Optical Polarization of Nuclear Spins in Silicon Carbide

We demonstrate optically pumped dynamic nuclear polarization of (29)Si nuclear spins that are strongly coupled to paramagnetic color centers in 4H- and 6H-SiC. The 99%±1% degree of polarization that we observe at room temperature corresponds to an effective nuclear temperature of 5 μK. By combining ab initio theory with the experimental identification of the color centers' optically excited states, we quantitatively model how the polarization derives from hyperfine-mediated level anticrossings. These results lay a foundation for SiC-based quantum memories, nuclear gyroscopes, and hyperpolarized probes for magnetic resonance imaging.