Trends in the hyperfine interactions of magnetic adatoms on thin insulating layers

Abstract

Nuclear spins are among the potential candidates prospected for quantum information technology. A recent breakthrough enabled to atomically resolve their interaction with the electron spin, the so-called hyperfine interaction, within individual atoms utilizing scanning tunneling microscopy (STM). Intriguingly, this was only realized for a few species put on a two-layers thick MgO. Here, we systematically quantify from first-principles the hyperfine interactions of the whole series of 3d transition adatoms deposited on various thicknesses of MgO, NaF, NaCl, h--BN and Cu${}_2$N films. We identify the adatom-substrate complexes with the largest hyperfine interactions and unveil the main trends and exceptions. We reveal the core mechanisms at play, such as the interplay of the local bonding geometry and the chemical nature of the thin films, which trigger transitions between high- and low-spin states accompanied with subtle internal rearrangements of the magnetic electrons. By providing a general map of hyperfine interactions, our work has immediate implications in future STM investigations aiming at detecting and realizing quantum concepts hinging on nuclear spins.

arXiv comment27 pages, 7 figures

References in corpus (25)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• A linear response approach to the calculation of the effective interaction parameters in the LDA+U method
• All-electron magnetic response with pseudopotentials: NMR chemical shifts
• Reading and Writing Single-Atom Magnets
• The role of magnetic anisotropy in the Kondo effect
• Colloquium: Atomic spin chains on surfaces
• Engineering the eigenstates of coupled spin-1/2 atoms on a surface
• Enhanced quantum coherence in exchange coupled spins via singlet-triplet transitions
• Metal adatoms on graphene and hexagonal boron nitride: Towards the rational design of self-assembly templates
• Quantum Engineering of Spin and Anisotropy in Magnetic Molecular Junctions
• Spin decoherence of magnetic atoms on surfaces
• Tuning Single-Atom Electron Spin Resonance in a Vector-Magnetic Field
• Exchange mechanism for electron paramagnetic resonance of individual adatoms
• Longitudinal and transverse electron paramagnetic resonance in a scanning tunneling microscope
• Quantifying the interplay between fine structure and geometry of an individual molecule on a surface
• A cotunneling mechanism for all-electrical Electron Spin Resonance of single adsorbed atoms
• Spin Resonance Amplitude and Frequency of a Single Atom on a Surface in a Vector Magnetic Field
• A quantum pathway to overcome the trilemma of magnetic data storage
• Adsorption Sites of Individual Metal Atoms on Ultrathin MgO(100) Films
• Efficient Ab-initio Multiplet Calculations for Magnetic Adatoms on MgO
• Electron Paramagnetic Resonance of Single Magnetic Moment on a Surface
• Complete reversal of the atomic unquenched orbital moment by a single electron
• Large effect of the metal substrate on the magnetic anisotropy of Co on hexagonal Boron Nitride
• A model for the ESR-STM phenomenon
• Site-dependent magnetism of Ni adatoms on MgO/Ag(001)

Cited by in corpus (5)

• Anisotropic hyperfine interaction of surface-adsorbed single atoms
• Electron-phonon coupling of Fe-adatom electron states on MgO/Ag(100)
• Hyperfine interactions in open-shell planar $s{p}^2$-carbon nanostructures
• 3d-oxide molecules to tailor large magnetic anisotropy energies on MgO films
• Interplay of magnetic states and hyperfine fields of iron dimers on MgO(001)