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The available theoretical approaches aiming at describing Dynamic Nuclearspin Polarization (DNP) in solutions containing molecules of biomedicalinterest and paramagnetic centers are not able to model the behaviour observedupon varying the concentration of trityl radicals or the polarizationenhancement caused by moderate addition of gadolinium complexes. In thismanuscript, we first show experimentally that the nuclear steady statepolarization reached in solutions of pyruvic acid with 15 mM trityl radicals issubstantially independent from the average internuclear distance. Thisevidences a leading role of electron (over nuclear) spin relaxation processesin determining the ultimate performances of DNP. Accordingly, we have devised avariant of the Thermal Mixing model for inhomogenously broadened electronresonance lines which includes a relaxation term describing the exchange ofmagnetic anisotropy energy of the electron spin system with the lattice. Thanksto this additional term, the dependence of the nuclear polarization on theelectron concentration can be properly accounted for. Moreover, the modelpredicts a strong increase of the final polarization on shortening the electronspin-lattice relaxation time, providing a possible explanation for the effectof gadolinium doping.

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