Optical hyperpolarization of nitrogen donor spins in bulk diamond

We report hyperpolarization of the electronic spins associated with substitutional nitrogen defects in bulk diamond crystals. Hyperpolarization is achieved by optical pumping of nitrogen vacancy centers followed by rapid cross relaxation at the energy level matching condition in a 51 mT bias field. The maximum observed donor spin polarization is $0.9%$, corresponding to an enhancement of 25 compared to the thermal Boltzmann polarization. A further accumulation of polarization is impeded by an anomalous optical saturation effect that we attribute to charge state conversion processes. Hyperpolarized nitrogen donors may form a useful resource for increasing the efficiency of diamond-based dynamic nuclear polarization devices.