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Proof of crystal-field-perturbation-enhanced luminescence of lanthanide-doped nanocrystals through interstitial H + doping.
- Source :
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Nature communications [Nat Commun] 2023 Sep 21; Vol. 14 (1), pp. 5870. Date of Electronic Publication: 2023 Sep 21. - Publication Year :
- 2023
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Abstract
- Crystal-field perturbation is theoretically the most direct and effective method of achieving highly efficient photoluminescence from trivalent lanthanide (Ln <superscript>3+</superscript> ) 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 <superscript>3+</superscript> -doped luminescent nanocrystals (NCs). Herein, we report crystal-field perturbation through interstitial H <superscript>+</superscript> -doping in orthorhombic-phase NaMgF <subscript>3</subscript> :Ln <superscript>3+</superscript> NCs and achieve a three-orders-of-magnitude emission amplification without a distinct lattice distortion. Mechanistic studies reveal that the interstitial H <superscript>+</superscript> ions perturb the local charge density distribution, leading to anisotropic polarization of the F <superscript>-</superscript> ligand, which affects the highly symmetric Ln <superscript>3+</superscript> -substituted [MgF <subscript>6</subscript> ] <superscript>4-</superscript> octahedral clusters. This effectively alleviates the parity-forbidden selective rule to enhance the 4f-4 f radiative transition rate of the Ln <superscript>3+</superscript> emitter and is directly corroborated by the apparent shortening of the radiative recombination lifetime. The interstitially H <superscript>+</superscript> -doped NaMgF <subscript>3</subscript> :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 Ln <superscript>3+</superscript> -doped luminescent NCs with high brightness.<br /> (© 2023. Springer Nature Limited.)
Details
- Language :
- English
- ISSN :
- 2041-1723
- Volume :
- 14
- Issue :
- 1
- Database :
- MEDLINE
- Journal :
- Nature communications
- Publication Type :
- Academic Journal
- Accession number :
- 37735451
- Full Text :
- https://doi.org/10.1038/s41467-023-41411-6