Abstract
We report the generation and observation of long-lived spin states in deuterated methyl groups by dissolution DNP. These states are based on population imbalances between manifolds of spin states corresponding to irreducible representations of the C3v point group and feature strongly dampened quadrupolar relaxation. Their lifetime depends on the activation energies of methyl group rotation. With dissolution DNP, we can reduce the deuterium relaxation rate by a factor up to 20, thereby extending the experimentally available time window. The intrinsic limitation of NMR spectroscopy of quadrupolar spins by short relaxation times can thus be alleviated.
Highlights
We report the generation and observation of long-lived spin states in deuterated methyl groups by dissolution DNP
These states are based on population imbalances between manifolds of spin states corresponding to irreducible representations of the C3v point group and feature strongly dampened quadrupolar relaxation
We highlight a curious and potentially valuable side-effect of hyperpolarisation by Dissolution dynamic nuclear polarization (D-DNP): the creation of non-equilibrium population distributions in symmetrical deuterated spin systems. The utility of this finding lies in the long-lived nature of these population imbalances, which exhibit lifetimes that can be 20 times longer than the spinlattice relaxation time T 1(Dz) of the Zeeman polarization Dz of deuterium nuclei that often relaxes too quickly (typically 0.5 < T 1(Dz) < 2 s) considering the time required to transfer a hyperpolarized solution to an NMR spectrometer or to an MRI system for spectroscopy or imaging (Fig. 1)
Summary
We report the generation and observation of long-lived spin states in deuterated methyl groups by dissolution DNP. These states are based on population imbalances between manifolds of spin states corresponding to irreducible representations of the C3v point group and feature strongly dampened quadrupolar relaxation. We report the observation of a spin-state imbalance (SSI) in deuterated methyl groups CD3.
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