Gd(III) complexes as paramagnetic tags: Evaluation of the spin delocalization over the nuclei of the ligand

Journal of Magnetic Resonance
A CollautoDaniella Goldfarb

Abstract

Complexes of the Gd(III) ion are currently being established as spin labels for distance determination in biomolecules by pulse dipolar spectroscopy. Because Gd(III) is an f ion, one expects electron spin density to be localized on the Gd(III) ion - an important feature for the mentioned application. Most of the complex ligands have nitrogens as Gd(III) coordinating atoms. Therefore, measurement of the (14)N hyperfine coupling gives access to information on the localization of the electron spin on the Gd(III) ion. We carried out W-band, 1D and 2D (14)N and (1)H ENDOR measurements on the Gd(III) complexes Gd-DOTA, Gd-538, Gd-595, and Gd-PyMTA that serve as spin labels for Gd-Gd distance measurements. The obtained (14)N spectra are particularly well resolved, revealing both the hyperfine and nuclear quadrupole splittings, which were assigned using 2D Mims ENDOR experiments. Additionally, the spectral contributions of the two different types of nitrogen atoms of Gd-PyMTA, the aliphatic N atom and the pyridine N atom, were distinguishable. The (14)N hyperfine interaction was found to have a very small isotropic hyperfine component of -0.25 to -0.37MHz. Furthermore, the anisotropic hyperfine interactions with the (14)N nuclei and wi...Continue Reading

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Citations

Mar 21, 2017·Angewandte Chemie·Monu KaushikBjörn Corzilius
Jul 1, 2017·Physical Chemistry Chemical Physics : PCCP·Katharina KellerMaxim Yulikov
Apr 23, 2016·Physical Chemistry Chemical Physics : PCCP·Marie Ramirez CohenDaniella Goldfarb
Oct 7, 2016·Physical Chemistry Chemical Physics : PCCP·Katharina KellerMaxim Yulikov
Dec 6, 2018·Metallomics : Integrated Biometal Science·Mariane Le Fur, Peter Caravan
Jun 28, 2019·Chembiochem : a European Journal of Chemical Biology·Alessio BonucciElisabetta Mileo
Sep 29, 2017·Physical Chemistry Chemical Physics : PCCP·Yin YangDaniella Goldfarb
Apr 10, 2018·Inorganic Chemistry·Georgia ProkopiouDaniella Goldfarb

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