Islands, craters, and a moving surface step on a hexagonally reconstructed (100) noble metal surface

Deposition/removal of metal atoms on the hex reconstructed (100) surface of Au, Pt and Ir should present intriguing aspects, since a new island implies hex -> square deconstruction of the substrate, and a new crater the square -> hex reconstruction of the uncovered layer. To obtain a microscopic understanding of how islands/craters form in these conditions, we have conducted simulations of island and crater growth on Au(100), whose atomistic behavior, including the hex reconstruction on top of the square substrate, is well described by mean s of classical many-body forces. By increasing/decreasing the Au coverage on Au(100), we find that island/craters will not grow unless they exceed a critical size of about 8-10 atoms. This value is close to that which explains the nonlinear coverage dependence observed in molecular adsorption on the closely related surface Pt (100). This threshold size is rationalized in terms of a transverse step correlation length, measuring the spatial extent where reconstruction of a given plane is disturbed by the nearby step.Comment: 11 pages, 5 figures, accepted for publication in Surface Science (ECOSS-18

Realistic grand canonical Monte Carlo surface simulation: application to Ar(111)

Most realistic, off-lattice surface simulations are done canonically--- conserving particles. For some applications, however, such as studying the thermal behavior of rare gas solid surfaces, these constitute bad working conditions. Surface layer occupancies are believed to change with temperature, particularly at preroughening, and naturally call for a grand canonical approach, where particle number is controlled by a chemical potential. We report preliminary results of novel realistic grand canonical Monte Carlo simulations of the Lennard-Jones (LJ) fcc(111) surface, believed to represent a quantitative model of e.g. Ar(111). The results are successful and highly informative for temperatures up to roughly 0.8 T_m, where clear precursor signals of preroughening are found. At higher temperatures, convergence to equilibrium is hampered by large fluctuations.Comment: 4 pages, REVTeX, 3 PostScript figure

Surface molecular dynamics simulation with two orthogonal surface steps: how to beat the particle conservation problem

Due to particle conservation, Canonical Molecular Dynamics (MD) simulations fail in the description of surface phase transitions involving coverage or lateral density changes. However, a step on the surface can act effectively as a source or a sink of atoms, in the simulation as well as in real life. A single surface step can be introduced by suitably modifying planar Periodic Boundary Conditions (PBC), to accommodate the generally inequivalent stacking of two adjacent layers. We discuss here how, through the introduction of two orthogonal surface steps, particle number conservation may no longer represent a fatal constraint for the study of these surface transitions. As an example, we apply the method for estimating temperature-induced lateral density increase of the reconstructed Au (001) surface; the resulting anisotropic cell change is consistent with experimental observations. Moreover, we implement this kind of scheme in conjunction with the variable curvature MD method, recently introduced by our group.Comment: 9 pages, 5 figures, accepted for publication in Surface Science (ECOSS-19

Role of Layering Oscillations at Liquid Metal Surfaces in Bulk Recrystallization and Surface Melting

The contrasting melting behavior of different surface orientations in metals can be explained in terms of a repulsive or attractive effective interaction between the solid-liquid and the liquid-vapor interface. We show how a crucial part of this interaction originates from the layering effects near the liquid metal surface. Its sign depends on the relative tuning of layering oscillations to the crystal interplanar spacing, thus explaining the orientational dependence. Molecular dynamics recrystallization simulations of Au surfaces provide direct and quantitative evidence of this phenomenon.Comment: 10 pages (RevTeX) plus 3 figures (PostScript

Variable Curvature Slab Molecular Dynamics as a Method to Determine Surface Stress

A thin plate or slab, prepared so that opposite faces have different surface stresses, will bend as a result of the stress difference. We have developed a classical molecular dynamics (MD) formulation where (similar in spirit to constant-pressure MD) the curvature of the slab enters as an additional dynamical degree of freedom. The equations of motion of the atoms have been modified according to a variable metric, and an additional equation of motion for the curvature is introduced. We demonstrate the method to Au surfaces, both clean and covered with Pb adsorbates, using many-body glue potentials. Applications to stepped surfaces, deconstruction and other surface phenomena are under study.Comment: 16 pages, 8 figures, REVTeX, submitted to Physical Review

Noncrystalline structures of ultrathin unsupported nanowires

Computer simulations suggest that ultrathin metal wires should develop exotic, non-crystalline stable atomic structures, once their diameter decreases below a critical size of the order of a few atomic spacings. The new structures, whose details depend upon the material and the wire thickness, may be dominated by icosahedral packings. Helical, spiral-structured wires with multi-atom pitches are also predicted. The phenomenon, analogous to the appearance of icosahedral and other non-crystalline shapes in small clusters, can be rationalized in terms of surface energy anisotropy and optimal packing

Molecular dynamics studies of gold: bulk, defects, surfaces and clusters

In recent years, computer simulation methods have provided much insight into several structural, dynamical and thermal properties of solids and liquids. Computational methods are particularly well suited to the study of low symmetry sys.terns (e.g., defects, surfaces, clusters), where the complexity of analytical treatments may become overwhelming, and of systems at finite temperature. The key ingredients in computer simulations are interatomic forces. The problem we wish to solve can be simply stated as follows: given a set of N atoms having some positions r 1 \u2022.. rN and linear momenta p1 .\u2022\u2022 PN, what forces will they experience ? Calculating these forces ab initio is a very difficult task. Even if we are not interested in the electronic\ub7 properties of the system, but only in ionic properties (e.g., vibrations, equilibrium structures, etc.), we must generally take into full account the electronic aspect of the problem. In the Born-Oppenheimer adiabatic approximation [1 J, the forces can be obtained by considering the nuclei as fixed and searching for the minimum energy state of the electronic system. This .may be done using the Hartree-Fock approximation, or in a density functional theory framework. The force acting on a nucleus is then determined as the gradient of the total energy respect to a displacement of that nucleus. After all nuclei have been moved accordingly to the forces computed in _this way, the whole process may be iterated for the new configuration, \ub7thus performing a dynamical calculation. This approach, however, is computationally extremely expensive, and not feasible when the number of particles is of the order of ten or more...

Lecture notes on Tight-Binding Molecular Dynamics,

and Tight-Binding justification of classical potential