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Direct observation of hyperpolarization breaking through the spin diffusion barrier

Citation

Stern, Quentin et al. (2021), Direct observation of hyperpolarization breaking through the spin diffusion barrier, Dryad, Dataset, https://doi.org/10.5061/dryad.fttdz08s3

Abstract

Dynamic nuclear polarization (DNP) is a widely used tool for overcoming the low intrinsic sensitivity of nuclear magnetic resonance spectroscopy and imaging. Its practical applicability is typically bounded, however, by the so-called ‘spin diffusion barrier’, which relates to the poor efficiency of polarization transfer from highly polarized nuclei close to paramagnetic centers to bulk nuclei. A quantitative assessment of this barrier has been hindered so far by the lack of general methods for studying nuclear-polarization flow in the vicinity of paramagnetic centers. Here we fill this gap and introduce a general set of experiments based on microwave gating that are readily implemented. We demonstrate the versatility of our approach in experiments conducted between 1.2 – 4.2 K in static mode and at 100 K under magic angle spinning (MAS) — conditions typical for dissolution-DNP and MAS-DNP — and for the first time directly observe the dramatic dependence of polarization flow on temperature.

Methods

All data consist of NMR spectra. Data were collected using high field NMR instruments by Bruker using the software Topspin 3.5.7 and Topspin 3.6.2. They were exported to CSV files.

Usage Notes

The data are organized in subfolders. A PDF document in the root folder summarizes the list of all experiments in the dataset with precisions on experimental parameters and remarks (README.pdf). For each subfolder, the figures of the paper which were produced using the data is the subfolder is listed.

Funding

European Research Council, Award: 714519: HP4all

H2020 Marie Skłodowska-Curie Actions, Award: 766402: ZULF

NSF/DMR and the State of Florida, Award: 1644779

NSF/DMR NIH, Award: S10 OD018519

National Institutes of Health, Award: P41 GM122698 01

National Science Foundation, Award: CHE 1229170

NSF/DMR and the State of Florida, Award: 1644779

NSF/DMR NIH, Award: S10 OD018519