Anisotropic hyperfine interaction of surface-adsorbed single atoms
arXiv:2207.06036 · doi:10.1021/acs.nanolett.2c02782
Abstract
Hyperfine interactions between electron and nuclear spins have been widely used in material science, organic chemistry, and structural biology as a sensitive probe to the local chemical environment through spatial identification of nuclear spins. With the nuclear spins identified, the isotropic and anisotropic components of the hyperfine interactions in turn offer unique insight into the electronic ground-state properties of the paramagnetic centers. 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-titanium (Ti) atoms on MgO/Ag(100) and thereby determine the isotropic and anisotropic hyperfine interactions at the single-atom level. By combining vector-field ESR spectroscopy with STM-based atom manipulation, we characterize the full hyperfine tensor of individual Ti-47 and Ti-49 atoms and identify significant spatial anisotropy of hyperfine interaction for both isotopes when they are adsorbed at low-symmetry binding sites. Density functional theory calculations reveal that the large hyperfine anisotropy arises from a highly anisotropic distribution of the ground-state electron spin density. Our work highlights the power of ESR-STM-enabled single-atom hyperfine spectroscopy as a powerful tool in revealing ground-state electronic structures and atomic-scale chemical environments with nano-electronvolt resolution.
arXiv comment17 pages, 4 figures
References in corpus (16)
- The nitrogen-vacancy colour centre in diamond
- Quantum ESPRESSO toward the exascale
- Silicon Quantum Electronics
- Atomic-scale imaging of a 27-nuclear-spin cluster using a single-spin quantum sensor
- Sensing remote nuclear spins
- Engineering the eigenstates of coupled spin-1/2 atoms on a surface
- Enhanced quantum coherence in exchange coupled spins via singlet-triplet transitions
- Longitudinal and transverse electron paramagnetic resonance in a scanning tunneling microscope
- Harnessing the Quantum Behavior of Spins on Surfaces
- Quantifying the interplay between fine structure and geometry of an individual molecule on a surface
- Robust two-qubit gates for donors in silicon controlled by hyperfine interactions
- Enhancement of DFT-calculations at Petascale: Nuclear Magnetic Resonance, Hybrid Density Functional Theory and Car-Parrinello calculations
- Spin Resonance Amplitude and Frequency of a Single Atom on a Surface in a Vector Magnetic Field
- Experimental Determination of a Single Atom Ground State Orbital through Hyperfine Anisotropy
- Inelastic electron tunneling spectroscopy of a single nuclear spin
- Trends in the hyperfine interactions of magnetic adatoms on thin insulating layers
Cited by in corpus (11)
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- Experimental Determination of a Single Atom Ground State Orbital through Hyperfine Anisotropy
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- Contrasting exchange-field and spin-transfer torque driving mechanisms in all-electric electron spin resonance
- Single-shot readout of the nuclear spin of an on-surface atom
- Efficient driving of a spin-qubit using single-atom magnets
- Spin-State Engineering of Single Titanium Adsorbates on Ultrathin Magnesium Oxide
- Coherent and Dissipative Spin Torques in Quantum Dots: A Unified Framework for Quantum Spin Dynamics
- 3d-oxide molecules to tailor large magnetic anisotropy energies on MgO films
- Theory of Electron Spin Resonance Scanning Tunneling Microscopy: The First Decade