High-Sensitivity Optical Detection of Electron-Nuclear Spin Clusters in Diamond

We perform sensitive nuclear magnetic resonance (NMR) with spin ensembles which are polarized by nitrogen vacancy centers (NV centers) in diamond at room-temperature. With a near shot-noise-limited photoluminescence detection and a highly uniform magnetic field, we resolve sharp NMR features arising from multiple spin clusters. In particular, we investigate the coupling between nuclear spins and NV centers in the neutral and negatively charged states. Further, we perform high precision NMR and coherent control of families of carbon 13 nuclear spin ensembles in the $m_s$=0 level of the NV ground state. Applying an off-axis magnetic field reveals the various sites associated with the otherwise degenerate couplings of the carbon 13 sites around the NV electronic spin providing access to all the hyperfine tensor components. Last, we observe spectroscopic signatures of pairs of nuclear spins coupled to the same NV center. These results are relevant for ensemble measurements of dynamical polarization that currently rely on expensive nuclear magnetic resonance systems as well as for recently proposed nuclear spin gyroscopes.