Anisotropic Hyperfine Interaction of Surface-Adsorbed Single Atoms

Jinkyung Kim, Kyungju Noh, Yi Chen, Fabio Donati, Andreas J. Heinrich, Christoph Wolf, Yujeong Bae

Research output: Contribution to journalArticlepeer-review

1 Scopus citations

Abstract

Hyperfine interactions have been widely used in material science, organic chemistry, and structural biology as a sensitive probe to local chemical environments. However, traditional ensemble measurements of hyperfine interactions average over a macroscopic number of spins with different geometrical locations and nuclear isotopes. Here, we use a scanning tunneling microscope (STM) combined with electron spin resonance (ESR) to measure hyperfine spectra of hydrogenated-Ti on MgO/Ag(100) at low-symmetry binding sites and thereby determine the isotropic and anisotropic hyperfine interactions at the single-atom level. Combining vector-field ESR spectroscopy with STM-based atom manipulation, we characterize the full hyperfine tensors of 47Ti and 49Ti and identify significant spatial anisotropy of the hyperfine interactions for both isotopes. Density functional theory calculations reveal that the large hyperfine anisotropy arises from highly anisotropic distributions of the ground-state electron spin density. Our work highlights the power of ESR-STM-enabled single-atom hyperfine spectroscopy in revealing electronic ground states and atomic-scale chemical environments.

Original languageEnglish
Pages (from-to)9766-9772
Number of pages7
JournalNano Letters
Volume22
Issue number23
DOIs
StatePublished - 14 Dec 2022

Keywords

  • Electron spin resonance
  • Hyperfine interaction
  • Nuclear spin
  • Scanning probe
  • Scanning tunneling microscopy

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