Gd(III) complexes for electron-electron dipolar spectroscopy: Effects of deuteration, pH and zero field splitting

Journal of Magnetic Resonance
Luca GarbuioMaxim Yulikov

Abstract

Spectral parameters of Gd(III) complexes are intimately linked to the performance of the Gd(III)-nitroxide or Gd(III)-Gd(III) double electron-electron resonance (DEER or PELDOR) techniques, as well as to that of relaxation induced dipolar modulation enhancement (RIDME) spectroscopy with Gd(III) ions. These techniques are of interest for applications in structural biology, since they can selectively detect site-to-site distances in biomolecules or biomolecular complexes in the nanometer range. Here we report relaxation properties, echo detected EPR spectra, as well as the magnitude of the echo reduction effect in Gd(III)-nitroxide DEER for a series of Gadolinium(III) complexes with chelating agents derived from tetraazacyclododecane. We observed that solvent deuteration does not only lengthen the relaxation times of Gd(III) centers but also weakens the DEER echo reduction effect. Both of these phenomena lead to an improved signal-to-noise ratios or, alternatively, longer accessible distance range in pulse EPR measurements. The presented data enrich the knowledge on paramagnetic Gd(III) chelate complexes in frozen solutions, and can help optimize the experimental conditions for most types of the pulse measurements of the electron...Continue Reading

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Citations

Jul 1, 2017·Physical Chemistry Chemical Physics : PCCP·Katharina KellerMaxim Yulikov
Apr 5, 2018·Physical Chemistry Chemical Physics : PCCP·Jessica A ClaytonMaxim Yulikov
Apr 23, 2016·Physical Chemistry Chemical Physics : PCCP·Marie Ramirez CohenDaniella Goldfarb
Oct 7, 2016·Physical Chemistry Chemical Physics : PCCP·Katharina KellerMaxim Yulikov
Jun 2, 2020·Physical Chemistry Chemical Physics : PCCP·Svetlana KucherHeinz-Jürgen Steinhoff
Feb 27, 2021·Physical Chemistry Chemical Physics : PCCP·Janne SoetbeerGunnar Jeschke
Apr 10, 2018·Inorganic Chemistry·Georgia ProkopiouDaniella Goldfarb

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