We experimentally demonstrate high degree of polarization of 13C nuclear spins weakly interacting with nitrogen-vacancy (NV) centers in diamond. We combine coherent microwave excitation pulses with optical illumination to provide controlled relaxation and achieve a polarity-tunable, fast nuclear polarization of degree higher than 85% at room temperature for remote 13C nuclear spins exhibiting hyperfine interaction strength with NV centers of the order of 600 kHz. We show with the aid of numerical simulation that the anisotropic hyperfine tensor components naturally provide a route to control spin mixing parameter so that highly efficient nuclear polarization is enabled through careful tuning of nuclear quantization axis by external magnetic field. We further discuss spin dynamics and wide applicability of this method to various target 13C nuclear spins around the NV center electron spin. The proposed control method demonstrates an efficient and versatile route to realize, for example, high-fidelity spin register initialization and quantum metrology using nuclear spin resources in solids.
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