A magnetic atom in a superconducting host induces so-called Yu-Shiba-Rusinov (YSR) bound states inside the superconducting energy gap. By combining spin-resolved scanning tunneling spectroscopy with simulations we demonstrate that the pair of peaks associated with the YSR states of an individual Fe atom coupled to an oxygen-reconstructed Ta surface gets spin polarized in an external magnetic field. As theoretically predicted, the electron and hole parts of the YSR states have opposite signs of spin polarizations which keep their spin character when crossing the Fermi level through the quantum phase transition. The simulation of a YSR state right at the Fermi level reveals zero spin polarization which can be used to distinguish such states from Majorana zero modes in chains of YSR atoms. DOI: 10.1103/PhysRevLett.119.197002 Recent investigations of chains [1][2][3] and arrays [4,5] of magnetic atoms in contact with surfaces of s-wave superconductors in view of Majorana zero modes and topological superconductivity triggered renewed interest in the properties of the basic constituent of such systems, the individual magnetic adatom. Typically, such adatoms induce quasiparticle excitations inside the superconducting energy gap [6][7][8], referred to as Yu-Shiba-Rusinov (YSR) states, which hamper the identification of topologically nontrivial edge states [3,9], calling for a thorough characterization of all experimentally accessible properties of YSR states.Following the first experimental verification of YSR states of individual atoms using scanning tunneling spectroscopy (STS) [10], there were numerous experimental studies, focusing on orbital effects [11][12][13], magnetic anisotropy [14], effects of reduced dimensionality of the superconductor [15], effects of coupling [11,16], and the competition between Kondo screening and superconducting pairing [17,18]. However, the investigation of the spin polarization of the YSR state of individual atoms, which could serve as a fingerprint for the distinction from topological states [19], was so far restricted to theoretical predictions [6][7][8][20][21][22].Neglecting orbital effects or magnetic anisotropy, theory predicts one pair of spin-polarized states of a YSR atom, an electron (e − )-and a hole (h)-like part with opposite spin character, which are located at AEjεj from the Fermi level E F [20]. There is a pronounced asymmetry in spectral weight between the e − and h parts due to electron-hole asymmetry of the band structure [21,22] and/or a nonmagnetic scattering potential of the impurity [20,23]. With increasing exchange coupling J between the adatom and substrate, the binding energy ε decreases until the YSR states eventually cross E F through a quantum phase transition (QPT), accompanied by an inversion of the asymmetry in the e − − h spectral weight [17]. Most notably, since both parts of the YSR states keep their spin character, the spin polarization above and below E F is expected to invert [20] through the QPT. Here, we experimentally verify these prediction...

Magnetic atoms on a superconductor give rise to Yu-Shiba-Rusinov (YSR) states within the superconducting energy gap. A spin chain of magnetic adatoms on an s-wave superconductor may lead to topological superconductivity accompanied by the emergence of Majorana modes at the chain ends. For their usage in quantum computation, it is a prerequisite to artificially assemble the chains and control the exchange couplings between the spins in the chain and in the substrate. Here, using a scanning tunneling microscope tip, we demonstrate engineering of the energy levels of the YSR states by placing interstitial Fe atoms in close proximity to adsorbed Fe atoms on an oxidized Ta surface. Based on this prototype platform, we show that the interaction within a long chain can be strengthened by linking the adsorbed Fe atoms with the interstitial ones. Our work adds an important step towards the controlled design and manipulation of Majorana end states.

The discovery of high-temperature superconductivity in Fe-based compounds triggered numerous investigations on the interplay between superconductivity and magnetism, and on the enhancement of transition temperatures through interface effects. It is widely believed that the emergence of optimal superconductivity is intimately linked to the suppression of long-range antiferromagnetic (AFM) order, although the exact microscopic picture remains elusive because of the lack of atomically resolved data. Here we present spin-polarized scanning tunnelling spectroscopy of ultrathin FeTe1−xSex (x=0, 0.5) films on bulk topological insulators. Surprisingly, we find an energy gap at the Fermi level, indicating superconducting correlations up to Tc∼6 K for one unit cell FeTe grown on Bi2Te3, in contrast to the non-superconducting bulk FeTe. The gap spatially coexists with bi-collinear AFM order. This finding opens perspectives for theoretical studies of competing orders in Fe-based superconductors and for experimental investigations of exotic phases in superconducting layers on topological insulators.

Establishing the relation between ubiquitous antiferromagnetism in the parent compounds of unconventional superconductors and their superconducting phase is important for understanding the complex physics in these materials. Going from bulk systems to thin films additionally affects their phase diagram. For Fe1+yTe, the parent compound of Fe1+ySe1−xTex superconductors, bulk-sensitive neutron diffraction revealed an in-plane oriented diagonal double-stripe antiferromagnetic spin structure. Here we show by spin-resolved scanning tunnelling microscopy that the spin direction at the surfaces of bulk Fe1+yTe and thin films grown on the topological insulator Bi2Te3 is canted out of the high-symmetry directions of the surface unit cell resulting in a perpendicular spin component, keeping the diagonal double-stripe order. As the magnetism of the Fe d-orbitals is intertwined with the superconducting pairing in Fe-based materials, our results imply that the superconducting properties at the surface of the related superconducting compounds might be different from the bulk.

Mutually interacting magnetic atoms coupled to a superconductor have gained enormous interest due to their potential for the realization of topological superconductivity. Individual magnetic impurities produce states within the superconducting energy gap known as Yu–Shiba–Rusinov (YSR) states. Here, using the tip of a scanning tunneling microscope, we artificially craft spin arrays consisting of an Fe adatom interacting with an assembly of interstitial Fe atoms (IFA) on a superconducting oxygen-reconstructed Ta(100) surface and show that the magnetic interaction between the adatom and the IFA assembly can be tuned by adjusting the number of IFAs in the assembly. The YSR state experiences a characteristic crossover in its energetic position and particle–hole spectral weight asymmetry when the Kondo resonance shows spectral depletion around the Fermi energy. By the help of slave-boson mean-field theory (SBMFT) and numerical renormalization group (NRG) calculations we associate the crossover with the transition from decoupled Kondo singlets to an antiferromagnetic ground state of the Fe adatom spin and the IFA assembly effective spin.