Coherent Control of Nitrogen Nuclear Spins via the VB−‐Center in Hexagonal Boron Nitride

ABSTRACT Charged boron vacancies () in hexagonal boron nitride (hBN) have emerged as a promising platform for quantum nanoscale sensing and imaging. While these primarily involve electron spins, nuclear spins provide an additional resource for quantum operations. This work presents a comprehensive experimental and theoretical study of the properties and coherent control of the nearest‐neighbor nuclear spins of ‐ensembles in isotope‐enriched . Multi‐nuclear spin states are selectively addressed, enabled by the state‐specific nuclear spin transitions arising from spin‐state mixing. We perform Rabi driving between selected state pairs, define elementary quantum gates, and measure longer than 10 nuclear Rabi coherence times. We observe a two orders of magnitude nuclear g‐factor enhancement that underpins fast nuclear spin gates. Accompanying numerical simulations provide a deep insight into the underlying mechanisms. These results establish the foundations for leveraging nuclear spins in center‐based quantum applications, particularly for extending coherence times and enhancing the sensitivity of 2D quantum sensing foils.