Band-Resolved Double Photoemission Spectroscopy on Correlated Valence Electron Pairs in Metals.

Correlated valence electrons in Ag and Cu are investigated using double photoemission spectroscopy driven by a high-order harmonic light source. Electron pairs consisting of two d electrons as well as pairs with one sp and one d electron are resolved in the two-dimensional energy spectrum. Surprisingly, the intensity ratio of sp-d to d-d pairs from Ag is 3 times higher than in the self-convoluted density of states. Our results directly show the band-resolved configurations of electron pairs in solids and emphasize a band-dependent picture for electron correlation even in these paradigmatic metals.

Modifying the Surface of a Rashba-Split Pb-Ag Alloy Using Tailored Metal-Organic Bonds.

Hybridization-related modifications of the first metal layer of a metal-organic interface are difficult to access experimentally and have been largely neglected so far. Here, we study the influence of specific chemical bonds (as formed by the organic molecules CuPc and PTCDA) on a Pb-Ag surface alloy. We find that delocalized van der Waals or weak chemical π-type bonds are not strong enough to alter the alloy, while localized σ-type bonds lead to a vertical displacement of the Pb surface atoms and to changes in the alloy's surface band structure. Our results provide an exciting platform for tuning the Rashba-type spin texture of surface alloys using organic molecules.

Phase-locked MHz pulse selector for x-ray sources.

Picosecond x-ray pulses are extracted with a phase-locked x-ray pulse selector at 1.25 MHz repetition rate from the pulse trains of the accelerator-driven multiuser x-ray source BESSY II preserving the peak brilliance at high pulse purity. The system consists of a specially designed in-vacuum chopper wheel rotating with ≈1 kHz angular frequency. The wheel is driven in an ultrahigh vacuum and is levitated on magnetic bearings being capable of withstanding high centrifugal forces. Pulses are picked by 1252 high-precision slits of 70 µm width on the outer rim of the wheel corresponding to a temporal opening window of the chopper of 70 ns. We demonstrate how the electronic phase stabilization of ±2 ns together with an arrival time jitter of the individual slits of the same order of magnitude allows us to pick short single bunch x-ray pulses out of a 200 ns ion clearing gap in a multibunch pulse train as emitted from a synchrotron facility at 1.25 MHz repetition rate with a pulse purity below the shot noise detection limit. The approach is applicable to any high-repetition pulsed radiation source, in particular in the x-ray spectral range up to 10 keV. The opening window in a real x-ray beamline, its stability, as well as the limits of mechanical pulse picking techniques in the MHz range are discussed.

Optical Generation of Hot Spin-Polarized Electrons from a Ferromagnetic Two-Dimensional Electron Gas.

Linearly polarized light with an energy of 3.1 eV has been used to excite highly spin-polarized electrons in an ultrathin film of face-centered-tetragonal cobalt to majority-spin quantum well states (QWS) derived from an sp band at the border of the Brillouin zone. The spin-selective excitation process has been studied by spin- and momentum-resolved two-photon photoemission. Analyzing the photoemission patterns in two-dimensional momentum planes, we find that the optically driven transition from the valence band to the QWS acts almost exclusively on majority-spin electrons. The mechanism providing the high spin polarization is discussed by the help of a density-functional theory calculation. Additionally, a sizable effect of spin-orbit coupling for the QWS is evidenced.

Separating Exchange Splitting from Spin Mixing in Gadolinium by Femtosecond Laser Excitation.

Employing spin-, time-, and energy-resolved photoemission spectroscopy, we present the first study on the spin polarization of a single electronic state after ultrafast optical excitation. Our investigation concentrates on the majority-spin component of the d-band-derived Gd(0001) surface state d(z(2))(↑). While its binding energy shows a rapid Stoner-like shift by 90 meV with an exponential time constant of τ(E)=0.6±0.1 ps, the d(z(2))(↑) spin polarization remains nearly constant within the first picoseconds and decays with τ(S)=15±8 ps. This behavior is in clear contrast to the equilibrium phase transition, where the spin polarization vanishes at the Curie temperature.

Nanoscale photoelectron mapping and spectroscopy with an atomic force microscope.

The tip of an atomic force microscope is used as a local probe for photoelectrons excited by laser illumination. The tip-sample distance is precisely controlled by the van der Waals force and the pure photoemission current is measured without tunneling current contribution. The nanoscale photoelectron mapping with high current contrast is obtained on a cesium covered Au(111) surface. By sweeping the laser photon energy, the local photoelectron spectra are measured on Cs islands and terraces. The results reveal distinct electronic states and photoemission thresholds for different Cs coverage, providing the photoemission current contrast mechanism. The contrast in photoelectron mapping can be further tuned by the incident laser polarization exploiting the symmetry selection rules in the optical excitation.

Magnetoelectric charge trap memory.

It is demonstrated that a charge-trapping layer placed in proximity to a ferromagnetic metal enables efficient electrical and optical control of the metal's magnetic properties. Retention of charge trapped inside the charge-trapping layer provides nonvolatility to the magnetoelectric effect and enhances its efficiency by an order of magnitude. As such, an engineered charge-trapping layer can be used to realize the magnetoelectric equivalent to today's pervasive charge trap flash memory technology. Moreover, by supplying trapped charges optically instead of electrically, a focused laser beam can be used to imprint the magnetic state into a continuous metal film.

Spatially modulated tunnel magnetoresistance on the nanoscale.

We investigate the local tunnel magnetoresistance (TMR) effect within a single Co nanoisland using spin-polarized scanning tunneling microscopy. We observe a clear spatial modulation of the TMR ratio with an amplitude of ~20% and a spacing of ~1.3 nm between maxima and minima around the Fermi level. This result can be ascribed to a spatially modulated spin polarization within the Co island due to spin-dependent quantum interference. Our combined experimental and theoretical study reveals that spin-dependent electron confinement affects all transport properties such as differential conductance, conductance, and TMR. We demonstrate that the TMR within a nanostructured magnetic tunnel junction can be controlled on a length scale of 1 nm through spin-dependent quantum interference.

The role of surface stress in structural transitions, epitaxial growth and magnetism on the nanoscale.

We review results on combined stress measurements by the crystal curvature technique and structural investigations on different nanoscale systems. It is shown that stress measurements offer highly sensitive and accurate data which identify even subtle structural changes in the sub-monolayer coverage regime. We discuss the unique potential of stress measurements to complement structural investigations of atomic layers and at surfaces. Our examples reveal that stress measurements enhance, support and clarify the interpretation of quantitative structural data. The role of surface stress and film stress for structural transitions in epitaxial growth, surfactant-mediated growth, surface reconstruction and adsorbate-induced spin reorientation transitions in monolayers is discussed.

Imaging properties of hemispherical electrostatic energy analyzers for high resolution momentum microscopy.

Hemispherical deflection analyzers are the most widely used energy filters for state-of-the-art electron spectroscopy. Due to the high spherical symmetry, they are also well suited as imaging energy filters for electron microscopy. Here, we review the imaging properties of hemispherical deflection analyzers with emphasis on the application for cathode lens microscopy. In particular, it turns out that aberrations, in general limiting the image resolution, cancel out at the entrance and exit of the analyzer. This finding allows more compact imaging energy filters for momentum microscopy or photoelectron emission microscopy. For instance, high resolution imaging is possible, using only a single hemisphere. Conversely, a double pass hemispherical analyzer can double the energy dispersion, which means it can double the energy resolution at certain transmission, or can multiply the transmission at certain energy resolution.

Cantilever measurements of surface stress, surface reconstruction, film stress and magnetoelastic stress of monolayers.

We review the application of cantilever-based stress measurements in surface science and magnetism. The application of thin (thickness appr. 0.1 mm) single crystalline substrates as cantilevers has been used successfully to measure adsorbate-induced surface stress changes, lattice misfit induced film stress, and magneto-elastic stress of ferromagnetic monolayers. Surface stress changes as small as 0.01 N/m can be readily measured, and this translates into a sensitivity for adsorbate-coverage well below 0.01 of one layer. Stress as large as several GPa, beyond the elasticity limits of high strength materials, is measured, and it is ascribed to the lattice misfit between film and substrate. Our results point at the intimate relation between surface stress and surface reconstruction, stress-induced structural changes in epitaxially strained films, and strain-induced modifications of the magneto-elastic coupling in ferromagnetic monolayers.

Nonlocal electron correlations in an itinerant ferromagnet.

Our understanding of the properties of ferromagnetic materials, widely used in spintronic devices, is fundamentally based on their electronic band structure. However, even for the most simple elemental ferromagnets, electron correlations are prevalent, requiring descriptions of their electronic structure beyond the simple picture of independent quasi-particles. Here, we give evidence that in itinerant ferromagnets like cobalt these electron correlations are of nonlocal origin, manifested in a complex self-energy Σσ(E,k) that disperses as function of spin σ, energy E, and momentum vector k. Together with one-step photoemission calculations, our experiments allow us to quantify the dispersive behaviour of the complex self-energy over the whole Brillouin zone. At the same time we observe regions of anomalously large "waterfall"-like band renormalization, previously only attributed to strong electron correlations in high-TC superconductors, making itinerant ferromagnets a paradigmatic test case for the interplay between band structure, magnetism, and many-body correlations.

Impact of orthogonal exchange coupling on magnetic anisotropy in antiferromagnetic oxides/ferromagnetic systems.

The influence of interface exchange coupling on magnetic anisotropy in the antiferromagnetic oxide/Ni system is investigated. We show how interfacial exchange coupling can be employed not only to pin the magnetization of the ferromagnetic layer but also to support magnetic anisotropy to orient the easy magnetization axis perpendicular to the film plane. The fact that this effect is only observed below the Néel temperature of all investigated antiferromagnetic oxides with significantly different magnetocrystalline anisotropies gives evidence that antiferromagnetic ordering is a source of the additional contribution to the perpendicular effective magnetic anisotropy.

Spin-texture inversion in the giant Rashba semiconductor BiTeI.

Semiconductors with strong spin-orbit interaction as the underlying mechanism for the generation of spin-polarized electrons are showing potential for applications in spintronic devices. Unveiling the full spin texture in momentum space for such materials and its relation to the microscopic structure of the electronic wave functions is experimentally challenging and yet essential for exploiting spin-orbit effects for spin manipulation. Here we employ a state-of-the-art photoelectron momentum microscope with a multichannel spin filter to directly image the spin texture of the layered polar semiconductor BiTeI within the full two-dimensional momentum plane. Our experimental results, supported by relativistic ab initio calculations, demonstrate that the valence and conduction band electrons in BiTeI have spin textures of opposite chirality and of pronounced orbital dependence beyond the standard Rashba model, the latter giving rise to strong optical selection-rule effects on the photoelectron spin polarization. These observations open avenues for spin-texture manipulation by atomic-layer and charge carrier control in polar semiconductors.

Topological frustrations in Mn films on Fe(001).

The high lateral resolution of spin-polarized scanning tunneling microscopy allows new insights into the spin structure of antiferromagnets on the nanometer range. We demonstrate the capability to image a well-defined in-plane component of the sample spin polarization and discuss the spin structure of antiferromagnetic bct Mn in contact with the ferromagnetic Fe(001) substrate. Mn atoms couple ferromagnetically within a Mn atomic plane, while normal to the surface a layer-wise antiferromagnetic order was found. Magnetic frustrations arise in this system at Fe substrate steps at the interface, where topologically induced 180 degrees domain walls are created in the Mn film. A clear widening of the enforced domain walls with increasing Mn thickness was found. The measured widths could be fitted with a linear function and are explained on the basis of a Heisenberg model.

Spin resolved bandstructure imaging with a high resolution momentum microscope.

We present a spin resolving "momentum microscope" for the high resolution imaging of the momentum distribution of photoelectrons. Measurements of the band structure of a Au(111) single crystal surface demonstrate an energy resolution of ΔE=12 meV and a momentum resolution of Δk∥=0.0049 Å(-1), measured at the line-width of the spin-orbit split Shockley surface state. The relative accuracy of the k∥ measurement in the order of 10(-4) Å(-1) reveals a deviation from the ideal two-dimensional free electron gas model of the Shockley surface state, manifested in a threefold radial symmetry. Spin resolution in the full momentum image is obtained by an imaging spin-filter based on low-energy electron diffraction at a Au passivated Ir(100) single crystal. Using working points at 10.5 eV and 11.5 eV scattering energy with a completely reversed asymmetry of ±60% we demonstrate the efficient mapping of the spin texture of the Au(111) surface state.

Visualizing Non-abrupt Transition of Quantum Well States at Stepped Silver Surfaces.

We use scanning tunneling spectroscopy (STS) experiments and first-principles density functional theory (DFT) calculations to address a fundamental question of how quantum well (QW) states for electrons in a metal evolve spatially in the lateral direction when there is a surface step that changes the vertical confinement thickness. This study reveals a clear spatially dependent, nearly continuous trend in the energetic shifts of quantum well (QW) states of thin Ag(111) film grown on Cu(111) substrate, showing the strongest change near the step edge. A large energetic shift equaling up to ~200 meV with a lateral extension of the QW states of the order of ~20 Å is found, even though the step-edge is atomically sharp as evidenced by a line scan. The observed lateral extension and the nearly smooth transition of QW states are understood within the context of step-induced charge oscillation, and Smoluchowski-type charge spreading and smoothing.

The impact of structural relaxation on spin polarization and magnetization reversal of individual nano structures studied by spin-polarized scanning tunneling microscopy.

The application of low temperature spin-polarized scanning tunneling microscopy and spectroscopy in magnetic fields for the quantitative characterization of spin polarization, magnetization reversal and magnetic anisotropy of individual nano structures is reviewed. We find that structural relaxation, spin polarization and magnetic anisotropy vary on the nm scale near the border of a bilayer Co island on Cu(1 1 1). This relaxation is lifted by perimetric decoration with Fe. We discuss the role of spatial variations of the spin-dependent electronic properties within and at the edge of a single nano structure for its magnetic properties.

Quantitative spin polarization analysis in photoelectron emission microscopy with an imaging spin filter.

Using a photoelectron emission microscope (PEEM), we demonstrate spin-resolved electron spectroscopic imaging of ultrathin magnetic Co films grown on Cu(100). The spin-filter, based on the spin-dependent reflection of low energy electrons from a W(100) crystal, is attached to an aberration corrected electrostatic energy analyzer coupled to an electrostatic PEEM column. We present a method for the quantitative measurement of the electron spin polarization at 4 × 10³ points of the PEEM image, simultaneously. This approach uses the subsequent acquisition of two images with different scattering energies of the electrons at the W(100) target to directly derive the spin polarization without the need of magnetization reversal of the sample.

Scanning tunneling spectroscopy of epitaxial graphene nanoisland on Ir(111).

Scanning tunneling spectroscopy (STS) was used to measure local differential conductance (dI/dV) spectra on nanometer-size graphene islands on an Ir(111) surface. Energy resolved dI/dV maps clearly show a spatial modulation, which we ascribe to a modulated local density of states due to quantum confinement. STS near graphene edges indicates a position dependence of the dI/dV signals, which suggests a reduced density of states near the edges of graphene islands on Ir(111).