Interfering Tunneling Paths through Magnetic Molecules on Superconductors: Asymmetries of Kondo and Yu-Shiba-Rusinov Resonances.

Magnetic adsorbates on superconductors induce a Kondo resonance outside and Yu-Shiba-Rusinov (YSR) bound states inside the superconducting energy gap. When probed by scanning tunneling spectroscopy, the associated differential-conductance spectra frequently exhibit characteristic bias-voltage asymmetries. Here, we observe correlated variations of Kondo and YSR asymmetries across an Fe-porphyrin molecule adsorbed on Pb(111).

Highly customized 1010 nm, ns-pulsed Yb-doped fiber amplifier as a key tool for on-demand single-photon generation.

The development of highly customized technical devices is a decisive feature of technically complex setups, as frequently observed in quantum experiments. This paper describes the development and realization of an Yb-doped all-fiber amplifier system designed for such a special application, more specifically, an on-demand single-photon source based on four-wave mixing with rubidium Rydberg atoms. The laser is capable of generating bandwidth-limited configurable nanosecond pulses up to peak powers of >100 W and with pulse repetition frequencies (PRF) between 50 Hz and 1 MHz at selectable wavelengths (1008-1024 nm).

Surface-orientation- and ligand-dependent quenching of the spin magnetic moment of Co porphyrins adsorbed on Cu substrates.

Porphyrin molecules are particularly interesting candidates for spintronic applications due to their bonding flexibility, which allows to modify their properties substantially by the addition or transformation of ligands. Here, we investigate the electronic and magnetic properties of cobalt octaethylporphyrin (CoOEP), deposited on copper substrates with two distinct crystallographic surface orientations, Cu(100) and Cu(111), with X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD). A significant magnetic moment is present in the Co ions of the molecules deposited on Cu(100), but it is completely quenched on Cu(111).

Yu-Shiba-Rusinov States in the Charge-Density Modulated Superconductor NbSe.

NbSe is a remarkable superconductor in which charge-density order coexists with pairing correlations at low temperatures. Here, we study the interplay of magnetic adatoms and their Yu-Shiba-Rusinov (YSR) bound states with the charge density order. Exploiting the incommensurate nature of the charge-density wave (CDW), our measurements provide a thorough picture of how the CDW affects both the energies and the wave functions of the YSR states.

Tuning the Coupling of an Individual Magnetic Impurity to a Superconductor: Quantum Phase Transition and Transport.

The exchange scattering at magnetic adsorbates on superconductors gives rise to Yu-Shiba-Rusinov (YSR) bound states. Depending on the strength of the exchange coupling, the magnetic moment perturbs the Cooper pair condensate only weakly, resulting in a free-spin ground state, or binds a quasiparticle in its vicinity, leading to a (partially) screened spin state. Here, we use the flexibility of Fe-porphin (FeP) molecules adsorbed on a Pb(111) surface to reversibly and continuously tune between these distinct ground states.

Visualizing Intramolecular Distortions as the Origin of Transverse Magnetic Anisotropy.

The magnetic properties of metal-organic complexes are strongly influenced by conformational changes in the ligand. The flexibility of Fe-tetra-pyridyl-porphyrin molecules leads to different adsorption configurations on a Au(111) surface. By combining low-temperature scanning tunneling spectroscopy and atomic force microscopy, we resolve a correlation of the molecular configuration with different spin states and magnitudes of magnetic anisotropy.

Wave-Function Hybridization in Yu-Shiba-Rusinov Dimers.

Magnetic adsorbates on superconductors induce local bound states within the superconducting gap. These Yu-Shiba-Rusinov (YSR) states decay slowly away from the impurity compared to atomic orbitals, even in 3D bulk crystals. Here, we use scanning tunneling spectroscopy to investigate their hybridization between two nearby magnetic Mn adatoms on a superconducting Pb(001) surface.

Control of Oxidation and Spin State in a Single-Molecule Junction.

The oxidation and spin state of a metal-organic molecule determine its chemical reactivity and magnetic properties. Here, we demonstrate the reversible control of the oxidation and spin state in a single Fe porphyrin molecule in the force field of the tip of a scanning tunneling microscope. Within the regimes of half-integer and integer spin state, we can further track the evolution of the magnetocrystalline anisotropy.

Scaling of Yu-Shiba-Rusinov energies in the weak-coupling Kondo regime.

The competition of the free-spin state of a paramagnetic impurity on a superconductor with its screened counterpart is characterized by the energy scale of Kondo screening compared to the superconducting pairing energy Δ. When the experimental temperature suppresses Kondo screening, but preserves superconductivity, i.e.

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-Perge , S. et al.

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.

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).

End States and Subgap Structure in Proximity-Coupled Chains of Magnetic Adatoms.

A recent experiment [Nadj-Perge et al., Science 346, 602 (2014)] provides evidence for Majorana zero modes in iron (Fe) chains on the superconducting Pb(110) surface. Here, we study this system by scanning tunneling microscopy using superconducting tips.

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.

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.

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.

Magnetic coupling of Gd3N@C80 endohedral fullerenes to a substrate.

Using magnetic endohedral fullerenes for molecular spintronics requires control over their encapsulated magnetic moments. We show by field-dependent x-ray magnetic circular dichroism measurements of Gd3N@C80 endohedral fullerenes adsorbed on a Cu surface that the magnetic moments of the encapsulated Gd atoms lie in a 4f7 ground state and couple ferromagnetically to each other. When the molecules are in contact with a ferromagnetic Ni substrate, we detect two different Gd species.

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.