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Bis-Gadolinium Complexes for Solid Effect and Cross Effect Dynamic Nuclear Polarization.

Monu Kaushik1, Mian Qi2, Adelheid Godt2

  • 1Goethe-Universität Frankfurt am Main, Institut für Physikalische und Theoretische Chemie, Institut für Biophysikalische Chemie und Biomolekulares Magnetresonanzzentrum (BMRZ), Max-von-Laue-Strasse 7-9, 60438, Frankfurt am Main, Germany.

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|March 21, 2017
PubMed
Summary
This summary is machine-generated.

High-spin complexes enhance nuclear magnetic resonance (NMR) signal via dynamic nuclear polarization (DNP). Gadolinium (Gd) complexes show distance-dependent DNP mechanisms, enabling cross-effect DNP for biomolecular NMR.

Keywords:
cross effectdynamic nuclear polarizationgadolinium complexespolarizing agentsolid-state NMR spectroscopy

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Area of Science:

  • Solid-state NMR spectroscopy
  • Dynamic Nuclear Polarization (DNP)
  • Electron Paramagnetic Resonance (EPR)

Background:

  • High-spin complexes serve as polarizing agents (PAs) for DNP in solid-state NMR.
  • Bis(Gd-chelate) complexes are promising for biomolecular DNP due to confined electron spins.

Purpose of the Study:

  • To investigate the Gd-Gd distance dependence of DNP mechanisms using bis(Gd-chelate) complexes.
  • To elucidate the relationship between distance, DNP enhancement, and NMR signal amplification.

Main Methods:

  • Synthesis and characterization of bis(Gd-chelate) complexes with defined Gd-Gd distances (1.2-3.4 nm).
  • Solid-state NMR spectroscopy to measure DNP enhancements.
  • Electron Paramagnetic Resonance (EPR) spectroscopy (263 GHz) to analyze electron spin interactions.

Main Results:

  • Gd-Gd distances > 2.1 nm yield solid effect DNP.
  • Gd-Gd distances between 1.2-2.1 nm enable cross-effect (CE) DNP for 1H, 13C, and 15N spins.
  • Comparison of EPR spectra and DNP field profiles revealed CE matching conditions.

Conclusions:

  • The study clarifies the Gd-Gd distance dependence of DNP mechanisms, distinguishing between solid effect and CE DNP.
  • Findings guide the design of high-spin PAs for targeted DNP applications in NMR spectroscopy.
  • Understanding CE matching conditions is crucial for optimizing DNP performance in high-spin systems.