Efficient Ab-initio Multiplet Calculations for Magnetic Adatoms on MgO

Abstract

Scanning probe microscopy and spectroscopy, and more recently in combination with electron spin resonance, have allowed the direct observation of electron dynamics on the single-atom limit. The interpretation of data is strongly depending on model Hamiltonians. However, fitting effective spin Hamiltonians to experimental data lacks the ability to explore a vast number of potential systems of interest. By using plane-wave density functional theory (DFT) as starting point, we build a multiplet Hamiltonian making use of maximally-localized Wannier functions. The Hamiltonian contains spin-orbit and electron-electron interactions needed to obtain the relevant spin dynamics. The resulting reduced Hamiltonian is solved by exact diagonalization. We compare three prototypical cases of 3d transition metals Mn (total spin $S=5/2$), Fe ($S=2$) and Co ($S=3/2$) on MgO with experimental data and find that our calculations can accurately predict the spin orientation and anisotropy of the magnetic adatom. Our method does not rely on experimental input and permits us to explore and predict the fundamental magnetic properties of adatoms on surfaces.

arXiv comment13 figures. It includes Supplementary Material

References in corpus (23)

• Advanced capabilities for materials modelling with Quantum ESPRESSO
• Maximally-localized generalized Wannier functions for composite energy bands
• A linear response approach to the calculation of the effective interaction parameters in the LDA+U method
• Maximally localized Wannier functions: Theory and applications
• Pseudopotentials for high-throughput DFT calculations
• Precision and efficiency in solid-state pseudopotential calculations
• Multiplet ligand-field theory using Wannier orbitals
• Reading and Writing Single-Atom Magnets
• Exponential localization of Wannier functions in insulators
• The role of magnetic anisotropy in the Kondo effect
• The role of spin in the calculation of Hubbard $U$ and Hund's $J$ parameters from first principles
• Giant magnetic anisotropy of Co, Ru, and Os adatoms on MgO (001) surface
• Multi-orbital Kondo physics of Co in Cu hosts
• Many-body models for molecular nanomagnets
• First-principles modelling of magnetic excitations in Mn12
• A cotunneling mechanism for all-electrical Electron Spin Resonance of single adsorbed atoms
• Electronic properties of transition metal atoms on Cu${}_2$N/Cu(100)
• Derivation of the spin Hamiltonians for Fe in MgO
• Complete reversal of the atomic unquenched orbital moment by a single electron
• Electronic and Magnetic Properties of single Fe atoms on a CuN Surface; Effects of Electron Correlations
• Correlation effects in insulating surface nanostructures
• Large effect of the metal substrate on the magnetic anisotropy of Co on hexagonal Boron Nitride
• Imaging the buried MgO/Ag interface: formation mechanism of the STM contrast

Cited by in corpus (14)

• Spin Resonance Amplitude and Frequency of a Single Atom on a Surface in a Vector Magnetic Field
• A theoretical review on the single-impurity electron spin resonance on surfaces
• A study of all-electric electron spin resonance using Floquet quantum master equations
• Trends in the hyperfine interactions of magnetic adatoms on thin insulating layers
• Contrasting exchange-field and spin-transfer torque driving mechanisms in all-electric electron spin resonance
• Microscopic theory of spin-relaxation of a single Fe adatom coupled to substrate vibrations
• Efficient driving of a spin-qubit using single-atom magnets
• Electron-phonon coupling of Fe-adatom electron states on MgO/Ag(100)
• Spin-State Engineering of Single Titanium Adsorbates on Ultrathin Magnesium Oxide
• Unraveling spin entanglement using quantum gates with scanning tunneling microscopy-driven electron spin resonance
• Orbital-resolved single atom magnetism measured with X-ray absorption spectroscopy
• Interplay of magnetic states and hyperfine fields of iron dimers on MgO(001)
• Theory of Electron Spin Resonance Scanning Tunneling Microscopy: The First Decade
• Inelastic electron tunneling through adatoms and molecular nanomagnets