Quantum sensing of large nuclear-spin clusters in diamond with atomic-scale resolution

The ability to resolve the 3D structure of large clusters of nuclear spins has the potential to be a revolutionary tool for NMR imaging of single molecules and solids. The nitrogen-vacancy (NV) center in diamond is a promising platform to achieve this goal. At the same time, its local nuclear spin environment already provides a model system to study, develop and test such new methods. Here we report on quantum sensing and atomic structure analysis of a 10+ nuclear-spin cluster in diamond with atomic-scale resolution. We develop pulse sequences to coherently control the nuclear spins forming the cluster, and directly measure the pairwise dipolar couplings between the nuclear spins with high precision. We then utilize the measured nuclear-nuclear couplings between the spins to determine their 3D structure with atomic-scale resolution. The methods developed in this work can be extended to samples outside the diamond, and mark an important step towards the ultimate goal of structural imaging of single molecules and proteins.