation

  • Guowei Li & Shihui Jiang & Aijun Liu & Lixiang Ye & Jianxi Ke & Caiping Liu & Lian Chen & Yongsheng Liu & Maochun Hong, 2023. "Proof of crystal-field-perturbation-enhanced luminescence of lanthanide-doped nanocrystals through interstitial H+ doping," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-41411-6
    DOI: 10.1038/s41467-023-41411-6
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    References listed on IDEAS

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