Suchergebnisse

A magnetic atom inside a superconductor locally distorts superconductivity. It scatters Cooper pairs as a potential with broken time-reversal symmetry, leading to localized bound states with subgap excitation energies, named Shiba states. Most conventional approaches regarding Shiba states treat magnetic impurities as point scatterers with isotropic exchange interaction. Here, we show that the number and the shape of Shiba states are correlated to the spin-polarized atomic orbitals of the impurity, hybridized with the superconductor. Using scanning tunnelling spectroscopy, we spatially map the five Shiba excitations found on subsurface chromium atoms in Pb(111), resolving their particle and hole components. While particle components resemble d orbitals of embedded Cr atoms, hole components differ strongly from them. Density functional theory simulations correlate the orbital shapes to the magnetic ground state of the atom, and identify scattering channels and interactions, all valuable tools for designing atomic-scale superconducting devices. ; D.-J.C. acknowledges the European Union for support under the H2020-MSCA-IF-2014 Marie-Curie Individual Fellowship programme proposal number 654469. We acknowledge financial support from Spanish MINECO (Grants No MAT2015-66888-C3-2-R, MAT2014-60996-R and MAT2013-46593-C6-1-P) and Diputacion Foral de Gipuzkoa for Grant No 64/15. ; Peer Reviewed

We show that the magnetic ordering of coupled atomic dimers on a superconductor is revealed by their intragap spectral features. Chromium atoms on the superconductor β-Bi2Pd surface display Yu-Shiba-Rusinov bound states, detected as pairs of intragap excitations in tunneling spectra. By means of atomic manipulation with a scanning tunneling microscope's tip, we form Cr dimers with different arrangements and find that their intragap features appear either shifted or split with respect to single atoms. These spectral variations are associated with the magnetic coupling, ferromagnetic or antiferromagnetic, of the dimer, as confirmed by density functional theory simulations. The striking qualitative differences between the observed tunneling spectra prove that intragap Shiba states are extremely sensitive to the magnetic ordering on the atomic scale ; We thank Javier Zaldivar and Joeri de Bruijckere for developing the deconvolution process and Sebastian Bergeret for discussions. D.-J. C. and J. I. P. thank the European Union for support under the H2020-MSCA-IF-2014 Marie-Curie Individual Fellowship program (Proposal No. 654469), Spanish MINECO (MAT2016-78293-C6-1-R), Diputacion Foral de Gipuzkoa for Grant No. 64/15, and the European Regional Development Fund (ERDF). N. L. thanks Spanish MINECO (Grant No. MAT2015-66888-C3-2-R). M. M. U. acknowledges Spanish MINECO (MAT2014-60996-R). E. H., I. G., and H. S. acknowledge FIS2014-54498-R and MDM-2014-0377, COST MP16218 nanocohybri, ERC PNICTEYES Grant Agreement No. 679080, and Departamento Administrativo de Ciencia, Tecnología e Innovación, COLCIENCIAS (Colombia), Programa doctorados en el exterior and convocatoria 568-2012, as well as Comunidad de Madrid through program Nanofrontmag-CM (Grant No. S2013/MIT-2850)

We show that the magnetic ordering of coupled atomic dimers on a superconductor is revealed by their intragap spectral features. Chromium atoms on the superconductor β−Bi2Pd surface display Yu-Shiba-Rusinov bound states, detected as pairs of intragap excitations in tunneling spectra. By means of atomic manipulation with a scanning tunneling microscope's tip, we form Cr dimers with different arrangements and find that their intragap features appear either shifted or split with respect to single atoms. These spectral variations are associated with the magnetic coupling, ferromagnetic or antiferromagnetic, of the dimer, as confirmed by density functional theory simulations. The striking qualitative differences between the observed tunneling spectra prove that intragap Shiba states are extremely sensitive to the magnetic ordering on the atomic scale. ; D.-J. C. and J. I. P. thank the European Union for support under the H2020-MSCA-IF2014 Marie-Curie Individual Fellowship program (Proposal No. 654469), Spanish MINECO (MAT2016-78293-C6-1-R), Diputacion Foral de Gipuzkoa for Grant No. 64/15, and the European Regional Development Fund (ERDF). N. L. thanks Spanish MINECO (Grant No. MAT2015-66888-C3-2-R). M. M. U. acknowledges Spanish MINECO (MAT2014-60996-R). E. H., I. G., and H. S. acknowledge FIS2014-54498-R and MDM-2014-0377, COST MP16218 nanocohybri, ERC PNICTEYES Grant Agreement No. 679080, and Departamento Administrativo de Ciencia, Tecnología e Innovación, COLCIENCIAS (Colombia), Programa doctorados en el exterior and convocatoria 568-2012, as well as Comunidad de Madrid through program NanofrontmagCM (Grant No. S2013/MIT-2850). ; Peer reviewed

Scattering of electrons by localized spins is the ultimate process enabling detection and control of the magnetic state of a spin-doped material. At the molecular scale, scattering is mediated by the orbitals hosting the spin. Here we report the selective excitation of a molecular spin by tunneling through different molecular orbitals. Spatially resolved tunneling spectra on iron-porphyrins reveal that the inelastic spin excitation extends beyond the iron site, changing shape and symmetry along the molecule. Combining density functional theory simulations with a phenomenological scattering model, we show that the extension and lineshape of the inelastic signal are due to excitation pathways assisted by different frontier orbitals. By selecting the intramolecular site for electron injection, the relative weight of iron and pyrrole orbitals in the tunneling process is modified. Thus, the excitation mechanism, reflected by its spectral lineshape, depends on the degree of localization and energy alignment of the chosen molecular orbital. ; This work has been funded by the COST 15128 Molecular Spintronics project, by Marie Curie IF ARTE, by the Spanish Ministerio de Economía y Competitividad (MINECO) through the cooperative grant No. MAT2016-78293 and grant No. FIS2016-75862-P, and by the Basque Government (Dep. Industry, Grant PI-2015-1-42, Dep. Education, Grant PI-2016-1-27 and Grant IT-756-13), the EU project PAMS (610446), and the European Regional Development Fund (ERDF). ; Peer reviewed

Scattering of electrons by localized spins is the ultimate process enabling detection and control of the magnetic state of a spin-doped material. At the molecular scale, scattering is mediated by the orbitals hosting the spin. Here we report the selective excitation of a molecular spin by tunneling through different molecular orbitals. Spatially resolved tunneling spectra on iron-porphyrins reveal that the inelastic spin excitation extends beyond the iron site, changing shape and symmetry along the molecule. Combining density functional theory simulations with a phenomenological scattering model, we show that the extension and lineshape of the inelastic signal are due to excitation pathways assisted by different frontier orbitals. By selecting the intramolecular site for electron injection, the relative weight of iron and pyrrole orbitals in the tunneling process is modified. Thus, the excitation mechanism, reflected by its spectral lineshape, depends on the degree of localization and energy alignment of the chosen molecular orbital. ; This work has been funded by the COST 15128 Molecular Spintronics project, by Marie Curie IF ARTE, by the Spanish Ministerio de Economía y Competitividad (MINECO) through the cooperative grant No. MAT2016-78293 and grant No. FIS2016-75862-P, and by the Basque Government (Dep. Industry, Grant PI-2015-1-42, Dep. Education, Grant PI-2016-1-27 and Grant IT-756-13), the EU project PAMS (610446), and the European Regional Development Fund (ERDF).

Vertically stacked two-dimensional (2D) heterostructures composed of 2D semiconductors have attracted great attention. Most of these include hexagonal boron nitride (h-BN) as either a substrate, an encapsulant, or a tunnel barrier. However, reliable synthesis of large-area and epitaxial 2D heterostructures incorporating BN remains challenging. Here, we demonstrate the epitaxial growth of nominal monolayer (ML) MoSe2 on h-BN/Rh(111) by molecular beam epitaxy, where the MoSe2/h-BN layer system can be transferred from the growth substrate onto SiO2. The valence band structure of ML MoSe2/h-BN/Rh(111) revealed by photoemission electron momentum microscopy (kPEEM) shows that the valence band maximum located at the K point is 1.33 eV below the Fermi level (EF), whereas the energy difference between K and Γ points is determined to be 0.23 eV, demonstrating that the electronic properties, such as the direct band gap and the effective mass of ML MoSe2, are well preserved in MoSe2/h-BN heterostructures. ; The access was provided by the NFFA-Europe Infrastructure (proposal ID 121) under Horizon 2020 EU Funding Program. We thank N. Gambacorti for coordinating the access to the NFFA-EU program. This work was financially supported by the European Research Council (Grant No. 240076) and has received funding from the European Union's Horizon 2020 research and innovation programme under Grant Agreement Nos. 696656 and 785219 (Graphene Flagship Core 1 and Core 2). M.P. acknowledges support by the Swiss National Science Foundation (Grant No. 200021-162612). ; Peer reviewed

Chalcogen vacancies are generally considered to be the most common point defects in transition metal dichalcogenide (TMD) semiconductors because of their low formation energy in vacuum and their frequent observation in transmission electron microscopy studies. Consequently, unexpected optical, transport, and catalytic properties in 2D-TMDs have been attributed to in-gap states associated with chalcogen vacancies, even in the absence of direct experimental evidence. Here, we combine low-temperature non-contact atomic force microscopy, scanning tunneling microscopy and spectroscopy, and state-of-the-art ab initio density functional theory and GW calculations to determine both the atomic structure and electronic properties of an abundant chalcogen-site point defect common to MoSe and WS monolayers grown by molecular beam epitaxy and chemical vapor deposition, respectively. Surprisingly, we observe no in-gap states. Our results strongly suggest that the common chalcogen defects in the described 2D-TMD semiconductors, measured in vacuum environment after gentle annealing, are oxygen substitutional defects, rather than vacancies. ; This work was supported by the Center for Computational Study of Excited State Phenomena in Energy Materials (C2SEPEM), which is funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division under Contract No. DE-AC02-05CH11231, as part of the Computational Materials Sciences Program. Work performed at the Molecular Foundry was also supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under the same contract number. S.B. acknowledges fellowship support by the European Union under FP7-PEOPLE-2012-IOF-327581. S.B. and M.M.U acknowledge Spanish MINECO (MAT2017-88377-C2-1-R). S.R.A acknowledges Rothschild and Fulbright fellowships. B.S. appreciates support from the Swiss National Science Foundation under project number P2SKP2_171770. A.P. and O.V.Y. acknowledge support by the ERC Starting grant "TopoMat" (Grant No. 306504). M.F.C. acknowledges support from the U.S. National Science Foundation under project number EFMA-1542741. C.H. acknowledges support from NRF grant funded by the Korea government (MSIT) (No. 2018R1A2B6004538). DFT calculations were performed at the Swiss National Supercomputing Centre (CSCS) under project s832 and the facilities of Scientific IT and Application Support Center of EPFL. This research used resources of the National Energy Research Scientific Computing Center (NERSC), a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231 for the GW calculations. This research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under contract no. DE-AC02-05CH11231.