In a theoretical study, we investigate the spin dynamics of interacting nitrogen-vacancy (NV) centers and quadrupolar $I=3/2$ nuclear spins, specifically ${}^{11}\mathrm{B}$ spins in hexagonal boron nitride (h-BN) nanosheets located near the microdiamond surface. We demonstrate the possibility of obtaining external spin-polarization by magnetic-field sweeps across the level anticrossings around zero field. To achieve this, we leverage crystal strains to establish a polarization transfer mechanism that remains robust against variations in NV orientation, crystal strain inhomogeneity, and electron-nuclear effective couplings. These results pave the way for hyperpolarization of spins in nanomaterials near the diamond surface without experiencing polarization loss to intrinsic nuclear spin-1/2 species, such as ${}^{13}\mathrm{C}$ and ${}^1\mathrm{H}$ nuclear spins in diamond. The ${}^{11}\mathrm{B}$ spins in h-BN nanosheets, with their extended relaxation time and large surface area, present a promising alternative for relayed nuclear polarization to the liquid phase and for the development of quantum simulators based on surface nuclear spins.

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• Quantum control
• Quantum protocols
• Spin polarization
• Strain
• Nitrogen vacancy centers in diamond