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Nuclear magnetic resonance (NMR) is a powerful method for determining the structure of molecules and proteins. While conventional NMR requires averaging over large ensembles, recent progress with single-spin quantum sensors has created the prospect of magnetic imaging of individual molecules. As an initial step towards this goal, isolated nuclear spins and spin pairs have been mapped. However, large clusters of interacting spins - such as found in molecules - result in highly complex spectra. Imaging these complex systems is an outstanding challenge due to the required high spectral resolution and efficient spatial reconstruction with sub-angstrom precision. Here we develop such atomic-scale imaging using a single nitrogen-vacancy (NV) centre as a quantum sensor, and demonstrate it on a model system of $27$ coupled $^{13}$C nuclear spins in a diamond. We present a new multidimensional spectroscopy method that isolates individual nuclear-nuclear spin interactions with high spectral resolution ($< 80,$mHz) and high accuracy ($2$ mHz). We show that these interactions encode the composition and inter-connectivity of the cluster, and develop methods to extract the 3D structure of the cluster with sub-angstrom resolution. Our results demonstrate a key capability towards magnetic imaging of individual molecules and other complex spin systems.
We report on a nanoscale quantum-sensing protocol which tracks a free precession of a single nuclear spin and is capable of estimating an azimuthal angle---a parameter which standard multipulse protocols cannot determine---of the target nucleus. Our
Understanding the dynamics of a quantum bits environment is essential for the realization of practical systems for quantum information processing and metrology. We use single nitrogen-vacancy (NV) centers in diamond to study the dynamics of a disorde
Electron and nuclear spins associated with point defects in insulators are promising systems for solid state quantum technology. While the electron spin usually is used for readout and addressing, nuclear spins are exquisite quantum bits and memory s
Robust, high-fidelity readout is central to quantum device performance. Overcoming poor readout is an increasingly urgent challenge for devices based on solid-state spin defects, particularly given their rapid adoption in quantum sensing, quantum inf
Magnetic field fluctuations arising from fundamental spins are ubiquitous in nanoscale biology, and are a rich source of information about the processes that generate them. However, the ability to detect the few spins involved without averaging over