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


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.

SUBMITTER: Li G 

PROVIDER: S-EPMC10514317 | biostudies-literature | 2023 Sep

REPOSITORIES: biostudies-literature

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Proof of crystal-field-perturbation-enhanced luminescence of lanthanide-doped nanocrystals through interstitial H<sup>+</sup> doping.

Li Guowei G   Jiang Shihui S   Liu Aijun A   Ye Lixiang L   Ke Jianxi J   Liu Caiping C   Chen Lian L   Liu Yongsheng Y   Hong Maochun M  

Nature communications 20230921 1


Crystal-field perturbation is theoretically the most direct and effective method of achieving highly efficient photoluminescence from trivalent lanthanide (Ln<sup>3+</sup>) 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 Ln<sup>3+</sup>-doped luminescent nanocrystals (NCs). Herein, we report crystal-field perturbation through interstitial H<sup>+</sup>-doping in orthorhombi  ...[more]

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