We demonstrate using inelastic scanning tunneling spectroscopy and simulations based on density functional theory that the amplitude and sign of the magnetic anisotropy energy for a single Fe atom adsorbed onto the Pt(111) surface can be manipulated by modifying the adatom binding site. Since the magnitude of the measured anisotropy is remarkably small, up to an order of magnitude smaller than previously reported, electron-hole excitations are weak and thus the spin excitation exhibits long lived precessional lifetimes compared to the values found for the same adatom on noble metal surfaces.

Thin-film sub-5 nm magnetic skyrmions constitute an ultimate scaling alternative for future digital data storage. Skyrmions are robust noncollinear spin textures that can be moved and manipulated by small electrical currents. Here we show here a technique to detect isolated nanoskyrmions with a current perpendicular-to-plane geometry, which has immediate implications for device concepts. We explore the physics behind such a mechanism by studying the atomistic electronic structure of the magnetic quasiparticles. We investigate from first principles how the isolated skyrmion local-density-of-states which tunnels into the vacuum, when compared with the ferromagnetic background, is modified by the site-dependent spin mixing of electronic states with different relative canting angles. Local transport properties are sensitive to this effect, as we report an atomistic conductance anisotropy of up to ∼20% for magnetic skyrmions in Pd/Fe/Ir(111) thin films. In single skyrmions, engineering this spin-mixing magnetoresistance could possibly be incorporated in future magnetic storage technologies.

We present a first-principles theory of dynamical spin excitations in the presence of spin-orbit coupling. The broken global spin rotational invariance leads to a new sum rule. We explore the competition between the magnetic anisotropy energy and the external magnetic field, as well as the role of electron-hole excitations, through calculations for 3d-metal adatoms on the Cu(111) surface. The spin excitation resonance energy and lifetime display non-trivial behavior, establishing the strong impact of relativistic effects. We legitimate the use of the Landau-Lifshitz-Gilbert equation down to the atomic limit, but with parameters that differ from a stationary theory.

Access to magnetic excitation spectra of single atoms deposited on surfaces is nowadays possible by means of low-temperature inelastic scanning tunneling spectroscopy. We present a first-principles method for the calculation of inelastic tunneling spectra utilizing the Korringa-Kohn-Rostoker Green function method combined with time-dependent density functional theory and many-body perturbation theory. The key quantity is the electron self-energy describing the coupling of the electrons to the spin excitation within the adsorbate. By investigating Cr, Mn, Fe and Co adatoms on a Cu(111) substrate, we spin-characterize the spectra and demonstrate that their shapes are altered by the magnetization of the adatoms, of the tip and the orbital decay into vacuum. Our method also predicts spectral features more complex than the steps obtained by simpler models for the adsorbate (e.g., localized spin models).

The dynamical transverse magnetic Kohn-Sham susceptibility calculated within time-dependent density functional theory shows a fairly linear behavior for a finite energy window. This observation is used to propose a scheme where the computation of this quantity is greatly simplified. Regular simulations based on static density functional theory can be used to extract the dynamical behavior of the magnetic response function. Besides the ability to calculate elegantly damping of magnetic excitations, we derive along the way useful equations giving the main characteristics of these excitations: effective g-factors and the resonance frequencies that can be accessed experimentally using inelastic scanning tunneling spectroscopy or spin-polarized electron energy loss spectroscopy.