arXiv subjects

K. Reuter

Publications and source records attributed to K. Reuter.

At least 19 recordsLinked to original sources

arXiv2022

\AA ngstrom depth resolution with chemical specificity at the liquid-vapor interface

The determination of depth profiles across interfaces is of primary importance in many scientific and technological areas. Photoemission spectroscopy is in principle well suited for this purpose, yet a quantitative implementation for investigations of liquid-vapor interfaces is hindered by the lack of understanding of electron-scattering processes in liquids. Previous studies have shown, however, that core-level photoelectron angular distributions (PADs) are altered by depth-dependent elastic electron scattering and can, thus, reveal information on the depth distribution of species across the interface. Here, we explore this concept further and show that the anisotropy parameter characterizing the PAD scales linearly with the average distance of atoms along the surface normal. This behavior can be accounted for in the low-collision-number regime. We also show that results for different atomic species can be compared on the same length scale. We demonstrate that atoms separated by about 1~\AA~along the surface normal can be clearly distinguished with this method, achieving excellent depth resolution.

physics.chem-ph↗

arXiv2018

Optimizations of the Eigensolvers in the ELPA Library

The solution of (generalized) eigenvalue problems for symmetric or Hermitian matrices is a common subtask of many numerical calculations in electronic structure theory or materials science. Solving the eigenvalue problem can easily amount to a sizeable fraction of the whole numerical calculation. For researchers in the field of computational materials science, an efficient and scalable solution of the eigenvalue problem is thus of major importance. The ELPA-library is a well-established dense direct eigenvalue solver library, which has proven to be very efficient and scalable up to very large core counts. In this paper, we describe the latest optimizations of the ELPA-library for new HPC architectures of the Intel Skylake processor family with an AVX-512 SIMD instruction set, or for HPC systems accelerated with recent GPUs. We also describe a complete redesign of the API in a modern modular way, which, apart from a much simpler and more flexible usability, leads to a new path to access system-specific performance optimizations. In order to ensure optimal performance for a particular scientific setting or a specific HPC system, the new API allows the user to influence in straightforward way the internal details of the algorithms and of performance-critical parameters used in the ELPA-library. On top of that, we introduced an autotuning functionality, which allows for finding the best settings in a self-contained automated way. In situations where many eigenvalue problems with similar settings have to be solved consecutively, the autotuning process of the ELPA-library can be done "on-the-fly". Practical applications from materials science which rely on so-called self-consistency iterations can profit from the autotuning. On some examples of scientific interest, simulated with the FHI-aims application, the advantages of the latest optimizations of the ELPA-library are demonstrated.

cs.MS↗

arXiv2016

Interplay between nanometer-scale strain variations and externally applied strain in graphene

We present a molecular modeling study analyzing nanometer-scale strain variations in graphene as a function of externally applied tensile strain. We consider two different mechanisms that could underlie nanometer-scale strain variations: static perturbations from lattice imperfections of an underlying substrate and thermal fluctuations. For both cases we observe a decrease in the out-of-plane atomic displacements with increasing strain, which is accompanied by an increase in the in-plane displacements. Reflecting the non-linear elastic properties of graphene, both trends together yield a non-monotonic variation of the total displacements with increasing tensile strain. This variation allows to test the role of nanometer-scale strain variations in limiting the carrier mobility of high-quality graphene samples.

cond-mat.mes-hall↗

arXiv2015

Evidence for the Active Phase of Heterogeneous Catalysts through In Situ Reaction Product Imaging and Multiscale Modeling

We use multi-scale modeling to analyze laser-induced fluorescence (LIF) measurements of the CO oxidation reaction over Pd(100) at near-ambient reaction conditions. Integrating density-functional theory based kinetic Monte Carlo simulations of the active catalyst into fluid-dynamical simulations of the mass transport inside the reactor chamber we calculate the reaction product concentration directly above the catalyst surface. Comparing corresponding data calculated for different surface models against the measured LIF signals we can discriminate the one that predominantly actuates the experimentally measured catalytic activity. For the probed CO oxidation reaction conditions the experimental activity is due to pristine Pd(100), possibly coexisting with other (oxidic) domains on the surface.

cond-mat.mtrl-sci↗

arXiv2014

Quantification of finite-temperature effects on adsorption geometries of $π$-conjugated molecules

The adsorption structure of the molecular switch azobenzene on Ag(111) is investigated by a combination of normal incidence x-ray standing waves and dispersion-corrected density functional theory. The inclusion of non-local collective substrate response (screening) in the dispersion correction improves the description of dense monolayers of azobenzene, which exhibit a substantial torsion of the molecule. Nevertheless, for a quantitative agreement with experiment explicit consideration of the effect of vibrational mode anharmonicity on the adsorption geometry is crucial.

cond-mat.mtrl-sci↗

arXiv2014

On the role of physisorption states in molecular scattering: A semi-local density-functional theory study on O2/Ag(111)

We simulate the scattering of O$_2$ from Ag(111) with classical dynamics simulations performed on a six-dimensional potential energy surface calculated within semi-local density-functional theory (DFT). The enigmatic experimental trends that originally required the conjecture of two types of repulsive walls, arising from a physisorption and chemisorption part of the interaction potential, are fully reproduced. Given the inadequate description of the physisorption properties in semi-local DFT, our work casts severe doubts on the prevalent notion to use molecular scattering data as indirect evidence for the existence of such states.

cond-mat.mtrl-sci↗

arXiv2014

kmos: A lattice kinetic Monte Carlo framework

Kinetic Monte Carlo (kMC) simulations have emerged as a key tool for microkinetic modeling in heterogeneous catalysis and other materials applications. Systems, where site-specificity of all elementary reactions allows a mapping onto a lattice of discrete active sites, can be addressed within the particularly efficient lattice kMC approach. To this end we describe the versatile kmos software package, which offers a most user-friendly implementation, execution, and evaluation of lattice kMC models of arbitrary complexity in one- to three-dimensional lattice systems, involving multiple active sites in periodic or aperiodic arrangements, as well as site-resolved pairwise and higher-order lateral interactions. Conceptually, kmos achieves a maximum runtime performance which is essentially independent of lattice size by generating code for the efficiency-determining local update of available events that is optimized for a defined kMC model. For this model definition and the control of all runtime and evaluation aspects kmos offers a high-level application programming interface. Usage proceeds interactively, via scripts, or a graphical user interface, which visualizes the model geometry, the lattice occupations and rates of selected elementary reactions, while allowing on-the-fly changes of simulation parameters. We demonstrate the performance and scaling of kmos with the application to kMC models for surface catalytic processes, where for given operation conditions (temperature and partial pressures of all reactants) central simulation outcomes are catalytic activity and selectivities, surface composition, and mechanistic insight into the occurrence of individual elementary processes in the reaction network.

cond-mat.mtrl-sci↗

arXiv2013

In situ X-ray photoelectron spectroscopy of model catalysts: At the edge of the gap

We present a High-Pressure X-ray Photoelectron Spectroscopy (HP-XPS) and first-principles kinetic Monte Carlo study addressing the nature of the active surface in CO oxidation over Pd(100). Simultaneously measuring the chemical composition at the surface and in the near-surface gas-phase, we reveal both O-covered pristine Pd(100) and a surface oxide as stable, highly active phases in the near-ambient regime accessible to HP-XPS. Surprisingly, no adsorbed CO can be detected during high CO2 production rates, which can be explained by a combination of a remarkably short residence time of the CO molecule on the surface and mass-transfer limitations in the present set-up.

physics.chem-ph↗

arXiv2009

Wave-driven dynamo action in spherical MHD systems

Hydrodynamic and magnetohydrodynamic numerical studies of a mechanically forced two-vortex flow inside a sphere are reported. The simulations are performed in the intermediate regime between the laminar flow and developed turbulence where a hydrodynamic instability is found to generate internal waves with a characteristic m=2 zonal wave number. It is shown that this time-periodic flow acts as a dynamo although snapshots of the flow as well as the mean flow are not dynamos. The magnetic fields' growth rate exhibits resonance effects depending on the wave frequency. Furthermore, a cyclic self-killing and self-recovering dynamo based on the relative alignment of the velocity and magnetic fields is presented. The phenomena are explained in terms of a mixing of non-orthogonal eigenstates of the time dependent linear operator of the magnetic induction equation. The potential relevance of this mechanism to dynamo experiments is discussed.

physics.flu-dyn↗

arXiv2009

A Spherical Plasma Dynamo Experiment

We propose a plasma experiment to be used to investigate fundamental properties of astrophysical dynamos. The highly conducting, fast-flowing plasma will allow experimenters to explore systems with magnetic Reynolds numbers an order of magnitude larger than those accessible with liquid-metal experiments. The plasma is confined using a ring-cusp strategy and subject to a toroidal differentially rotating outer boundary condition. As proof of principle, we present magnetohydrodynamic simulations of the proposed experiment. When a von Kármán-type boundary condition is specified, and the magnetic Reynolds number is large enough, dynamo action is observed. At different values of the magnetic Prandtl and Reynolds numbers the simulations demonstrate either laminar or turbulent dynamo action.

physics.plasm-ph↗

arXiv2008

O- and H- induced surface core level shifts on Ru(0001): Prevalence of the additivity rule

In previous work on adsorbate-induced surface core level shifts (SCLSs), the effects caused by O atom adsorption on Rh(111) and Ru(0001) were found to be additive: the measured shifts for first layer Ru atoms depended linearly on the number of directly coordinated O atoms. Density-functional theory calculations quantitatively reproduced this effect, allowed separation of initial and final state contributions, and provided an explanation in terms of a roughly constant charge transfer per O atom. We have now conducted similar measurements and calculations for three well-defined adsorbate and coadsorbate layers containing O and H atoms: (1 x 1)-H, (2 x 2)-(O+H), and (2 x 2)-(O+3H) on Ru(0001). As H is stabilized in fcc sites in the prior two structures and in hcp sites in the latter, this enables us to not only study coverage and coadsorption effects on the adsorbate-induced SCLSs, but also the sensitivity to similar adsorption sites. Remarkably good agreement is obtained between experiment and calculations for the energies and geometries of the layers, as well as for all aspects of the SCLS values. The additivity of the next-neighbor adsorbate-induced SCLSs is found to prevail even for the coadsorbate structures. While this confirms the suggested use of SCLSs as fingerprints of the adsorbate configuration, their sensitivity is further demonstrated by the slightly different shifts unambiguously determined for H adsorption in either fcc or hcp hollow sites.

cond-mat.mtrl-sci↗

arXiv2003

Kinetic hindrance during the initial oxidation of Pd(100) at ambient pressures

The oxidation of the Pd(100) surface at oxygen pressures in the 10^-6 to 10^3 mbar range and temperatures up to 1000 K has been studied in-situ by surface x-ray diffraction (SXRD). The results provide direct structural information on the phases present in the surface region and on the kinetics of the oxide formation. Depending on the (T,p) environmental conditions we either observe a thin sqrt(5) x sqrt(5) R27 surface oxide or the growth of a rough, poorly ordered bulk oxide film of PdO predominantly with (001) orientation. By either comparison to the surface phase diagram from first-principles atomistic thermodynamics or by explicit time-resolved measurements we identify a strong kinetic hindrance to the bulk oxide formation even at temperatures as high as 675 K.

cond-mat.mtrl-sci↗

arXiv2003

The Pd(100)-(SQRT(5) x SQRT(5) R27^o)-O surface oxide revisited

Combining high-resolution core-level spectroscopy (HRCLS), scanning tunneling microscopy (STM) and density-functional theory (DFT) calculations we reanalyze the Pd(100)-(SQRT(5) x SQRT(5) R27^o)-O surface oxide phase. We find that the prevalent structural model, a rumpled PdO(001) film suggested by previous low energy electron diffraction (LEED) work (M. Saidy et al., Surf. Sci. 494, L799 (2001)), is incompatible with all three employed methods. Instead, we suggest the two-dimensional film to consist of a strained PdO(101) layer on top of Pd(100). LEED intensity calculations show that this model is compatible with the experimental data of Saidy et al.

cond-mat.mtrl-sci↗

arXiv2001

Surface Core Level Shifts of Clean and Oxygen Covered Ru(0001)

We have performed high resolution XPS experiments of the Ru(0001) surface, both clean and covered with well-defined amounts of oxygen up to 1 ML coverage. For the clean surface we detected two distinct components in the Ru 3d_{5/2} core level spectra, for which a definite assignment was made using the high resolution Angle-Scan Photoelectron Diffraction approach. For the p(2x2), p(2x1), (2x2)-3O and (1x1)-O oxygen structures we found Ru 3d_{5/2} core level peaks which are shifted up to 1 eV to higher binding energies. Very good agreement with density functional theory calculations of these Surface Core Level Shifts (SCLS) is reported. The overriding parameter for the resulting Ru SCLSs turns out to be the number of directly coordinated O atoms. Since the calculations permit the separation of initial and final state effects, our results give valuable information for the understanding of bonding and screening at the surface, otherwise not accessible in the measurement of the core level energies alone.

cond-mat.mtrl-sci↗

arXiv1998

Ballistic Electron Emission Microscopy on CoSi${}_2$/Si(111) interfaces: band structure induced atomic-scale resolution and role of localized surface states

Applying a Keldysh Green`s function method it is shown that hot electrons injected from a STM-tip into a CoSi${}_2$/Si(111) system form a highly focused beam due to the silicide band structure. This explains the atomic resolution obtained in recent Ballistic Electron Emission Microscopy (BEEM) experiments. Localized surface states in the $(2 \times 1)$-reconstruction are found to be responsible for the also reported anticorrugation of the BEEM current. These results clearly demonstrate the importance of bulk and surface band structure effects for a detailed understanding of BEEM data.

cond-mat.mtrl-sci↗

arXiv1998

LEED Holography applied to a complex superstructure: a direct view of the adatom cluster on SiC(111)-(3x3)

For the example of the SiC(111)-(3x3) reconstruction we show that a holographic interpretation of discrete Low Energy Electron Diffraction (LEED) spot intensities arising from ordered, large unit cell superstructures can give direct access to the local geometry of a cluster around an elevated atom, provided there is only one such prominent atom per surface unit cell. By comparing the holographic images obtained from experimental and calculated data we illuminate validity, current limits and possible shortcomings of the method. In particular, we show that periodic vacancies such as cornerholes may inhibit the correct detection of the atomic positions. By contrast, the extra diffraction intensity due to slight substrate reconstructions, as for example buckling, seems to have negligible influence on the images. Due to the spatial information depth of the method the stacking of the cluster can be imaged down to the fourth layer. Finally, it is demonstrated how this structural knowledge of the adcluster geometry can be used to guide the dynamical intensity analysis subsequent to the holographic reconstruction and necessary to retrieve the full unit cell structure.

cond-mat.mtrl-sci↗

arXiv1998

Extending holographic LEED to ordered small unit cell superstructures

Following on the success of the recent application of holographic LEED to the determination of the 3D atomic geometry of Si adatoms on a SiC(111) p(3x3) surface, which enabled that structure to be solved, we show in this paper that a similar technique allows the direct recovery of the local geometry of adsorbates forming superstructures as small as p(2x2), even in the presence of a local substrate reconstruction.

cond-mat.mtrl-sci↗

arXiv1998

Quantum mechanical analysis of the elastic propagation of electrons in the Au/Si system: application to Ballistic Electron Emission Microscopy

We present a Green's function approach based on a LCAO scheme to compute the elastic propagation of electrons injected from a STM tip into a metallic film. The obtained 2D current distribution in real and reciprocal space furnish a good representation of the elastic component of Ballistic Electron Emission Microscopy (BEEM) currents. Since this component accurately approximates the total current in the near threshold region, this procedure allows --in contrast to prior analyses-- to take into account effects of the metal band structure in the modeling of these experiments. The Au band structure, and in particular its gaps appearing in the [111] and [100] directions provides a good explanation for the previously irreconcilable results of nanometric resolution and similarity of BEEM spectra on both Au/Si(111) and Au/Si(100).

cond-mat.mtrl-sci↗