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Single-molecule sensitivity of nuclear magnetic resonance (NMR) and angstromresolution of magnetic resonance imaging (MRI) are the highest challenges inmagnetic microscopy. Recent development in dynamical-decoupling- (DD) enhanceddiamond quantum sensing has enabled single-nucleus NMR and nanoscale NMR.Similar to conventional NMR and MRI, current DD-based quantum sensing utilizesthe frequency fingerprints of target nuclear spins. The frequency fingerprintsby their nature cannot resolve different nuclear spins that have the same noisefrequency or differentiate different types of correlations in nuclear-spinclusters, which limit the resolution of single-molecule MRI. Here we show thatthis limitation can be overcome by using wave-function fingerprints of targetnuclear spins, which is much more sensitive than the frequency fingerprints tothe weak hyperfine interaction between the targets and a sensor under resonantDD control. We demonstrate a scheme of angstrom-resolution MRI that is capableof counting and individually localizing single nuclear spins of the samefrequency and characterizing the correlations in nuclear-spin clusters. Anitrogen-vacancy-center spin sensor near a diamond surface, provided that thecoherence time is improved by surface engineering in the near future, may beemployed to determine with angstrom resolution the positions and conformationof single molecules that are isotope labeled. The scheme in this work offers anapproach to breaking the resolution limit set by the frequency gradients inconventional MRI and to reaching the angstrom-scale resolution.

Angstrom-resolution magnetic resonance imaging of single molecules via wavefunction fingerprints of nuclear spins