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High Relaxivities and Strong Vascular Signal Enhancement for NaGdF4 Nanoparticles Designed for Dual MR/Optical Imaging

Authors

  • Rafik Naccache,

    1. Department of Chemistry and Biochemistry and Centre for NanoScience Research, Concordia University, Montréal, Québec, H4B 1R6, Canada
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  • Pascale Chevallier,

    1. Centre de recherche du Centre hospitalier universitaire de, Québec (CR-CHUQ), Québec, G1L 3L5, Canada
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  • Jean Lagueux,

    1. Centre de recherche du Centre hospitalier universitaire de, Québec (CR-CHUQ), Québec, G1L 3L5, Canada
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  • Yves Gossuin,

    1. Service de physique expérimentale et biologique, Université de Mons, Mons, B7000, Belgium
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  • Sophie Laurent,

    1. Service de chimie générale, organique et biomédicale, Université de Mons, Mons, B7000, Belgium
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  • Luce Vander Elst,

    1. Service de chimie générale, organique et biomédicale, Université de Mons, Mons, B7000, Belgium
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  • Cornelia Chilian,

    1. Ecole Polytechnique de Montréal, Montréal, Québec, H3T 1J4, Canada
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  • John A. Capobianco,

    Corresponding author
    1. Department of Chemistry and Biochemistry and Centre for NanoScience Research, Concordia University, Montréal, Québec, H4B 1R6, Canada
    • John A. Capobianco, Department of Chemistry and Biochemistry and Centre for NanoScience Research, Concordia University, Montréal, Québec, H4B 1R6, Canada

      Marc-André Fortin, Centre de recherche du Centre hospitalier universitaire de Québec, (CR-CHUQ), Québec, G1L 3L5, Canada, Département de génie des mines, de la métallurgie et des matériaux and Centre de recherche sur, les matériaux avancés (CERMA), Université Laval, Québec, G1V 0A6, Canada.

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  • Marc-André Fortin

    Corresponding author
    1. Centre de recherche du Centre hospitalier universitaire de Québec, (CR-CHUQ), Québec, G1L 3L5, Canada, Département de génie des mines, de la métallurgie et des matériaux and Centre de recherche sur, les matériaux avancés (CERMA), Université Laval, Québec, G1V 0A6, Canada
    • John A. Capobianco, Department of Chemistry and Biochemistry and Centre for NanoScience Research, Concordia University, Montréal, Québec, H4B 1R6, Canada

      Marc-André Fortin, Centre de recherche du Centre hospitalier universitaire de Québec, (CR-CHUQ), Québec, G1L 3L5, Canada, Département de génie des mines, de la métallurgie et des matériaux and Centre de recherche sur, les matériaux avancés (CERMA), Université Laval, Québec, G1V 0A6, Canada.

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Abstract

Near-infrared (NIR)-to-NIR upconverting NaY(Gd)F4:Tm3+,Yb3+ paramagnetic nanoparticles (NPs) are efficiently detected by NIR imaging techniques. As they contain Gd3+ ions, they also provide efficient “positive” contrast in magnetic resonance imaging (MRI). Water-dispersible small (≈25 nm, “S-”) and ultrasmall (<5 nm diam., “US-”) NaY(Gd)F4:Tm3+,Yb3+ NPs are synthesized by thermal decomposition and capped with citrate. The surface of citrate-coated US-NPs shows sodium depletion and high Gd elemental ratios, as confirmed by a comparative X-ray photoelectron spectroscopy (XPS)/neutron absorption analysis study. US-NaGd0.745F4:Tm0.005,Yb0.25 NPs have hydrodynamic diameters close to that measured by TEM, with the lowest relaxometric ratios (r2/r1 = 1.18) reported for NaGdF4 nanoparticle suspensions (r1 = 3.37 mM−1 s−1 at 1.4 T and 37 °C). Strong relaxivity peaks in the range of 20 (0.47 T) - 300 MHz (7.05 T) are revealed in nuclear magnetic resonance dispersion profiles, with high r2/r1 ratios at increasing field strengths for S-NPs. This indicates the superiority of US-NPs over S-NPs for achieving high positive contrast at clinical MRI field strengths. I.-v. injected citrate-coated US-NPs evidence long blood retention times (>90 min) in mice. Biodistribution studies (48 h, 8 d) show elimination through the reticuloendothelial and urinary systems, similarly to other citrate-capped US-NP systems. In summary, upconverting NaY(Gd)F4:Tm3+,Yb3+ nanoparticles have promising luminescent, relaxometric and blood-retention properties for dual MRI/optical imaging.

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