Markus Ternes

Large magnetic anisotropy of a single atomic spin embedded in a surface molecular network.

Magnetic anisotropy allows magnets to maintain their direction of magnetization over time. Using a scanning tunneling microscope to observe spin excitations, we determined the orientation and strength of the anisotropies of individual iron and manganese atoms on a thin layer of copper nitride. The relative intensities of the inelastic tunneling processes are consistent with dipolar interactions, as seen for inelastic neutron scattering. First-principles calculations indicate that the magnetic atoms become incorporated into a polar covalent surface molecular network in the copper nitride. These structures, which provide atom-by-atom accessibility via local probes, have the potential for engineering anisotropies large enough to produce stable magnetization at low temperatures for a single atomic spin.

The Force Needed to Move an Atom on a Surface

Manipulation of individual atoms and molecules by scanning probe microscopy offers the ability of controlled assembly at the single-atom scale. However, the driving forces behind atomic manipulation have not yet been measured. We used an atomic force microscope to measure the vertical and lateral forces exerted on individual adsorbed atoms or molecules by the probe tip. We found that the force that it takes to move an atom depends strongly on the adsorbate and the surface. Our results indicate that for moving metal atoms on metal surfaces, the lateral force component plays the dominant role. Furthermore, measuring spatial maps of the forces during manipulation yielded the full potential energy landscape of the tip-sample interaction.

The Quantum Magnetism of Individual Manganese-12-Acetate Molecular Magnets Anchored at Surfaces

The high intrinsic spin and long spin relaxation time of manganese-12-acetate (Mn(12)) makes it an archetypical single molecular magnet. While these characteristics have been measured on bulk samples, questions remain whether the magnetic properties replicate themselves in surface supported isolated molecules, a prerequisite for any application. Here we demonstrate that electrospray ion beam deposition facilitates grafting of intact Mn(12) molecules on metal as well as ultrathin insulating surfaces enabling submolecular resolution imaging by scanning tunneling microscopy. Using scanning tunneling spectroscopy we detect spin excitations from the magnetic ground state of the molecule at an ultrathin boron nitride decoupling layer. Our results are supported by density functional theory based calculations and establish that individual Mn(12) molecules retain their intrinsic spin on a well chosen solid support.

Temperature and magnetic field dependence of a Kondo system in the weak coupling regime

The Kondo effect arises due to the interaction between a localized spin and the electrons of a surrounding host. Studies of individual magnetic impurities by scanning tunneling spectroscopy have renewed interest in Kondo physics; however, a quantitative comparison with theoretical predictions remained challenging. Here we show that the zero-bias anomaly detected on an organic radical weakly coupled to a Au (111) surface can be described with astonishing agreement by perturbation theory as originally developed by Kondo 60 years ago. Our results demonstrate that Kondo physics can only be fully conceived by studying both temperature and magnetic field dependence of the resonance. The identification of a spin 1/2 Kondo system is of relevance not only as a benchmark for predictions for Kondo physics but also for correlated electron materials in general.

Spin excitations and correlations in scanning tunneling spectroscopy

In recent years inelastic spin-flip spectroscopy using a lowtemperature scanning tunneling microscope has been a very successful tool for studying not only individual spins but also complex coupled systems. When these systems interact with the electrons of the supporting substrate correlated manyparticle states can emerge, making them ideal prototypical quantum systems. The spin systems, which can be constructed by arranging individual atoms on appropriate surfaces or embedded in synthesized molecular structures, can reveal very rich spectral features. Up to now the spectral complexity has only been partly described. This manuscript shows that perturbation theory enables one to describe the tunneling transport, reproducing the differential conductance with surprisingly high accuracy. Well established scattering models, which include Kondo-like spin-spin and potential interactions, are expanded to enable calculation of arbitrary complex spin systems in reasonable time scale and the extraction of important physical properties. The emergence of correlations between spins and, in particular, between the localized spins and the supporting bath electrons are discussed and related to experimentally tunable parameters. These results might stimulate new experiments by providing experimentalists with an easily applicable modeling tool.

Quantum engineering of spin and anisotropy in magnetic molecular junctions

Single molecule magnets and single spin centres can be individually addressed when coupled to contacts forming an electrical junction. To control and engineer the magnetism of quantum devices, it is necessary to quantify how the structural and chemical environment of the junction affects the spin centre. Metrics such as coordination number or symmetry provide a simple method to quantify the local environment, but neglect the many-body interactions of an impurity spin coupled to contacts. Here, we utilize a highly corrugated hexagonal boron nitride monolayer to mediate the coupling between a cobalt spin in CoHx (x=1,2) complexes and the metal contact. While hydrogen controls the total effective spin, the corrugation smoothly tunes the Kondo exchange interaction between the spin and the underlying metal. Using scanning tunnelling microscopy and spectroscopy together with numerical simulations, we quantitatively demonstrate how the Kondo exchange interaction mimics chemical tailoring and changes the magnetic anisotropy.

Coverage-dependent self-organization: from individual adatoms to adatom superlattices

The coverage-dependent self-organization of Ce-adatoms on a Ag(111) surface is studied by scanning tunnelling microscopy at temperatures ranging from 3.9 to 10 K. At a coverage of 0.03% of a Ce monolayer individual Ce-adatoms and Ce dimers are observed, the mutual interatomic distances of which are clearly related to multiples of the Fermi wavelength λF/2, reflecting surface-state-mediated electronic interactions. At a coverage of 0.2% the formation of chains and small islands with hexagonal structure prevails. At a coverage of 1% a hexagonal superlattice with a periodicity of 3.2 nm is observed. At a coverage of 2% the superlattice of Ce-adatoms is found to be compressed, showing an interatomic distance of 2.2 nm. At higher coverage the number of dimers increases considerably and the superlattice collapses into compact islands. An increase in the temperature towards about 10 K at a coverage of 1% also causes the collapse of the hexagonal Ce superlattice. These experimental findings are rationalized within the electron scattering model of Hyldgard and Persson, which specifically takes into account the electronic surface-state on Ag(111). The experimentally derived two-body interaction potential is able to account for the observed phenomena as a function of concentration and temperature.

Tracking Temperature-Dependent Relaxation Times of Ferritin Nanomagnets with a Wideband Quantum Spectrometer

We demonstrate the tracking of the spin dynamics of ensemble and individual magnetic ferritin proteins from cryogenic up to room temperature using the nitrogen-vacancy color center in diamond as a magnetic sensor. We employ different detection protocols to probe the influence of the ferritin nanomagnets on the longitudinal and transverse relaxation of the nitrogen-vacancy center, which enables magnetic sensing over a wide frequency range from Hz to GHz. The temperature dependence of the observed spectral features can be well understood by the thermally induced magnetization reversals of the ferritin and enables the determination of the anisotropy barrier of single ferritin molecules.

Exploring the phase diagram of the two-impurity Kondo problem

A system of two exchange-coupled Kondo impurities in a magnetic field gives rise to a rich phase space hosting a multitude of correlated phenomena. Magnetic atoms on surfaces probed through scanning tunnelling microscopy provide an excellent platform to investigate coupled impurities, but typical high Kondo temperatures prevent field-dependent studies from being performed, rendering large parts of the phase space inaccessible. We present a study of pairs of Co atoms on insulating Cu2N/Cu(100), which each have a Kondo temperature of only 2.6 K. The pairs are designed to have interaction strengths similar to the Kondo temperature. By applying a sufficiently strong magnetic field, we are able to access a new phase in which the two coupled impurities are simultaneously screened. Comparison of differential conductance spectra taken on the atoms to simulated curves, calculated using a third-order transport model, allows us to independently determine the degree of Kondo screening in each phase.

Tailoring the chiral magnetic interaction between two individual atoms

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.