Steffen Rolf-Pissarczyk

Control of quantum magnets by atomic exchange bias

Mixing of discretized states in quantum magnets has a radical impact on their properties. Managing this effect is key for spintronics in the quantum limit. Magnetic fields can modify state mixing and, for example, mitigate destabilizing effects in single-molecule magnets. The exchange bias field has been proposed as a mechanism for localized control of individual nanomagnets. Here, we demonstrate that exchange coupling with the magnetic tip of a scanning tunnelling microscope provides continuous tuning of spin state mixing in an individual nanomagnet. By directly measuring spin relaxation time with electronic pump-probe spectroscopy, we find that the exchange interaction acts analogously to a local magnetic field that can be applied to a specific atom. It can be tuned in strength by up to several tesla and cancel external magnetic fields, thereby demonstrating the feasibility of complete control over individual quantum magnets with atomically localized exchange coupling.

Magnetic fingerprint of individual Fe4 molecular magnets under compression by a scanning tunnelling microscope

Single-molecule magnets (SMMs) present a promising avenue to develop spintronic technologies. Addressing individual molecules with electrical leads in SMM-based spintronic devices remains a ubiquitous challenge: interactions with metallic electrodes can drastically modify the SMMs properties by charge transfer or through changes in the molecular structure. Here, we probe electrical transport through individual Fe4 SMMs using a scanning tunnelling microscope at 0.5 K. Correlation of topographic and spectroscopic information permits identification of the spin excitation fingerprint of intact Fe4 molecules. Building from this, we find that the exchange coupling strength within the molecules magnetic core is significantly enhanced. First-principles calculations support the conclusion that this is the result of confinement of the molecule in the two-contact junction formed by the microscope tip and the sample surface.

Atomic-scale sensing of the magnetic dipolar field from single atoms

Spin resonance provides the high-energy resolution needed to determine biological and material structures by sensing weak magnetic interactions. In recent years, there have been notable achievements in detecting and coherently controlling individual atomic-scale spin centres for sensitive local magnetometry. However, positioning the spin sensor and characterizing spin-spin interactions with sub-nanometre precision have remained outstanding challenges. Here, we use individual Fe atoms as an electron spin resonance (ESR) sensor in a scanning tunnelling microscope to measure the magnetic field emanating from nearby spins with atomic-scale precision. On artificially built assemblies of magnetic atoms (Fe and Co) on a magnesium oxide surface, we measure that the interaction energy between the ESR sensor and an adatom shows an inverse-cube distance dependence (r-3.01±0.04). This demonstrates that the atoms are predominantly coupled by the magnetic dipole-dipole interaction, which, according to our observations, dominates for atom separations greater than 1 nm. This dipolar sensor can determine the magnetic moments of individual adatoms with high accuracy. The achieved atomic-scale spatial resolution in remote sensing of spins may ultimately allow the structural imaging of individual magnetic molecules, nanostructures and spin-labelled biomolecules.

Three-Dimensional Mapping of Single-Atom Magnetic Anisotropy

Magnetic anisotropy plays a key role in the magnetic stability and spin-related quantum phenomena of surface adatoms. It manifests as angular variations of the atoms magnetic properties. We measure the spin excitations of individual Fe atoms on a copper nitride surface with inelastic electron tunneling spectroscopy. Using a three-axis vector magnet we rotate the magnetic field and map out the resulting variations of the spin excitations. We quantitatively determine the three-dimensional distribution of the magnetic anisotropy of single Fe atoms by fitting the spin excitation spectra with a spin Hamiltonian. This experiment demonstrates the feasibility of fully mapping the vector magnetic properties of individual spins and characterizing complex three-dimensional magnetic systems.

Building Complex Kondo Impurities by Manipulating Entangled Spin Chains

The creation of molecule-like structures in which magnetic atoms interact controllably is full of potential for the study of complex or strongly correlated systems. Here, we create spin chains in which a strongly correlated Kondo state emerges from magnetic coupling of transition-metal atoms. We build chains up to ten atoms in length by placing Fe and Mn atoms on a Cu2N surface with a scanning tunneling microscope. The atoms couple antiferromagnetically via superexchange interaction through the nitrogen atom network of the surface. The emergent Kondo resonance is spatially distributed along the chain. Its strength can be controlled by mixing atoms of different transition metal elements and manipulating their spatial distribution. We show that the Kondo screening of the full chain by the electrons of the nonmagnetic substrate depends on the interatomic entanglement of the spins in the chain, demonstrating the prerequisites to build and probe spatially extended strongly correlated nanostructures.

Closing the superconducting gap in small Pb nanoislands with high magnetic fields

Superconducting properties change in confined geometries. Here we study the effects of strong confinement in nanosized Pb islands on Si(111)

Entanglement-induced Kondo screening in atomic spin chains

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Magnetic dipole-dipole sensing at atomic scale using electron spin resonance STM

. Small hexagonal islands with diameters less than 50 nm and a uniform height of seven atomic layers are formed by depositing Pb at low temperature and annealing at 300 K. We measure the tunneling spectra of individual Pb nanoislands using a low-temperature scanning tunneling microscope operated at 0.6 K and follow the narrowing of the superconducting gap as a function of magnetic field. We find the critical magnetic field, at which the superconducting gap vanishes, reaches several Tesla, which represents a greater than 50-fold enhancement compared to the bulk value. By independently measuring the size of the superconducting gap, and the critical magnetic field that quenches superconductivity for a range of nanoislands, we can correlate these two fundamental parameters and estimate the maximal achievable critical field for 7 ML Pb nanoislands to be 7 T.