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Issue 2, 2014
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Relevance of electron spin dissipative processes to dynamic nuclear polarization via thermal mixing

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Abstract

The available theoretical approaches aiming at describing Dynamic Nuclear spin Polarization (DNP) in solutions containing molecules of biomedical interest and paramagnetic centers are not able to model the behaviour observed upon varying the concentration of trityl radicals or the polarization enhancement caused by moderate addition of gadolinium complexes. In this manuscript, we first show experimentally that the nuclear steady state polarization reached in solutions of pyruvic acid with 15 mM trityl radicals is substantially independent on the average internuclear distance. This evidences a leading role of electron (over nuclear) spin relaxation processes in determining the ultimate performances of DNP. Accordingly, we have devised a variant of the Thermal Mixing model for inhomogenously broadened electron resonance lines which includes a relaxation term describing the exchange of magnetic anisotropy energy of the electron spin system with the lattice. Thanks to this additional term, the dependence of the nuclear polarization on the electron concentration can be properly accounted for. Moreover, the model predicts a strong increase of the final polarization upon shortening the electron spin–lattice relaxation time, providing a possible explanation for the effect of gadolinium doping.

Graphical abstract: Relevance of electron spin dissipative processes to dynamic nuclear polarization via thermal mixing

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Publication details

The article was received on 18 Jun 2013, accepted on 05 Nov 2013 and first published on 08 Nov 2013


Article type: Paper
DOI: 10.1039/C3CP52534A
Citation: Phys. Chem. Chem. Phys., 2014,16, 753-764
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    Relevance of electron spin dissipative processes to dynamic nuclear polarization via thermal mixing

    S. Colombo Serra, M. Filibian, P. Carretta, A. Rosso and F. Tedoldi, Phys. Chem. Chem. Phys., 2014, 16, 753
    DOI: 10.1039/C3CP52534A

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