115 research outputs found
Realistic simulations of Au(100): Grand Canonical Monte Carlo and Molecular Dynamics
The large surface density changes associated with the (100) noble metals
surface hex-reconstruction suggest the use of non-particle conserving
simulation methods. We present an example of a surface Grand Canonical Monte
Carlo applied to the transformation of a square non reconstructed surface to
the hexagonally covered low temperature stable Au(100). On the other hand,
classical Molecular Dynamics allows to investigate microscopic details of the
reconstruction dynamics, and we show, as an example, retraction of a step and
its interplay with the surface reconstruction/deconstruction mechanism.Comment: 9 pages, 5 figures, accepted for publication in Surf. Rev. and
Letters (ICSOS-6
Ab initio simulations of the Ag(111)/Al2O3 interface at intermediate oxygen partial pressures
The relative stability of different realizations of the Ag(111)/Alumina interfaces with varying oxygen partial pressures is investigated by means of ab initio density functional theory (DFT) simulations. Previous theoretical studies of similar systems always involve oversimplified geometries like stoichiometric Al-terminated, Al-rich, or O-terminated alumina interfaces. Such framework cannot explain the experimental behavior observed at intermediate oxygen partial pressure. Our approach, instead, suggests that the oxygen at the interface can play an important role at intermediate concentrations, leading to a more realistic interpretation of the experimental dat
Bent surface free energy differences from simulation
We present a calculation of the change of free energy of a solid surface upon
bending of the solid. It is based on extracting the surface stress through a
molecular dynamics simulation of a bent slab by using a generalized stress
theorem formula, and subsequent integration of the stress with respect to
strain as a function of bending curvature. The method is exemplified by
obtaining and comparing free energy changes with curvature of various
reconstructed Au(001) surfaces.Comment: 14 pages, 2 figures, accepted for publication in Surface Science
(ECOSS-19
A simple approach for describing metal-supported cyclohexaphenylene dehydrogenation: Hybrid classical/DFT metadynamics simulations
The mechanisms for the dehydrogenation reaction of cyclohexaphenylene at a copper surface are investigated with the help of density functional theory and metadynamics. Our results represent a showcase for an approach that describes the surface using many-body classical potentials and molecule-surface interactions with a van der Waals model. Starting from the experimental observation that dispersion-assisted mechanisms are at least as important as catalytic processes for the description of the reaction, we fully describe the former, we identify intermediate states and estimate the free energy barriers that characterize the reactio
Two-Stage Rotational Disordering of a Molecular Crystal Surface: C60
We propose a two-stage mechanism for the rotational surface disordering phase
transition of a molecular crystal, as realized in C fullerite. Our
study, based on Monte Carlo simulations, uncovers the existence of a new
intermediate regime, between a low temperature ordered state,
and a high temperature disordered phase. In the intermediate
regime there is partial disorder, strongest for a subset of particularly
frustrated surface molecules. These concepts and calculations provide a
coherent understanding of experimental observations, with possible extension to
other molecular crystal surfaces.Comment: 4 pages, 2 figure
String Method for the Study of Rare Events
We present a new and efficient method for computing the transition pathways,
free energy barriers, and transition rates in complex systems with relatively
smooth energy landscapes. The method proceeds by evolving strings, i.e. smooth
curves with intrinsic parametrization whose dynamics takes them to the most
probable transition path between two metastable regions in the configuration
space. Free energy barriers and transition rates can then be determined by
standard umbrella sampling technique around the string. Applications to
Lennard-Jones cluster rearrangement and thermally induced switching of a
magnetic film are presented.Comment: 4 pages, 4 figure
Feedback Loops Between Fields and Underlying Space Curvature: an Augmented Lagrangian Approach
We demonstrate a systematic implementation of coupling between a scalar field
and the geometry of the space (curve, surface, etc.) which carries the field.
This naturally gives rise to a feedback mechanism between the field and the
geometry. We develop a systematic model for the feedback in a general form,
inspired by a specific implementation in the context of molecular dynamics (the
so-called Rahman-Parrinello molecular dynamics, or RP-MD). We use a generalized
Lagrangian that allows for the coupling of the space's metric tensor (the first
fundamental form) to the scalar field, and add terms motivated by RP-MD. We
present two implementations of the scheme: one in which the metric is only
time-dependent [which gives rise to ordinary differential equation (ODE) for
its temporal evolution], and one with spatio-temporal dependence [wherein the
metric's evolution is governed by a partial differential equation (PDE)].
Numerical results are reported for the (1+1)-dimensional model with a
nonlinearity of the sine-Gordon type.Comment: 5 pages, 3 figures, Phys. Rev. E in pres
A Geometric Formulation of Quantum Stress Fields
We present a derivation of the stress field for an interacting quantum system
within the framework of local density functional theory. The formulation is
geometric in nature and exploits the relationship between the strain tensor
field and Riemannian metric tensor field. Within this formulation, we
demonstrate that the stress field is unique up to a single ambiguous parameter.
The ambiguity is due to the non-unique dependence of the kinetic energy on the
metric tensor. To illustrate this formalism, we compute the pressure field for
two phases of solid molecular hydrogen. Furthermore, we demonstrate that
qualitative results obtained by interpreting the hydrogen pressure field are
not influenced by the presence of the kinetic ambiguity.Comment: 22 pages, 2 figures. Submitted to Physical Review B. This paper
supersedes cond-mat/000627
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