Three-dimensional localization spectroscopy of individual nuclear spins with sub-Angstrom resolution

Nuclear magnetic resonance (NMR) spectroscopy is a powerful method for analyzing the chemical composition and molecular structure of materials. At the nanometer scale, NMR has the prospect of mapping the atomic-scale structure of individual molecules, provided a method that can sensitively detect single nuclei and measure inter-atomic distances. Here, we report on precise localization spectroscopy experiments of individual ¹³ C nuclear spins near the central electronic sensor spin of a nitrogen-vacancy (NV) center in a diamond chip. By detecting the nuclear free precession signals in rapidly switchable external magnetic fields, we retrieve the three-dimensional spatial coordinates of the nuclear spins with sub-Angstrom resolution and for distances beyond 10 Å. We further show that the Fermi contact contribution can be constrained by measuring the nuclear g-factor enhancement. The presented method will be useful for mapping atomic positions in single molecules, an ambitious yet important goal of nanoscale nuclear magnetic resonance spectroscopy.