Benjamin W. Heinrich

Visualizing the spin of individual cobalt-phthalocyanine molecules.

Low-temperature spin-polarized scanning tunneling microscopy is employed to study spin transport across single Cobalt-Phathalocyanine molecules adsorbed on well characterized magnetic nanoleads. A spin-polarized electronic resonance is identified over the center of the molecule and exploited to spatially resolve stationary spin states. These states reflect two molecular spin orientations and, as established by density functional calculations, originate from a ferromagnetic molecule-lead superexchange interaction mediated by the organic ligands.

Size-Dependent Surface States of Strained Cobalt Nanoislands on Cu(111)

Low-temperature scanning tunneling spectroscopy over Co nanoislands on Cu(111) showed that the surface states of the islands vary with their size. Occupied states exhibit a sizable downward energy shift as the island size decreases. The position of the occupied states also significantly changes across the islands. Atomic-scale simulations and ab initio calculations demonstrate that the driving force for the observed shift is related to size-dependent mesoscopic relaxations in the nanoislands.

Protection of excited spin states by a superconducting energy gap

When a paramagnetic molecule is placed on a superconducting surface the lifetime of its spin excitations increases dramatically. This effect, caused by the depletion of the electronic states within the energy gap at the Fermi level, could find application in coherent spin manipulation.

Change of the magnetic coupling of a metal-organic complex with the substrate by a stepwise ligand reaction.

The surface-assisted intramolecular ligand reaction of a porphyrin molecule adsorbed on Au(111) is studied by scanning tunneling microscopy and spectroscopy. The temperature-induced stepwise transformation of iron octaethylporphyrin proceeds via a concentric electrocyclic ring closure, with the final product iron tetrabenzoporphyrin being identified by its characteristic Kondo resonance. Along with the transformation of the organic ligand, changes in the magnetic fingerprint are observed, indicating an increasing coupling of the iron spin with the substrate electrons.

Tuning the Magnetic Anisotropy of Single Molecules

The magnetism of single atoms and molecules is governed by the atomic scale environment. In general, the reduced symmetry of the surrounding splits the d states and aligns the magnetic moment along certain favorable directions. Here, we show that we can reversibly modify the magnetocrystalline anisotropy by manipulating the environment of single iron(II) porphyrin molecules adsorbed on Pb(111) with the tip of a scanning tunneling microscope. When we decrease the tip-molecule distance, we first observe a small increase followed by an exponential decrease of the axial anisotropy on the molecules. This is in contrast to the monotonous increase observed earlier for the same molecule with an additional axial Cl ligand ( Nat. Phys. 2013 , 9 , 765 ). We ascribe the changes in the anisotropy of both species to a deformation of the molecules in the presence of the attractive force of the tip, which leads to a change in the d level alignment. These experiments demonstrate the feasibility of a precise tuning of the magnetic anisotropy of an individual molecule by mechanical control.

Tunneling Processes into Localized Subgap States in Superconductors

We combine scanning-tunneling-spectroscopy experiments probing magnetic impurities on a superconducting surface with a theoretical analysis of the tunneling processes between (superconducting) tip and substrate. We show that the current through impurity-induced Shiba bound states is carried by single-electron tunneling at large tip-substrate distances and Andreev reflections at smaller distances. The single-electron current requires relaxation processes, allowing us to extract information on quasiparticle transitions and lifetimes.

Experimental demonstration of a two-band superconducting state for lead using scanning tunneling spectroscopy.

The type I superconductor lead (Pb) has been theoretically predicted to be a two-band superconductor. We use scanning tunneling spectroscopy (STS) to resolve two superconducting gaps with an energy difference of 150  μeV. Tunneling into Pb(111), Pb(110), and Pb(100) crystals reveals a strong dependence of the two coherence peak intensities on the crystal orientation. We show that this is the result of a selective tunneling into the two bands at the energy of the two coherence peaks. This is further sustained by the observation of signatures of the Fermi sheets in differential conductance maps around subsurface defects. A modification of the density of states of the two bands by adatoms on the surface confirms the different orbital character of each of the two subbands.

Magnetic anisotropy in Shiba bound states across a quantum phase transition

The exchange coupling between magnetic adsorbates and a superconducting substrate leads to Shiba states inside the superconducting energy gap and a Kondo resonance outside the gap. The exchange coupling strength determines whether the quantum many-body ground state is a Kondo singlet or a singlet of the paired superconducting quasiparticles. Here we use scanning tunnelling spectroscopy to identify the different quantum ground states of manganese phthalocyanine on Pb(111). We observe Shiba states, which are split into triplets by magnetocrystalline anisotropy. Their characteristic spectral weight yields an unambiguous proof of the nature of the quantum ground state. Our results provide experimental insights into the phase diagram of a magnetic impurity on a superconducting host and shine light on the effects induced by magnetic anisotropy on many-body interactions.

Orbital Picture of Yu-Shiba-Rusinov Multiplets

We investigate the nature of Yu-Shiba-Rusinov (YSR) subgap states induced by single manganese (Mn) atoms adsorbed on different surface orientations of superconducting lead (Pb). Depending on the adsorption site, we detect a distinct number and characteristic patterns of YSR states around the Mn atoms. We suggest that the YSR states inherit their properties from the Mn d levels, which are split by the surrounding crystal field. The periodicity of the long-range YSR oscillations allows us to identify a dominant coupling of the d states to the outer Fermi sheet of the two-band superconductor Pb.

Exploring a Proximity-Coupled Co Chain on Pb(110) as a Possible Majorana Platform

Linear chains of magnetic atoms proximity coupled to an s-wave superconductor are predicted to host Majorana zero modes at the chain ends in the presence of strong spin–orbit coupling. Specifically, iron (Fe) chains on Pb(110) have been explored as a possible system to exhibit topological superconductivity and host Majorana zero modes [Nadj-PergeS. et al., Science2014, 346, 602−60725278507]. Here, we study chains of the transition metal cobalt (Co) on Pb(110) and check for topological signatures. Using spin-polarized scanning tunneling spectroscopy, we resolve ferromagnetic order in the d bands of the chains. Interestingly, also the subgap Yu–Shiba–Rusinov (YSR) bands carry a spin polarization as was predicted decades ago. Superconducting tips allow us to resolve further details of the YSR bands and in particular resonances at zero energy. We map the spatial distribution of the zero-energy signal and find it delocalized along the chain. Hence, despite the ferromagnetic coupling within the chains and the strong spin-orbit coupling in the superconductor, we do not find clear evidence of Majorana modes. Simple tight-binding calculations suggest that the spin–orbit–split bands may cross the Fermi level four times which suppresses the zero-energy modes.