Not yet reviewed by Pith; the record is open.

Van der Waals layered materials are a focus of materials research as they support strong quantum effects and can easily form heterostructures. Electron spins in van der Waals materials played crucial roles in many recent breakthroughs, including topological insulators, two-dimensional (2D) magnets, and spin liquids. However, nuclear spins in van der Waals materials remain an unexplored quantum resource. Here we report the first demonstration of optical polarization and coherent control of nuclear spins in a van der Waals material at room temperature. We use negatively-charged boron vacancy ($V_B^-$) spin defects in hexagonal boron nitride to polarize nearby nitrogen nuclear spins. Remarkably, we observe the Rabi frequency of nuclear spins at the excited-state level anti-crossing of $V_B^-$ defects to be 350 times larger than that of an isolated nucleus, and demonstrate fast coherent control of nuclear spins. We also detect strong electron-mediated nuclear-nuclear spin coupling that is 5 orders of magnitude larger than the direct nuclear spin dipolar coupling, enabling multi-qubit operations. Nitrogen nuclear spins in a triangle lattice will be suitable for large-scale quantum simulation. Our work opens a new frontier with nuclear spins in van der Waals materials for quantum information science and technology.