Plasmon localization by adatoms in gold atomic wires on Si(775)

Self-organized gold chains on vicinal Si(111) surfaces represent prototype examples of quasi-one-dimensional objects that are stabilized by hybridization with Si surface states. Their plasmons contain important information about the unoccupied bandstructure close to the Fermi level. Using Si(775)-Au as an example, we report here the modifications of the plasmon dispersion by the simple atomic adatom species H and O. Using a combination of low energy electron diffraction and high-resolution electron energy loss spectroscopy, we study the interconnection between plasmonic excitation and the corresponding local surface structure. Both adsorbates do not destroy metallicity, but, similar to Si(553)-Au, atomic hydrogen enhances dimerization of the Au chains, which at small concentrations counteracts the disorder introduced by random adsorption. This effect, most likely caused by electron donation of H to the surface states, is missing in case of adsorbed oxygen, so that only the effect of disorder is observed. For both adsorbates increasing disorder as a function of adsorbate concentration finally results in plasmon localization and opening of a band gap

Observation of correlated spin-orbit order in a strongly anisotropic quantum wire system

Quantum wires with spin-orbit coupling provide a unique opportunity to simultaneously control the coupling strength and the screened Coulomb interactions where new exotic phases of matter can be explored. Here we report on the observation of an exotic spin-orbit density wave in Pb-atomic wires on Si(557) surfaces by mapping out the evolution of the modulated spin-texture at various conditions with spin- and angle-resolved photoelectron spectroscopy. The results are independently quantified by surface transport measurements. The spin polarization, coherence length, spin dephasing rate, and the associated quasiparticle gap decrease simultaneously as the screened Coulomb interaction decreases with increasing excess coverage, providing a new mechanism for generating and manipulating a spin-orbit entanglement effect via electronic interaction. Despite clear evidence of spontaneous spin-rotation symmetry breaking and modulation of spin-momentum structure as a function of excess coverage, the average spin-polarization over the Brillouin zone vanishes, indicating that time-reversal symmetry is intact as theoretically predicted

Scaling of the Hysteresis Loop in Two-dimensional Solidification

The first order phase transitions between a two-dimensional (2d) gas and the 2d solid of the first monolayer have been studied for the noble gases Ar, Kr and Xe on a NaCl(100) surface in quasi-equilibrium with the three-dimensional gas phase. Using linear temperature ramps, we show that the widths of the hysteresis loops of these transitions as a function of the heating rate, r, scales with a power law r^alpha with alpha between 0.4 and 0.5 depending on the system. The hysteresis loops for different heating rates are similar. The island area of the condensed layer was found to grow initially with a t^4 time dependence. These results are in agreement with theory, which predicts alpha = 0.5 and hysteresis loop similarity.Comment: 4 pages, 5 figures, Revte

Towards a first-principles theory of surface thermodynamics and kinetics

Understanding of the complex behavior of particles at surfaces requires detailed knowledge of both macroscopic and microscopic processes that take place; also certain processes depend critically on temperature and gas pressure. To link these processes we combine state-of-the-art microscopic, and macroscopic phenomenological, theories. We apply our theory to the O/Ru(0001) system and calculate thermal desorption spectra, heat of adsorption, and the surface phase diagram. The agreement with experiment provides validity for our approach which thus identifies the way for a predictive simulation of surface thermodynamics and kinetics.Comment: 4 pages including 3 figures. Related publications can be found at http://www.fhi-berlin.mpg.de/th/paper.htm

Diffusion in a strongly correlated anisotropic overlayer

We study the collective diffusion in chain structures on anisotropic substrates like (112) bcc and (110) fcc surfaces with deep troughs in the substrate potential corrugation. These chain structures are aligned normal to the troughs and can move only along the troughs. In a combination of theoretical arguments and of numerical simulations, we study the mass transport in these anisotropic systems. We find that a mechanism similar to soliton diffusion, instead of single particle diffusion, is still effective at temperatures well above the melting temperature of the ordered chain structures. This mechanism is directly correlated with the ordered phases that appear at much lower temperatures. As a consequence, also the influence of frozen disorder is still visible above the melting temperature. Theoretically we predict a strong dependence of the pre-exponential factor and weak dependence of the activation energy on the concentration of frozen surface defects. These predictions are confirmed by the simulations.Comment: Latex file, 18 pages and 9 eps figures include

Oxidation of graphene on metals

We use low-energy electron microscopy to investigate how graphene is removed from Ru(0001) and Ir(111) by reaction with oxygen. We find two mechanisms on Ru(0001). At short times, oxygen reacts with carbon monomers on the surrounding Ru surface, decreasing their concentration below the equilibrium value. This undersaturation causes a flux of carbon from graphene to the monomer gas. In this initial mechanism, graphene is etched at a rate that is given precisely by the same non-linear dependence on carbon monomer concentration that governs growth. Thus, during both growth and etching, carbon attaches and detaches to graphene as clusters of several carbon atoms. At later times, etching accelerates. We present evidence that this process involves intercalated oxygen, which destabilizes graphene. On Ir, this mechanism creates observable holes. It also occurs mostly quickly near wrinkles in the graphene islands, depends on the orientation of the graphene with respect to the Ir substrate, and, in contrast to the first mechanism, can increase the density of carbon monomers. We also observe that both layers of bilayer graphene islands on Ir etch together, not sequentially.Comment: 15 pages, 10 figures. Manuscript revised to improve discussion, following referee comments. Accepted for publication in Journal of Physical Chemistry C, Feb. 11, 201

Anomalous thickness dependence of the Hall effect in ultrathin Pb layers on Si(111)

The magnetoconductive properties of ultrathin Pb films deposited on Si(111) are measured and compared with density-functional electronic band-structure calculations on two-dimensional, free-standing, 1 to 8 monolayers thick Pb(111) slabs. A description with free-standing slabs is possible because it turned out that the Hall coefficient is independent of the substrate and of the crystalline order in the film. We show that the oscillations in sign of the Hall coefficient observed as a function of film thickness can be explained directly from the thickness dependent variations of the electronic bandstructure at the Fermi energy.Comment: 4 pages incl. 3 figures, RevTeX, to appear in Phys. Rev.

Anomalous Behavior of Ru for Catalytic Oxidation: A Theoretical Study of the Catalytic Reaction CO + 1/2 O_2 --> CO_2

Recent experiments revealed an anomalous dependence of carbon monoxide oxidation at Ru(0001) on oxygen pressure and a particularly high reaction rate. Below we report density functional theory calculations of the energetics and reaction pathways of the speculated mechanism. We will show that the exceptionally high rate is actuated by a weakly but nevertheless well bound (1x1) oxygen adsorbate layer. Furthermore it is found that reactions via scattering of gas-phase CO at the oxygen covered surface may play an important role. Our analysis reveals, however, that reactions via adsorbed CO molecules (the so-called Langmuir-Hinshelwood mechanism) dominate.Comment: 5 pages, 4 figures, Phys. Rev. Letters, Feb. 1997, in prin