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Hyperfine interactions between electron and nuclear spins have been widelyused in material science, organic chemistry, and structural biology as asensitive probe to the local chemical environment through spatialidentification of nuclear spins. With the nuclear spins identified, theisotropic and anisotropic components of the hyperfine interactions in turnoffer unique insight into the electronic ground-state properties of theparamagnetic centers. However, traditional ensemble measurements of hyperfineinteractions average over a macroscopic number of spins with differentgeometrical locations and nuclear isotopes. Here, we use a scanning tunnelingmicroscope (STM) combined with electron spin resonance (ESR) to measurehyperfine spectra of hydrogenated-titanium (Ti) atoms on MgO/Ag(100) andthereby determine the isotropic and anisotropic hyperfine interactions at thesingle-atom level. By combining vector-field ESR spectroscopy with STM-basedatom manipulation, we characterize the full hyperfine tensor of individualTi-47 and Ti-49 atoms and identify significant spatial anisotropy of hyperfineinteraction for both isotopes when they are adsorbed at low-symmetry bindingsites. Density functional theory calculations reveal that the large hyperfineanisotropy arises from a highly anisotropic distribution of the ground-stateelectron spin density. Our work highlights the power of ESR-STM-enabledsingle-atom hyperfine spectroscopy as a powerful tool in revealing ground-stateelectronic structures and atomic-scale chemical environments withnano-electronvolt resolution.

Anisotropic hyperfine interaction of surface-adsorbed single atoms