Sensing and atomic-scale structure analysis of single nuclear-spin clusters in diamond

Single-molecule nuclear magnetic resonance is a current challenge in the field of magnetic resonance spectroscopy and has important applications in chemical analysis and quantum computing. Through decoherence measurements of nitrogen-vacancy centres under dynamical decoupling control, the sensing of a single C-13 nuclear spin at nanometre distance has recently been realized(1-3). A further step towards the ultimate goal of structure analysis of single molecules would be the direct measurement of the interactions within single nuclear-spin clusters(4). Here we sense a single C-13-C-13 nuclear-spin dimer located about 1nm from the nitrogen-vacancy centre and characterize the interaction (similar to 690 Hz) between the two nuclear spins. From the measured interaction we derive the spatial configuration of the dimer with atomic-scale resolution. These results indicate that, in combination with advanced material-surface engineering, central spin decoherence under dynamical decoupling control may be a useful probe for nuclear magnetic resonance single-molecule structure analysis.