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 13 C 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 13 C spin polarization as a function of the applied magnetic field, we show 13 C spin pumping takes place via a multi-spin cross relaxation process involving the NVspin 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 13 C 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.

Nuclear spin hyperpolarization provides a promising route to overcome the challenges imposed by the limited sensitivity of nuclear magnetic resonance. Here we demonstrate that dissolution of spin-polarized pentacene-doped naphthalene crystals enables transfer of polarization to target molecules via intermolecular cross-relaxation at room temperature and moderate magnetic fields (1.45 T). This makes it possible to exploit the high spin polarization of optically polarized crystals, while mitigating the challenges of its transfer to external nuclei. With this method, we inject the highly polarized mixture into a benchtop NMR spectrometer and observe the polarization dynamics for target 1H nuclei. Although the spectra are radiation damped due to the high naphthalene magnetization, we describe a procedure to process the data to obtain more conventional NMR spectra and extract the target nuclei polarization. With the entire process occurring on a time scale of 1 min, we observe NMR signals enhanced by factors between −200 and −1730 at 1.45 T for a range of small molecules.

Optically detected magnetic resonance of nitrogen vacancy centers in diamond offers novel routes to both DC and AC magnetometry in diamond anvil cells under high pressures (> 3 GPa). However, a serious challenge to realizing experiments has been the insertion of microwave radiation in to the sample space without screening by the gasket material. We utilize designer anvils with lithographically-deposited metallic microchannels on the diamond culet as a microwave antenna. We detected the spin resonance of an ensemble of microdiamonds under pressure, and measure the pressure dependence of the zero field splitting parameters. These experiments enable the possibility for all-optical magnetic resonance experiments on sub-µL sample volumes at high pressures.

Magnetic resonance imaging of 13 C-labeled metabolites enhanced by parahydrogen-induced polarization (PHIP) enables real-time monitoring of processes within the body. We introduce a robust, easily implementable technique for transferring parahydrogen-derived singlet order into 13 C magnetization using adiabatic radio frequency sweeps at microtesla 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% nuclear spin polarization. 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.