Valence Orbitals Driving the Spin Dynamics in a Rare-Earth Single-Atom Magnet.

We combine spin-polarized scanning tunneling microscopy with quantum master equation analysis to investigate the spin dynamics of the single atom magnet Dy on graphene/Ir(111). By performing reading and writing experiments, we show that the strongly spin polarized 5d6s valence shells, as well as their intra-atomic exchange coupling to the 4f shell, determine the pathways for magnetization relaxation and thus the spin dynamics. The good quantum number that determines which states are stable and which mechanisms for reversal exist in a given crystal field is the atomic total angular momentum J_{z}^{tot} and not the commonly considered J_{z}^{4f} of the 4f shell only.

Spin Excitations in a 4f-3d Heterodimer on MgO.

We report on the magnetic properties of HoCo dimers as a model system for the smallest intermetallic compound of a lanthanide and a transition metal atom. The dimers are adsorbed on ultrathin MgO(100) films grown on Ag(100). New for 4f elements, we detect inelastic excitations with scanning tunneling spectroscopy and prove their magnetic origin by applying an external magnetic field. In combination with density functional theory and spin Hamiltonian analysis, we determine the magnetic level distribution, as well as sign and magnitude of the exchange interaction between the two atoms. In contrast to typical 4f-3d bulk compounds, we find ferromagnetic coupling in the dimer.

Tailoring the magnetism of Co atoms on graphene through substrate hybridization.

We determine the magnetic properties of individual Co atoms adsorbed on graphene (G) with x-ray absorption spectroscopy and magnetic circular dichroism. The magnetic ground state of Co adatoms strongly depends on the choice of the metal substrate on which graphene is grown. Cobalt atoms on G/Ru(0001) feature exceptionally large orbital and spin moments, as well as an out-of-plane easy axis with large magnetic anisotropy. Conversely, the magnetic moments are strongly reduced for Co/G/Ir(111), and the magnetization is of the easy-plane type. We demonstrate how the Co magnetic properties, which ultimately depend on the degree of hybridization between the Co 3d orbitals and graphene π bands, can be tailored through the strength of the graphene-substrate coupling.

Magnetic moment and anisotropy of individual Co atoms on graphene.

We report on the magnetic properties of single Co atoms on graphene on Pt(111). By means of scanning tunneling microscopy spin-excitation spectroscopy, we infer a magnetic anisotropy of K=-8.1 meV with out-of-plane hard axis and a magnetic moment of 2.2µ(B). Co adsorbs on the sixfold graphene hollow site. Upon hydrogen adsorption, three differently hydrogenated species are identified. Their magnetic properties are very different from those of clean Co. Ab initio calculations support our results and reveal that the large magnetic anisotropy stems from strong ligand field effects due to the interaction between Co and graphene orbitals.

Antiferromagnetic MnNi tips for spin-polarized scanning probe microscopy.

Spin-polarized scanning tunneling microscopy (SP-STM) measures magnetoresistance with atomic resolution. While various methods for achieving SP probes have been developed, each is limited with respect to fabrication, performance, and operating conditions. In this study, we present the fabrication and use of SP-STM tips made from commercially available antiferromagnetic Mn88Ni12 foils. The tips are intrinsically SP, which is attractive for exploring magnetic phenomena in the zero field limit. The tip material is relatively ductile, is straightforward to etch, and has a Néel temperature exceeding 300 K. We benchmark the topographic and spectroscopic performance of our tips and demonstrate their spin sensitivity by measuring the two-state switching of holmium single atom magnets on MgO/Ag(100).

Magnetic remanence in single atoms.

A permanent magnet retains a substantial fraction of its saturation magnetization in the absence of an external magnetic field. Realizing magnetic remanence in a single atom allows for storing and processing information in the smallest unit of matter. We show that individual holmium (Ho) atoms adsorbed on ultrathin MgO(100) layers on Ag(100) exhibit magnetic remanence up to a temperature of 30 kelvin and a relaxation time of 1500 seconds at 10 kelvin. This extraordinary stability is achieved by the realization of a symmetry-protected magnetic ground state and by decoupling the Ho spin from the underlying metal by a tunnel barrier.