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Nuclear spins nearby nitrogen-vacancy (NV) centers in diamond are excellentquantum memory for quantum computing and quantum sensing, but are difficult tobe initialized due to their weak interactions with the environment. Here wepropose and demonstrate a magnetic-field-independent, deterministic and highlyefficient polarization scheme by introducing chopped laser pulses into thedouble-resonance initialization method. With this method, we demonstrateinitialization of single-nuclear-spin approaching $98.1\%$ and a$^{14}N$-$^{13}C$ double-nuclear-spin system approaching $96.8\%$ at roomtemperature. The initialization is limited by a nuclear-spin depolarizationeffect due to chopped laser excitation. Our approach could be extended to NVsystems with more nuclear spins and would be a useful tool in futureapplications such as nano-MRI and single-cell NMR.

Dynamically Polarizing Spin Register of NV Centers in Diamond using Chopped Laser Pulses