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Proof of crystal-field-perturbation-enhanced luminescence of lanthanide-doped nanocrystals through interstitial H+ doping.
- Source :
- Nature Communications; 9/21/2023, Vol. 14 Issue 1, p1-12, 12p
- Publication Year :
- 2023
-
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>â</superscript> ligand, which affects the highly symmetric Ln<superscript>3+</superscript>-substituted [MgF<subscript>6</subscript>]<superscript>4â</superscript> octahedral clusters. This effectively alleviates the parity-forbidden selective rule to enhance the 4fâ4 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. Lanthanide-doped inorganic nanocrystals are promising for optical imaging and biomedical applications. Here authors show that interstitial H<superscript>+</superscript> doping-induced crystal-field perturbation enhances the photoluminescence intensity of lanthanide-doped inorganic nanocrystals. [ABSTRACT FROM AUTHOR]
- Subjects :
- NANOCRYSTALS
RARE earth metals
LUMINESCENCE
DIAGNOSTIC imaging
RADIATIVE transitions
Subjects
Details
- Language :
- English
- ISSN :
- 20411723
- Volume :
- 14
- Issue :
- 1
- Database :
- Complementary Index
- Journal :
- Nature Communications
- Publication Type :
- Academic Journal
- Accession number :
- 172284928
- Full Text :
- https://doi.org/10.1038/s41467-023-41411-6