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Magnetic resonance imaging of $^{13}$C-labeled metabolites enhanced by parahydrogen-induced polarization (PHIP) can enable real-time monitoring of processes within the body. We introduce a robust, easily implementable technique for transferring parahydrogen-derived singlet order into 13C magnetization using adiabatic radio-frequency sweeps at $μ$T fields. We experimentally demonstrate the applicability of this technique to several molecules, including some molecules relevant for metabolic imaging, where we show significant improvements in the achievable polarization, in some cases reaching above 60%. Furthermore, we introduce a site-selective deuteration scheme, where deuterium is included in the coupling network of a pyruvate ester to enhance the efficiency of the polarization transfer. These improvements are enabled by the fact that the transfer protocol avoids relaxation induced by strongly coupled quadrupolar nuclei.

We investigate nuclear spin hyperpolarization from nitrogen vacancy centers in isotopically enriched diamonds with $^{13}$C concentrations up to 100%. $^{13}$C enrichment leads to hyperfine structure of the nitrogen vacancy electron spin resonance spectrum and as a result the spectrum of dynamic nuclear polarization. We show that strongly-coupled $^{13}$C spins in the first shell surrounding a nitrogen vacancy center generate resolved hyperfine splittings, but do not act as an intermediary in the transfer of hyperpolarization of bulk nuclear spins. High levels of $^{13}$C enrichment are desirable to increase the efficiency of hyperpolarizaiton for magnetic resonance signal enhancement, imaging contrast agents, and as a platform for quantum sensing and many-body physics.

Nanodiamonds containing nitrogen vacancy (NV-) centers show promise for a number of emerging applications including targeted in vivo imaging and generating nuclear spin hyperpolarization for enhanced NMR spectroscopy and imaging. Here, we develop a detailed understanding of the magnetic resonance behavior of NV- centers in an ensemble of nanodiamonds with random crystal orientations. Two-dimensional optically detected magnetic resonance spectroscopy reveals the distribution of energy levels, spin populations, and transition probabilities that give rise to a complex spectrum. We identify overtone transitions that are inherently insensitive to crystal orientation and give well-defined transition frequencies that access the entire nanodiamond ensemble. These transitions may be harnessed for high-resolution imaging and generation of nuclear spin hyperpolarization. The data are well described by numerical simulations from the zero- to high-field regimes, including the intermediate regime of maximum complexity. We evaluate the prospects of nanodiamond ensembles specifically for nuclear hyperpolarization and show that frequency-swept dynamic nuclear polarization may transfer a large amount of the NV- center's hyperpolarization to nuclear spins by sweeping over a small region of its spectrum., 6 pages, 5 figures

One of the most remarkable properties of the nitrogen-vacancy (NV) center in diamond is that optical illumination initializes its electronic spin almost completely, a feature that can be exploited to polarize other spin species in their proximity. Here we use field-cycled nuclear magnetic resonance (NMR) to investigate the mechanisms of spin polarization transfer from NVs to 13C spins in diamond at room temperature. We focus on the dynamics near 51 mT, where a fortuitous combination of energy matching conditions between electron and nuclear spin levels gives rise to alternative polarization transfer channels. By monitoring the 13C spin polarization as a function of the applied magnetic field, we show 13C spin pumping takes place via a multi-spin cross relaxation process involving the NV- spin and the electronic and nuclear spins of neighboring P1 centers. Further, we find that this mechanism is insensitive to the crystal orientation relative to the magnetic field, although the absolute level of 13C polarization - reaching up to ~3% under optimal conditions - can vary substantially depending on the interplay between optical pumping efficiency, photo-generated carriers, and laser-induced heating.

Nitrogen vacancy (NV-) color centers in diamond are a prime candidate for use in quantum information devices, owing to their spin-1 ground state, straightforward optical initialization and readout, and long intrinsic coherence times in a room-temperature solid. While the 13C nuclear spin is often a dominant source of magnetic noise, we observe transitions between electron-nuclear hyperfine states of NV- centers in 99% 13C diamond that are robust to decoherence. At magnetic field strengths ranging from 550 - 900 G, these transitions are observable by optically detected magnetic resonance (ODMR), and exhibit linewidths narrowed by factors as high as ~130 at room temperature over typical electron-type transitions observed from this spin system. We anticipate the use of these decoherence-protected transitions, in combination with dynamical decoupling methods, for storage of quantum information., 21 pages, 1 table, 5 figures