Intrinsic high-fidelity spin polarization of charged vacancies in hexagonal boron nitride

The negatively charged boron vacancy ($\mathrm{V}_{\mathrm{B}}^-$) in hexagonal boron nitride (hBN) has garnered significant attention among defects in two-dimensional materials. This owes, in part, to its deterministic generation, well-characterized atomic structure, and optical polarizability at room temperature. We investigate the latter through extensive measurements probing both the ground and excited state polarization dynamics. We develop a semiclassical model based on these measurements that predicts a near-unity degree of spin polarization, surpassing other solid-state spin defects under ambient conditions. Building upon our model, we include the presence of nuclear spin degrees of freedom adjacent to the $\mathrm{V}_{\mathrm{B}}^-$ and perform a comprehensive set of Lindbladian numerics to investigate the hyperfine-induced polarization of the nuclear spins. Our simulations predict a number of important features that emerge as a function of magnetic field which are borne out by experiment.