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Issue 4, 2019
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De novo prediction of cross-effect efficiency for magic angle spinning dynamic nuclear polarization

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Abstract

Magic angle spinning dynamic nuclear polarization (MAS-DNP) has become a key approach to boost the intrinsic low sensitivity of NMR in solids. This method relies on the use of both stable radicals as polarizing agents (PAs) and suitable high frequency microwave irradiation to hyperpolarize nuclei of interest. Relating PA chemical structure to DNP efficiency has been, and is still, a long-standing problem. The complexity of the polarization transfer mechanism has so far limited the impact of analytical derivation. However, recent numerical approaches have profoundly improved the basic understanding of the phenomenon and have now evolved to a point where they can be used to help design new PAs. In this work, the potential of advanced MAS-DNP simulations combined with DFT calculations and high-field EPR to qualitatively and quantitatively predict hyperpolarization efficiency of particular PAs is analyzed. This approach is demonstrated on AMUPol and TEKPol, two widely-used bis-nitroxide PAs. The results notably highlight how the PA structure and EPR characteristics affect the detailed shape of the DNP field profile. We also show that refined simulations of this profile using the orientation dependency of the electron spin–lattice relaxation times can be used to estimate the microwave B1 field experienced by the sample. Finally, we show how modelling the nuclear spin–lattice relaxation times of close and bulk nuclei while accounting for PA concentration allows for a prediction of DNP enhancement factors and hyperpolarization build-up times.

Graphical abstract: De novo prediction of cross-effect efficiency for magic angle spinning dynamic nuclear polarization

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Publication details

The article was received on 02 Nov 2018, accepted on 27 Dec 2018 and first published on 03 Jan 2019


Article type: Paper
DOI: 10.1039/C8CP06819D
Phys. Chem. Chem. Phys., 2019,21, 2166-2176

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    De novo prediction of cross-effect efficiency for magic angle spinning dynamic nuclear polarization

    F. Mentink-Vigier, A. Barra, J. van Tol, S. Hediger, D. Lee and G. De Paëpe, Phys. Chem. Chem. Phys., 2019, 21, 2166
    DOI: 10.1039/C8CP06819D

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