Angewandte Chemie - International Edition
Angewandte Chemie - International Edition
5 years ago

Sample Ripening through Nanophase Separation Impacts the Performance of Dynamic Nuclear Polarization

Geoffrey Bodenhausen, Hervé Vezin, Dennis Kurzbach, Emmanuelle Weber, Ghislaine Frébourg, Giuseppe Sicoli, Daniel Abergel
Mixtures of water and glycerol provide popular matrices for low-temperature spectroscopy of vitrified samples. However, they involve counterintuitive physicochemical properties, such as spontaneous nanoscopic phase separations (NPS) in solutions that appear macroscopically homogeneous. We demonstrate that such phenomena can substantially impact the efficiency of dynamic nuclear polarization (DNP) by factors up to 20% by causing fluctuations in local concentrations of polarization agents (radicals). Thus, a spontaneous NPS of water/glycerol mixtures that takes place on time scales on the order of 30-60 min results in a confinement of polarization agents in nanoscopic water-rich vesicles, which in return affects the DNP. Such effects were found for three common polarization agents, TEMPOL, AMUPol and Trityl.

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/anie.201800493

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