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.

We describe an ab initio disordered local moment theory for materials with quenched static compositional disorder traversing first-order magnetic phase transitions. It accounts quantitatively for metamagnetic changes and the magnetocaloric effect. For perfect stoichiometric B2-ordered FeRh, we calculate the transition temperature of the ferromagnetic-antiferromagnetic transition to be T t = 495 K and a maximum isothermal entropy change in 2 T of | S| = 21.1 J K −1 kg −1 . A large (40%) component of | S| is electronic. The transition results from a fine balance of competing electronic effects which is disturbed by small compositional changes; e.g., swapping just 2% Fe of "defects" onto the Rh sublattice makes T t drop by 290 K. This hypersensitivity explains the narrow compositional range of the transition and impurity doping effects.

Chiral magnets are a promising route towards dense magnetic storage technology due to their inherent nano-scale dimensions and energy efficient properties. Engineering chiral magnets requires atomic-level control of the magnetic exchange interactions, including the Dzyaloshinskii–Moriya interaction, which defines a rotational sense for the magnetization of two coupled magnetic moments. Here we show that the indirect conduction electron-mediated Dzyaloshinskii–Moriya interaction between two individual magnetic atoms on a metallic surface can be manipulated by changing the interatomic distance with the tip of a scanning tunnelling microscope. We quantify this interaction by comparing our measurements to a quantum magnetic model and ab-initio calculations yielding a map of the chiral ground states of pairs of atoms depending on the interatomic separation. The map enables tailoring the chirality of the magnetization in dilute atomic-scale magnets.

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).

Magnetic interactions underpin a plethora of magnetic states of matter, hence playing a central role both in fundamental physics and for future spintronic and quantum computation devices. The Dzyaloshinskii-Moriya interaction, D S S ij i j · ( ), being chiral and driven by relativistic effects, leads to the stabilization of highly-noncollinear spin textures such as skyrmions, which thanks to their topological nature are promising building blocks for magnetic data storage and processing elements.Here, we reveal and study a new chiral pair interaction, C S S S S ij i j i j · ( )( · ), which is the biquadratic equivalent of the DMI. First, we derive this interaction and its guiding principles from a microscopic model, and we connect the atomistic form to the micromagnetic one. Second, we study its properties in the simplest prototypical systems, magnetic 3d transition metal dimers deposited on the Pt(111), Pt(100), Ir(111), and Re(0001) surfaces, resorting to systematic first-principles calculations. Lastly, we discuss its importance and implications not only for magnetic dimers but also for extended systems, namely one-dimensional spin spirals and complex two-dimensional magnetic structures, such as a nanoskyrmion lattice found in an Fe monolayer on Ir(111).

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.

A cluster of a few magnetic atoms on the surface of a nonmagnetic substrate is one suitable realization of a bit for spin-based information technology. The prevalent approach to achieve magnetic stability is decoupling the cluster spin from substrate conduction electrons in order to suppress destabilizing spin-flips. However, this route entails less flexibility in tailoring the coupling between the bits needed for spin-processing. Here, we use a spin-resolved scanning tunneling microscope to write, read, and store spin information for hours in clusters of three atoms strongly coupled to a substrate featuring a cloud of non-collinearly polarized host atoms, a so-called non-collinear giant moment cluster. The giant moment cluster can be driven into a Kondo screened state by simply moving one of its atoms to a different site. Using the exceptional atomic tunability of the non-collinear substrate mediated Dzyaloshinskii–Moriya interaction, we propose a logical scheme for a four-state memory.