Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 132, Issue 21, Pages -Publisher
AMER INST PHYSICS
DOI: 10.1063/1.3428665
Keywords
density functional theory; dynamic nuclear polarisation; ELDOR; gadolinium; paramagnetic resonance; positive ions
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Electron-electron double resonance pulsed electron paramagnetic resonance (EPR) at 95 GHz (3.3 T) is used to follow the dynamics of the electron spin polarization during the first stages of dynamic nuclear polarization in solids. The experiments were performed on a frozen solution of Gd+3 (S=7/2) in water/glycerol. Focusing on the central vertical bar-1/2 >->vertical bar+1/2 > transition we measured the polarization transfer from the Gd3+ electron spin to the adjacent H-1 protons. The dependence of the echo detected EPR signal on the length of the microwave irradiation at the EPR forbidden transition corresponding to an electron and a proton spin flip is measured for different powers, showing dynamics on the microsecond to millisecond time scales. A theoretical model based on the spin density matrix formalism is suggested to account for this dynamics. The central transition of the Gd3+ ion is considered as an effective S=1/2 system and is coupled to H-1 (I=1/2) nuclei. Simulations based on a single electron-single nucleus four level system are shown to deviate from the experimental results and an alternative approach taking into account the more realistic multinuclei picture is shown to agree qualitatively with the experiments. (C) 2010 American Institute of Physics. [doi: 10.1063/1.3428665]
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