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What is the spatiotemporal limit of a macroscopic model that describes the optoelectronic interaction at the interface between different media? This fundamental question has become relevant for time-dependent photoemission from solid surfaces using probes that resolve attosecond electron dynamics on an atomic length scale. We address this fundamental question by investigating how ultrafast electron screening affects the infrared field distribution for a noble metal such as Cu(111) at the solid-vacuum interface. Attosecond photoemission delay measurements performed at different angles of incidence of the light allow us to study the detailed spatiotemporal dependence of the electromagnetic field distribution. Surprisingly, comparison with Monte Carlo semiclassical calculations reveals that the macroscopic Fresnel equations still properly describe the observed phase of the IR field on the Cu(111) surface on an atomic length and an attosecond time scale.

By means of spin- and angle-resolved photoelectron spectroscopy we studied the spin structure of thin films of the topological insulator Bi2Se3 grown on InP(111). For thicknesses below six quintuple layers the spin-polarized metallic topological surface states interact with each other via quantum tunneling and a gap opens. Our measurements show that the resulting surface states can be described by massive Dirac cones which are split in a Rashba-like manner due to the substrate induced inversion asymmetry. The inner and the outer Rashba branches have distinct localization in the top and the bottom part of the film, whereas the band apices are delocalized throughout the entire film. Supported by calculations, our observations help in the understanding of the evolution of the surface states at the topological phase transition and provide the groundwork for the realization of two-dimensional spintronic devices based on topological semiconductors.

We present time-resolved photoemission experiments from a peculiar bismuth surface, Bi(114). The strong one-dimensional character of this surface is reflected in the Fermi surface, which consists of spin-polarized straight lines. Our results show that the depletion of the surface state and the population of the bulk conduction band after the initial optical excitation persist for very long times. The disequilibrium within the hot electron gas along with strong electron-phonon coupling cause a displacive excitation of coherent phonons, which in turn are reflected in coherent modulations of the electronic states. Beside the well-known A(1g) bulk phonon mode at 2.76 THz, the time-resolved photoelectron spectra reveal a second mode at 0.72 THz which can be attributed to an optical surface phonon mode along the atomic rows of the Bi(114) surface.

BiTeI has a layered and noncentrosymmetric structure where strong spin-orbit interaction leads to a giant Rashba spin splitting in the bulk bands. We present direct measurements of the bulk band structure obtained with soft x-ray angle-resolved photoemission (ARPES), revealing the three-dimensional Fermi surface. The observed spindle torus shape bears the potential for a topological transition in the bulk by hole doping. Moreover, the bulk electronic structure is clearly disentangled from the two-dimensional surface electronic structure by means of high-resolution and spin-resolved ARPES measurements in the ultraviolet regime. All findings are supported by ab initio calculations.

We report a Rashba spin splitting of a two-dimensional electron gas in the topological insulator Bi(2)Se(3) from angle-resolved photoemission spectroscopy. We further demonstrate its electrostatic control, and show that spin splittings can be achieved which are at least an order-of-magnitude larger than in other semiconductors. Together these results show promise for the miniaturization of spintronic devices to the nanoscale and their operation at room temperature., (© 2011 American Physical Society)

Energy distribution curves of laser-induced electron pulses from a tungsten tip have been measured as a function of tip voltage and laser power. Electron emission via tunneling through and/or excitation over the surface barrier from photoexcited nonequilibrium electron distributions are clearly observed. The spectral shapes largely vary with the emission processes and are strongly affected by electron dynamics. Simulations successfully reproduce the spectra, thus allowing direct insight into the involved electron dynamics and revealing the temporal tunability of electron emission via the two experimental parameters. These results should be useful to optimize the pulse characteristics for many applications based on ultrafast laser-induced electron emission., (© 2011 American Physical Society)

The influence of structural defects, in the form of step lattices, on the spin polarization of the spin-orbit split Shockley surface state of Au(111) has been investigated. Spin- and angle-resolved photoemission data from three vicinal surfaces with different step densities are presented. The spin splitting is preserved in all three cases, and there is no reduction of the spin polarization of individual subbands, including the umklapp bands induced by the step lattice. On the sample with the highest step density studied, where the wave functions are delocalized over several terraces, the spin splitting is enhanced substantially, likely as an effect of the effective surface corrugation as on related surface alloys. The spin texture shows in all cases spin polarization vectors tangential to the Fermi circles, with the same helicities as on Au(111).

We have investigated field-emission patterns from a clean tungsten tip apex induced by femtosecond laser pulses. Strongly asymmetric modulations of the field-emission intensity distributions are observed depending on the polarization of the light and the laser incidence direction relative to the azimuthal orientation of tip apex. In effect, we have realized an ultrafast pulsed field-emission source with site selectivity. Simulations of local fields on the tip apex and of electron emission patterns based on photoexcited nonequilibrium electron distributions explain our observations quantitatively.

We show that the strongly spin-orbit coupled materials Bi2Te3 and Sb2Te3 and their derivatives belong to the Z2 topological-insulator class. Using a combination of first-principles theoretical calculations and photoemission spectroscopy, we directly show that Bi2Te3 is a large spin-orbit-induced indirect bulk band gap (delta approximately 150 meV) semiconductor whose surface is characterized by a single topological spin-Dirac cone. The electronic structure of self-doped Sb2Te3 exhibits similar Z2 topological properties. We demonstrate that the dynamics of spin-Dirac fermions can be controlled through systematic Mn doping, making these materials classes potentially suitable for topological device applications.

The (114) surface of the semimetal Bi is found to support a quasi-one-dimensional, metallic surface state. As required by symmetry, the state is degenerate along the Gamma-Y line of the surface Brillouin zone with a highest binding energy of approximately 150 meV. In the Gamma-X direction the degeneracy is lifted by the strong spin-orbit splitting in Bi, as directly shown by spin-resolved photoemission. This results in a Fermi contour consisting of two closely separated, parallel lines of opposite spin direction. It is argued that similar states on related insulators would give rise to a one-dimensional quantum spin Hall effect.

A Rashba-type spin-orbit splitting is found for quantum well states formed in ultrathin Pb films on Si (111). The resulting momentum splitting is comparable to what is found for semiconductor heterostructures. The splitting shows no coverage dependency and the sign of the spin polarization is reversed compared to Rashba splitting in the Au(111) surface state. We explain our results by competing effects at the two boundaries of the Pb layer.

The character of the surface state wave function on regularly stepped Cu(111) is reinvestigated. It is shown that the qualitative change at terrace lengths around 17 A observed previously by Ortega et al. [Phys. Rev. Lett. 84, 6110 (2000)]] must necessarily be described as a change from a propagating superlattice state to a terrace-confined quasi-one-dimensional state. This reconciles previous, apparently contradictory experimental results and sheds new light on the behavior of nearly free electrons in nanostructures. Possible mechanisms driving the localization are discussed on the basis of the surface state bulk penetration depth, which has been measured in both regimes.

The interaction of the Shockley surface state with the step lattice of vicinal Cu(111) leads to the formation of an electronic superlattice state. On Cu(443), where the average terrace length forms a "shape resonance" with the Fermi wavelength, we find a step-lattice-induced band-gap opening at the Fermi level. A gap magnitude >200 meV is inferred from high resolution photoemission experiments and line shape analysis. The corresponding energy gain with respect to a gapless case is approximately 11 meV/unit cell, and is a substantial contribution to the stabilization of the step lattice.

Visible and UV light spectra display striking differences in optical reflectivity for the two types of monatomic steps on copper (111) surfaces. Electronic structure calculations trace these differences to the specific contributions of p(axially) and p(radially) local densities of states, parallel and perpendicular to the steps, of the distinctly coordinated corner atoms. The local origin of the spectral reflectance anisotropy is further corroborated by experiments on Cu(111) surfaces with varying step densities. Site specificity of the electronic structure of atoms in low coordinated sites on Cu(111) vicinals is thus revealed by reflectance anisotropy spectroscopy which can thereby detect step atom densities down to 10(13) atoms/cm(2).

The influence of CO adsorption on the Shockley type surface state on vicinal Cu(111) surfaces is investigated using angle resolved photoemission. As the steps are decorated with CO the surface state shifts to higher binding energies, which is opposite to the known behavior on flat Cu(111). This is described within a one-dimensional potential model in which clean steps represent repulsive barriers and decorated steps become attractive wells. From the coverage dependence the integrated CO well potential can be quantified. It is U(CO)a = -2.9 eV A on both Cu(332) and Cu(221) surfaces. Density functional calculations reveal that this attractive potential is due to the very local charge transfer from the Cu step atom to the adsorbed molecule.

The low-energy electronic excitations in cobalt are studied by a theoretical method that includes many-body effects and a realistic description of the band structure. Angle-resolved photoemission spectra measured on a thick film of hexagonal close-packed Co on Cu(111) agree well with calculated spectral functions. Because of many-body effects no sharp quasiparticle peaks exist for binding energies larger than 2 eV and in this energy region the spectrum is essentially incoherent. The many-body corrections are much stronger in the majority-spin channel and drastically affect the spin polarization of the spectra.

Szöke's concept for electron holography is hampered by forward scattering that dominates electron diffraction from electron point sources below the surface top layer. Forward scattering was proposed to be suppressed if the anisotropic nature of the electron source wave is exploited [T. Greber and J. Osterwalder, Chem. Phys. Lett. 256, 653 (1996)]. Experiments show a strong suppression of forward scattering in Al(111) if Al 2s photoelectrons (E(kin) = 952 eV) are measured near the nodal plane of the outgoing p wave. The holographic reconstruction from such diffraction data provides three dimensional images of atomic sites in unit cells with a size of more than 10 A.