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

Fluctuations of an Atomic Ledge Bordering a Crystalline Facet

When a high symmetry facet joins the rounded part of a crystal, the step line density vanishes as sqrt(r) with r denoting the distance from the facet edge. This means that the ledge bordering the facet has a lot of space to meander as caused by thermal activation. We investigate the statistical properties of the border ledge fluctuations. In the scaling regime they turn out to be non-Gaussian and related to the edge statistics of GUE multi-matrix models.Comment: Version with major revisions -- RevTeX, 4 pages, 2 figure

Theoretical study of O adlayers on Ru(0001)

Recent experiments performed at high pressures indicate that ruthenium can support unusually high concentrations of oxygen at the surface. To investigate the structure and stability of high coverage oxygen structures, we performed density functional theory calculations, within the generalized gradient approximation, for O adlayers on Ru(0001) from low coverage up to a full monolayer. We achieve quantitative agreement with previous low energy electron diffraction intensity analyses for the (2x2) and (2x1) phases and predict that an O adlayer with a (1x1) periodicity and coverage of 1 monolayer can form on Ru(0001), where the O adatoms occupy hcp-hollow sites.Comment: RevTeX, 6 pages, 4 figure

Automatic kelvin probe compatible with ultrahigh vacuum

This article describes a new type of in situ ultrahigh‐vacuum compatible kelvin probe based on a voice‐coil driving mechanism. This design exhibits several advantages over conventional mechanical feed‐through and (in situ) piezoelectric devices in regard to the possibility of multiple probe geometry, flexibility of probe geometry, amplitude of oscillation, and pure parallel vibration. Automatic setup and constant spacing features are achieved using a digital‐to‐analog converter (DAC) steered offset potential. The combination of very low driver noise pick‐up and data‐acquisition system (DAS) signal processing techniques results in a work function (wf  ) resolution, under optimal conditions, of <0.1 meV. Due to its high surface sensitivity and compatibility with standard sample cleaning and analysis techniques this design has numerous applications in surface studies, e.g., adsorption kinetics, sample topography and homogeneity, sputter profiles, etc. For semiconductor specimens the high wf resolution makes it eminently suitable for surface photovoltage (SPV) spectroscopy

Surface structure of nickel oxide layers on a Rh(111) surface

The formation of nickel oxide nanolayers by oxidizing Ni overlayers on Rh(111) has been investigated and their structures are reported as a function of the nickel coverage and oxygen pressure. Scanning tunneling microscopy (STM), low-energy electron diffraction (LEED), X-ray photoelectron spectroscopy (XPS) and diffraction (XPD), and high-resolution electron energy loss spectroscopy (HREELS) have been applied to characterize the structure and stoichiometry of the nickel oxide nanolayers. Several different phases have been observed depending on the strain state of the metallic Ni overlayers. For the pseudomorphic Ni monolayer, two distinctly different oxide phases with (6 x 1)-Ni5O5 and (2 root 3 x 2)-Ni8O10 structures have been identified at oxygen-poor (p = 5 x 10(-8) mbar) and oxygen-rich (p >= 1 x 10(-6) mbar) conditions, respectively. Above one monolayer, where the Ni layers are relaxed, bulk-like NiO(100) films form at the O-rich conditions, whereas chemisorbed-type p(2 x 2)O-Ni(111) layers develop in the O-poor regime. X-ray photoelectron diffraction analysis has provided additional insight into the relaxation mechanism and the detailed atomic structure of the Ni-oxide nanolayers. (C) 2013 Elsevier B.V. All rights reserved

Growth and properties of strained VOx thin films with controlled stoichiometry

We have succeeded in growing epitaxial films of rocksalt VOx on MgO(001) substrates. The oxygen content as a function of oxygen flux was determined using 18O2-RBS and the vanadium valence using XAS. The upper and lower stoichiometry limits found are similar to the ones known for bulk material (0.8<x<1.3). From the RHEED oscillation period a large number of vacancies for both vanadium and oxygen were deduced, i.e. ~16% for stoichiometric VO. These numbers are, surprisingly, very similar to those for bulk material and consequently quite strain-insensitive. XAS measurements reveal that the vacancies give rise to strong low symmetry ligand fields to be present. The electrical conductivity of the films is much lower than the conductivity of bulk samples which we attribute to a decrease in the direct overlap between t2g orbitals in the coherently strained layers. The temperature dependence of the conductivity is consistent with a variable range hopping mechanism.Comment: 12 pages, 16 figures included, revised versio

Low-energy electron diffraction analysis of the structure of a Cs-O/Ru(0001) coadsorbate phase

The structure of the (√3 × √3 )R30° overlayer formed by coadsorption of Cs and O atoms (θCs=θ0=0.33) on a Ru(0001) surface was determined by low-energy electron diffraction. Both adsorbates occupy hcp-type hollow sites. If compared with the structures of the respective pure adsorbate phases, the bond lengths are modified in a way consistent with an effective transfer of electronic charge from Cs to O