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

Single-molecule nuclear magnetic resonance (NMR) is a crown-jewel challenge in the field of magnetic resonance spectroscopy and has important applications in chemical analysis and in quantum computing. Recently, it becomes possible to tackle this grand challenge thanks to experimental advances in preserving quantum coherence of nitrogen-vacancy (NV) center spins in diamond as a sensitive probe and theoretical proposals on atomic-scale magnetometry via dynamical decoupling control. Through decoherence measurement of NV centers under dynamical decoupling control, sensing of single $^{13}\textbf{C}$ at nanometer distance has been realized. Toward the ultimate goal of structure analysis of single molecules, it is highly desirable to directly measure the interactions within single nuclear spin clusters. Here we sensed a single $^{13}\textbf{C}$-$^{13}\textbf{C}$ nuclear spin dimer located about 1 nm from the NV center and characterized the interaction between the two nuclear spins, by measuring NV center spin decoherence under various dynamical decoupling control. From the measured interaction we derived the spatial configuration of the dimer with atomic-scale resolution. These results demonstrate that central spin decoherence under dynamical decoupling control is a feasible probe for NMR structure analysis of single molecules.