C. M. Wei

Ab initio calculation of the potential energy surface for the dissociation of H_2 on the sulfur-covered Pd(100) surface

The presence of sulfur atoms on the Pd(100) surface is known to hinder the dissociative adsorption of hydrogen. Using density-functional theory and the full-potential linear augmented plane-wave method, we investigate the potential energy surface (PES) of the dissociative adsorption of H_2 on the sulfur covered Pd(100) surface. The PES is changed significantly compared to the dissociation on the clean Pd(100) surface, in particular for hydrogen close to the S atoms. While the hydrogen dissociation at the clean Pd(100) surface is non-activated, for the (2x2) sulfur adlayer (coverage Theta_S= 0.25) the dissociation of H_2 is inhibited by energy barriers. Their heights strongly depend on the distance between the hydrogen and sulfur atoms leading to a highly corrugated PES. The largest barriers are in the vicinity of the sulfur atoms due to the strong repulsion between sulfur and hydrogen. Still the hydrogen dissociation on the (2x2) sulfur covered Pd(100) surface is exothermic. Thus the poisoning effect of sulfur adatoms for H_2 dissociation at low sulfur coverage (Theta_S <= 0.25) is mainly governed by the formation of energy barriers, not by blocking of the adsorption sites. For the c(2x2) sulfur adlayer (Theta_S= 0.5), the PES for hydrogen dissociation is purely repulsive. This is due to the fact that for all different possible adsorption geometries the hydrogen molecules come too close to the sulfur adatoms before the dissociation is completed.

A molecular dynamics study of self-diffusion on metal surfaces

We propose in this paper a theoretical model to investigate surface self-diffusion of single adatoms on the face-centered-cubic metals. Calculations are performed on the channeled (110), densely packed (111) and loosely packed (001) surfaces of indium at temperature T = 800 K. Three realistic model potentials, Embedded Atom method, Sutton-Chen and Rosato-Guillope-Legrand potentials, are applied to describe the interatomic interaction of the adatom/substrate systems. These potentials all involve a few empirical fittings of bulk properties of solid which incorporate with many-body effects. With these potentials, conventional molecular dynamics (MD) is employed to obtain trajectories of the atoms. On the (111) plane, via the Einstein relation, the estimated random walk exponential prefactors and activation energies do exhibit Arrhenius behavior, which are in reasonably good agreement with the experimental results. On the (001) and (110) faces, a number of theoretical evidences for atomic diffusion by exchange mechanism of the adatom with a surface atom are presented, which are again in fairly good agreement with the experiments. In addition, an examination of the exchange diffusion characteristics on several systems (Cu, Rh and Pt) is also presented.

Poisoning of hydrogen dissociation at Pd(100) by adsorbed sulfur studied by ab initio quantum dynamics and ab initio molecular dynamics

Abstract We report calculations of the dissociative adsorption of H 2 at Pd (100) covered with 1/4 monolayer of sulfur using quantum dynamics as well as molecular dynamics and taking all six degrees of freedom of the two H atoms fully into account. The ab-initio potential-energy surface (PES) is found to be very strongly corrugated. In particular, we discuss the influence of tunneling, zero-point vibrations due to the localization of the wave function of the nuclei when narrow valleys of the PES are passed, steering of the approaching H 2 molecules towards low-energy barrier configurations, and the important role of subsurface absorbates for the hydrogen dissociation. It is shown that “established” concepts derived from low-dimensional dynamical studies are not necessarily valid in a high-dimensional treatment.

A Strategy to Create Spin-Split Metallic Bands on Silicon Using a Dense Alloy Layer

To exploit Rashba effect in a 2D electron gas on silicon surface for spin transport, it is necessary to have surface reconstruction with spin-split metallic surface-state bands. However, metals with strong spin-orbit coupling (e.g., Bi, Tl, Sb, Pt) induce reconstructions on silicon with almost exclusively spin-split insulating bands. We propose a strategy to create spin-split metallic bands using a dense 2D alloy layer containing a metal with strong spin-orbit coupling and another metal to modify the surface reconstruction. Here we report two examples, i.e., alloying reconstruction with Na and Tl/Si(111)1 × 1 reconstruction with Pb. The strategy provides a new paradigm for creating metallic surface state bands with various spin textures on silicon and therefore enhances the possibility to integrate fascinating and promising capabilities of spintronics with current semiconductor technology.

A NEW DIRECT SURFACE STRUCTURAL PROBE: INVERSION OF MEASURED KIKUCHI ELECTRON PATTERNS

The technique of electron-emission holography (EEH) is reviewed with respect to its potential as a direct local structural probe. Direct inversion of the measured Kikuchi electron patterns is emphasized. The description of how the multiple scattering effects are eliminated by the integral-energy phase-summing method is presented. High-fidelity, artifact-free three-dimensional atomic images obtained by inverting simulated diffuse LEED and photoelectron diffraction patterns are shown. Direct inversion of the measured Kikuchi patterns shows clear images of the neighboring atoms within the range of the electron mean free path, thus yielding structural information with high resolution (~1 A) in all directions. Special attention is paid to the correct role of background subtraction in removing artifacts, and to the selection of minimal experimental data in the practical application of EEH. Moreover, direct inversion of diffraction patterns from many different local emitters is found to yield a three-dimensional Patterson function of the near-surface structure. This leads to direct surface structural determination by inverting Kikuchi electron patterns. Finally, the future of this direct method based upon inverting Kikuchi electron patterns, including the comparison with diffuse LEED and photoelectron holography, is discussed.

Direct atomic structure by holographic diffuse LEED

Abstract A multiple-energy phase-summing method is applied to diffuse low-energy electron diffraction intensity spectra to obtain three-dimensional images of surface atoms. In this demonstration, calculated DLEED intensity spectra from a multiple scattering method are directly inverted to produce high-fidelity 3D images of near-neighbor atoms measured from an adatom. No prior knowledge of adsorption site, bond length, bond angle, or type of atom is needed. The images are essentially free from artifacts and have a spatial resolution of ~ 1 A when viewed along any cut-plane. These results demonstrate that holographic DLEED has the potential of being an accurate and direct structural tool for low-density disordered adsorption systems.

Van der Waals interaction in a boron nitride bilayer

We have carried out quantum Monte Carlo (QMC) calculations to study the interlayer interaction in a boron nitride (BN) bilayer. The binding energy, 81 meV/2BN after finite-size corrections, was found to be larger than that obtained by density functional theory (DFT) with local density approximation, and smaller than those using van der Waals density functionals, both by considerable amounts. The QMC calculated interaction beyond the equilibrium interlayer separation was found to have a longer-range behavior than all the available DFT schemes.

Synthesis of two-dimensional Tl x Bi 1− x compounds and Archimedean encoding of their atomic structure

Crystalline atomic layers on solid surfaces are composed of a single building block, unit cell, that is copied and stacked together to form the entire two-dimensional crystal structure. However, it appears that this is not an unique possibility. We report here on synthesis and characterization of the one-atomic-layer-thick TlxBi1−x compounds which display quite a different arrangement. It represents a quasi-periodic tiling structures that are built by a set of tiling elements as building blocks. Though the layer is lacking strict periodicity, it shows up as an ideally-packed tiling of basic elements without any skips or halting. The two-dimensional TlxBi1−x compounds were formed by depositing Bi onto the Tl-covered Si(111) surface where Bi atoms substitute appropriate amount of Tl atoms. Atomic structure of each tiling element as well as arrangement of TlxBi1−x compounds were established in a detail. Electronic properties and spin texture of the selected compounds having periodic structures were characterized. The shown example demonstrates possibility for the formation of the exotic low-dimensional materials via unusual growth mechanisms.

Photoelectron-Diffraction Studies of Nb(001)

Photoelectron-diffration studies of Nb(001) have been performed to determine the first-interlayer contraction using Mg Kα radiation (hν=1253.6 eV) as an excitation source. Photoemission intensities of the 3d5/2 core level were measured as a function of the polar angle along several azimuths on the single-crystal surface. The 202.3-eV (205.O-eV) binding energy for the 3d5/2(3d3/2) core level was well resolved in the photoemission spectra, where the peak intensity could be easily evaluated by curve-fitting processes. Large oscillations of the 3d5/2 intensity as a function of the polar angle due to forward-focusing were observed. Based on multiple-scattering calculations for several first-interlayer spacings ranging from the bulk value to 16% contraction, the best agreement with experiment was obtained for a (13±5)% contraction of the first-interlayer spacing.

Electron-emission holography. A new direct method for surface structural determination

Abstract Direct inversion of measured Kikuchi and simulated photoelectron diffraction patterns shows clear images of the neighboring atoms within the range of the electron mean free path. More than ten nearby atoms are obtained for the Ag(100), Si(100) and (2 × 1) Na/Si (100) systems by the integral-energy phase-summing method. The key point in removing artifacts is a correct role of background subtraction. When this is achieved, the three-dimensional images are essentially high fidelity and artifact free. This demonstrates that electron-emission holography can be used as a direct local structural probe.