NDLI: Self-Aggregated Dinuclear Lanthanide(III) Complexes as Potential Bimodal Probes for Magnetic Resonance and Optical Imaging

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Self-Aggregated Dinuclear Lanthanide(III) Complexes as Potential Bimodal Probes for Magnetic Resonance and Optical Imaging

Content Provider	World Health Organization (WHO)-Global Index Medicus
Author	Charbonnière, Loïc J. De Blas, Andrés Nonat, Aline Esteban-gómez, David Platas-iglesias, Carlos Rolla, Gabriele A. Rodríguez-blas, Teresa Regueiro-figueroa, Martín Botta, Mauro
Description	Author Affiliation: Regueiro-Figueroa M ( Departamento de Química Fundamental, Universidade da Coruña, Campus da Zapateira, Rúa da Fraga 10, 15008A Coruña, Spain.)
Abstract	Homodinuclear lanthanide complexes (Ln=La, Eu, Gd, Tb, Yb and Lu) derived from a bis-macrocyclic ligand featuring two 2,2′,2′′-(1,4,7,10-tetraazacyclododecane-1,4,7-triyl)triacetic acid chelating sites linked by a 2,6-bis(pyrazol-1-yl)pyridine spacer $(H_{2}L^{3})$ were prepared and characterized. Luminescence lifetime measurements recorded on solutions of the $Eu^{III}$ and $Tb^{III}$ complexes indicate the presence of one inner-sphere water molecule coordinated to each metal ion in these complexes. The overall luminescence quantum yields were determined (ϕ=0.01 for $[Eu_{2}(L^{3})]$ and 0.50 for $[Tb_{2}(L^{3})]$ in 0.01 M TRIS/HCl, pH 7.4; TRIS=tris(hydroxymethyl)aminomethane), pointing to an effective sensitization of the metal ion by the bispyrazolylpyridyl unit of the ligand, especially with Tb. The nuclear magnetic relaxation dispersion (NMRD) profiles recorded for $[Gd_{2}(L^{3})]$ are characteristic of slowly tumbling systems, showing a low-field plateau and a broad maximum around 30 MHz. This suggests the occurrence of aggregation of the complexes giving rise to slowly rotating species. A similar behavior is observed for the analogous $Gd^{III}$ complex containing a 4,4′-dimethyl-2,2′-bipyridyl spacer $([Gd_{2}(L^{1})]).$ The relaxivity of $[Gd_{2}(L^{3})]$ recorded at 0.5 T and 298 K (pH 6.9) amounts to $13.7 mM^{−1} s^{−1}.$ The formation of aggregates has been confirmed by dynamic light scattering (DLS) experiments, which provided mean particle sizes of 114 and 38 nm for $[Gd_{2}(L^{1})]$ and $[Gd_{2}(L^{3})],$ respectively. TEM images of $[Gd_{2}(L^{3})]$ indicate the formation of nearly spherical nanosized aggregates with a mean diameter of about 41 nm, together with some nonspherical particles with larger size.
ISSN	09476539
e-ISSN	15213765
Journal	Chemistry - A European Journal
Issue Number	35
Volume Number	19
Language	English
Publisher	Wiley-VCH;ChemPubSoc Europe
Publisher Date	2013-08-26
Publisher Place	Germany
Access Restriction	Open
Subject Keyword	Chemistry
Content Type	Text
Resource Type	Article
Subject	Organic Chemistry Catalysis

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