Diffusion rates of Cu adatoms on Cu(111) in the presence of an adisland nucleated at FCC or HCP sites

The surface diffusion of Cu adatoms in the presence of an adisland at FCC or HCP sites on Cu(111) is studied using the EAM potential derived by Mishin {\it et al.} [Phys. Rev. B {\bf 63} 224106 (2001)]. The diffusion rates along straight (with close-packed edges) steps with (100) and (111)-type microfacets (resp. step A and step B) are first investigated using the transition state theory in the harmonic approximation. It is found that the classical limit beyond which the diffusion rates follow an Arrhenius law is reached above the Debye temperature. The Vineyard attempt frequencies and the (static) energy barriers are reported. Then a comparison is made with the results of more realistic classical molecular dynamic simulations which also exhibit an Arrhenius-like behavior. It is concluded that the corresponding energy barriers are completely consistent with the static ones within the statistical errors and that the diffusion barrier along step B is significantly larger than along step A. In contrast the prefactors are very different from the Vineyard frequencies. They increase with the static energy barrier in agreement with the Meyer-Neldel compensation rule and this increase is well approximated by the law proposed by Boisvert {\it et al.} [Phys. Rev. Lett. {\bf 75} 469 (1995)]. As a consequence, the remaining part of this work is devoted to the determination of static energy barriers for a large number of diffusion events that can occur in the presence of an adisland. In particular, it is found that the corner crossing diffusion process for triangular adislands is markedly different for the two types of borders (A or B). From this set of results the diffusion rates of the most important atomic displacements can be predicted and used as input in Kinetic Monte-Carlo simulations

Efficient and accurate three dimensional Poisson solver for surface problems

We present a method that gives highly accurate electrostatic potentials for systems where we have periodic boundary conditions in two spatial directions but free boundary conditions in the third direction. These boundary conditions are needed for all kind of surface problems. Our method has an O(N log N) computational cost, where N is the number of grid points, with a very small prefactor. This Poisson solver is primarily intended for real space methods where the charge density and the potential are given on a uniform grid.Comment: 6 pages, 2 figure

Analysis of Clean Transition Metal Surfaces by Core Level Spectroscopy

The shifts in the binding energy of core electrons detected by high resolution X-ray photoelectron spectroscopy are a very sensitive probe of the chemical bonding of the excited atom. Since the surface atoms have their geometrical environment perturbed, their core levels are shifted from their bulk positions. A very large number of experiments have been performed on the 4f core level positions of tantalum and tungsten for various orientations of the surface plane. Systematic trends have been put forward and explained by theoretical models. Furthermore, the analysis of the angular variation of the core level line intensities gives structural information when compared with theoretical calculations. In the case of W(100) a single scattering theory is sufficient to reproduce experimental data. Finally we show that, in some particular cases, the core level lineshapes may differ strongly from a Doniach Sunjic model. The temperature dependence of their widths due to core hole-phonon coupling can be reproduced within the independent boson theory

Orbital contribution to the magnetic properties of nanowires: Is the orbital polarization ansatz justified?

We show that considerable orbital magnetic moments and magneto-crystalline anisotropy energies are obtained for a Fe monatomic wire described in a tight-binding method with intra-atomic electronic interactions treated in a full Hartree Fock (HF) decoupling scheme. Even-though the use of the orbital polarization ansatz with simplified Hamiltonians leads to fairly good results when the spin magnetization is saturated this is not the case of unsaturated systems. We conclude that the full HF scheme is necessary to investigate low dimensional systems

Lifetime of the first and second collective excitations in metallic nanoparticles

We determine the lifetime of the surface plasmon in metallic nanoparticles under various conditions, concentrating on the Landau damping, which is the dominant mechanism for intermediate-size particles. Besides the main contribution to the lifetime, which smoothly increases with the size of the particle, our semiclassical evaluation yields an additional oscillating component. For the case of noble metal particles embedded in a dielectric medium, it is crucial to consider the details of the electronic confinement; we show that in this case the lifetime is determined by the shape of the self-consistent potential near the surface. Strong enough perturbations may lead to the second collective excitation of the electronic system. We study its lifetime, which is limited by two decay channels: Landau damping and ionization. We determine the size dependence of both contributions and show that the second collective excitation remains as a well defined resonance.Comment: 18 pages, 5 figures; few minor change

Giant orbital moments are responsible for the anisotropic magnetoresistance of atomic contacts

We study here, both experimentally and theoretically, the anisotropy of magnetoresistance in atomic contacts. Our measurements on iron break junctions reveal an abrupt and hysteretic switch between two conductance levels when a large applied field is continuously rotated. We show that this behaviour stems from the coexistence of two metastable electronic states which result from the anisotropy of electronic interactions responsible for the enhancement of orbital magnetization. In both states giant orbital moments appear on the low coordinated central atom in a realistic contact geometry. However they differ by their orientation, parallel or perpendicular, with respect to the axis of the contact. Our explanation is totally at variance with the usual model based on the band structure of a monatomic linear chain, which we argue cannot be applied to 3d ferromagnetic metals

Broken-Bond Rule for the Surface Energies of Noble Metals

Using two different full-potential ab-initio techniques we introduce a simple, universal rule based on the number of broken first-neighbor bonds to determine the surface energies of the three noble metals Cu, Ag and Au. When a bond is broken, the rearrangement of the electronic charge for these metals does not lead to a change of the remaining bonds. Thus the energy needed to break a bond is independent of the surface orientation. This novel finding can lead to the development of simple models to describe the energetics of a surface like step and kink formation, crystal growth, alloy formation, equilibrium shape of mesoscopic crystallites and surface faceting.Comment: 4 pages, 2 figure

Temperature dependence of the magnetic Casimir-Polder interaction

We analyze the magnetic dipole contribution to atom-surface dispersion forces. Unlike its electrical counterpart, it involves small transition frequencies that are comparable to thermal energy scales. A significant temperature dependence is found near surfaces with a nonzero DC conductivity, leading to a strong suppression of the dispersion force at T > 0. We use thermal response theory for the surface material and discuss both normal metals and superconductors. The asymptotes of the free energy of interaction and of the entropy are calculated analytically over a large range of distances. Near a superconductor, the onset of dissipation at the phase transition strongly changes the interaction, including a discontinuous entropy. We discuss the similarities with the Casimir interaction beween two surfaces and suggest that precision measurements of the atom-surface interaction may shed new light upon open questions around the temperature dependence of dispersion forces between lossy media.Comment: 11 figure

Theory of Vibrationally Inelastic Electron Transport through Molecular Bridges

Vibrationally inelastic electron transport through a molecular bridge that is connected to two leads is investigated. The study is based on a generic model of vibrational excitation in resonant transmission of electrons through a molecular junction. Employing methods from electron-molecule scattering theory, the transmittance through the molecular bridge can be evaluated numerically exactly. The current through the junction is obtained approximately using a Landauer-type formula. Considering different parameter regimes, which include both the case of a molecular bridge that is weakly coupled to the leads, resulting in narrow resonance structures, and the opposite case of a broad resonance caused by strong interaction with the leads, we investigate the characteristic effects of coherent and dissipative vibrational motion on the electron transport. Furthermore, the validity of widely used approximations such as the wide-band approximation and the restriction to elastic transport mechanisms is investigated in some detail.Comment: Submited to PRB, revised version according to comments of referees (minor text changes and new citations