142 research outputs found
Communication: Diverse nanoscale cluster dynamics: Diffusion of 2D epitaxial clusters
The dynamics of nanoscale clusters can be distinct from macroscale behavior described by continuum formalisms. For diffusion of 2D clusters of N atoms in homoepitaxial systems mediated by edge atom hopping, macroscale theory predicts simple monotonic size scaling of the diffusion coefficient, DN ∼ N−β, with β = 3/2. However, modeling for nanoclusters on metal(100) surfaces reveals that slow nucleation-mediated diffusion displaying weak size scaling β \u3c 1 occurs for “perfect” sizes Np = L2 and L(L+1) for integer L = 3,4,… (with unique square or near-square ground state shapes), and also for Np+3, Np+4,…. In contrast, fast facile nucleation-free diffusion displaying strong size scaling β ≈ 2.5 occurs for sizes Np+1 and Np+2. DN versus N oscillates strongly between the slowest branch (for Np+3) and the fastest branch (for Np+1). All branches merge for N = O(102), but macroscale behavior is only achieved for much larger N = O(103). This analysis reveals the unprecedented diversity of behavior on the nanoscale
Kinetics of catalysis with surface disorder
We study the effects of generalised surface disorder on the monomer-monomer
model of heterogeneous catalysis, where disorder is implemented by allowing
different adsorption rates for each lattice site. By mapping the system in the
reaction-controlled limit onto a kinetic Ising model, we derive the rate
equations for the one and two-spin correlation functions. There is good
agreement between these equations and numerical simulations. We then study the
inclusion of desorption of monomers from the substrate, first by both species
and then by just one, and find exact time-dependent solutions for the one-spin
correlation functions.Comment: LaTex, 19 pages, 1 figure included, requires epsf.st
Voting and Catalytic Processes with Inhomogeneities
We consider the dynamics of the voter model and of the monomer-monomer
catalytic process in the presence of many ``competing'' inhomogeneities and
show, through exact calculations and numerical simulations, that their presence
results in a nontrivial fluctuating steady state whose properties are studied
and turn out to specifically depend on the dimensionality of the system, the
strength of the inhomogeneities and their separating distances. In fact, in
arbitrary dimensions, we obtain an exact (yet formal) expression of the order
parameters (magnetization and concentration of adsorbed particles) in the
presence of an arbitrary number of inhomogeneities (``zealots'' in the
voter language) and formal similarities with {\it suitable electrostatic
systems} are pointed out. In the nontrivial cases , we explicitly
compute the static and long-time properties of the order parameters and
therefore capture the generic features of the systems. When , the problems
are studied through numerical simulations. In one spatial dimension, we also
compute the expressions of the stationary order parameters in the completely
disordered case, where is arbitrary large. Particular attention is paid to
the spatial dependence of the stationary order parameters and formal
connections with electrostatics.Comment: 17 pages, 6 figures, revtex4 2-column format. Original title ("Are
Voting and Catalytic Processes Electrostatic Problems ?") changed upon
editorial request. Minor typos corrected. Published in Physical Review
Island diffusion on metal fcc(100) surfaces
We present Monte Carlo simulations for the size and temperature dependence of
the diffusion coefficient of adatom islands on the Cu(100) surface. We show
that the scaling exponent for the size dependence is not a constant but a
decreasing function of the island size and approaches unity for very large
islands. This is due to a crossover from periphery dominated mass transport to
a regime where vacancies diffuse inside the island. The effective scaling
exponents are in good agreement with theory and experiments.Comment: 13 pages, 2 figures, to be published in Phys. Rev. Let
Rejection-free Monte-Carlo sampling for general potentials
A Monte Carlo method to sample the classical configurational canonical
ensemble is introduced. In contrast to the Metropolis algorithm, where trial
moves can be rejected, in this approach collisions take place. The
implementation is event-driven, i.e., at scheduled times the collisions occur.
A unique feature of the new method is that smooth potentials (instead of only
step-wise changing ones) can be used. Besides an event-driven approach where
all particles move simultaneously, we also introduce a straight event-chain
implementation. As proof-of-principle a system of Lennard-Jones particles is
simulated
Influence of auto-organization and fluctuation effects on the kinetics of a monomer-monomer catalytic scheme
We study analytically kinetics of an elementary bimolecular reaction scheme
of the Langmuir-Hinshelwood type taking place on a d-dimensional catalytic
substrate. We propose a general approach which takes into account explicitly
the influence of spatial correlations on the time evolution of particles mean
densities and allows for the analytical analysis. In terms of this approach we
recover some of known results concerning the time evolution of particles mean
densities and establish several new ones.Comment: Latex, 25 pages, one figure, submitted to J. Chem. Phy
Domain Growth and Finite-Size-Scaling in the Kinetic Ising Model
This paper describes the application of finite-size scaling concepts to
domain growth in systems with a non-conserved order parameter. A finite-size
scaling ansatz for the time-dependent order parameter distribution function is
proposed, and tested with extensive Monte-Carlo simulations of domain growth in
the 2-D spin-flip kinetic Ising model. The scaling properties of the
distribution functions serve to elucidate the configurational self-similarity
that underlies the dynamic scaling picture. Moreover, it is demonstrated that
the application of finite-size-scaling techniques facilitates the accurate
determination of the bulk growth exponent even in the presence of strong
finite-size effects, the scale and character of which are graphically exposed
by the order parameter distribution function. In addition it is found that one
commonly used measure of domain size--the scaled second moment of the
magnetisation distribution--belies the full extent of these finite-size
effects.Comment: 13 pages, Latex. Figures available on request. Rep #9401
Implication of the overlap representation for modelling generalized parton distributions
Based on a field theoretically inspired model of light-cone wave functions,
we derive valence-like generalized parton distributions and their double
distributions from the wave function overlap in the parton number conserved
s-channel. The parton number changing contributions in the t-channel are
restored from duality. In our construction constraints of positivity and
polynomiality are simultaneously satisfied and it also implies a model
dependent relation between generalized parton distributions and transverse
momentum dependent parton distribution functions. The model predicts that the
t-behavior of resulting hadronic amplitudes depends on the Bjorken variable
x_Bj. We also propose an improved ansatz for double distributions that embeds
this property.Comment: 15 pages, 8 eps figure
Soluble two-species diffusion-limited Models in arbitrary dimensions
A class of two-species ({\it three-states}) bimolecular diffusion-limited
models of classical particles with hard-core reacting and diffusing in a
hypercubic lattice of arbitrary dimension is investigated. The manifolds on
which the equations of motion of the correlation functions close, are
determined explicitly. This property allows to solve for the density and the
two-point (two-time) correlation functions in arbitrary dimension for both, a
translation invariant class and another one where translation invariance is
broken. Systems with correlated as well as uncorrelated, yet random initial
states can also be treated exactly by this approach. We discuss the asymptotic
behavior of density and correlation functions in the various cases. The
dynamics studied is very rich.Comment: 28 pages, 0 figure. To appear in Physical Review E (February 2001
Ab initio atomistic thermodynamics and statistical mechanics of surface properties and functions
Previous and present "academic" research aiming at atomic scale understanding
is mainly concerned with the study of individual molecular processes possibly
underlying materials science applications. Appealing properties of an
individual process are then frequently discussed in terms of their direct
importance for the envisioned material function, or reciprocally, the function
of materials is somehow believed to be understandable by essentially one
prominent elementary process only. What is often overlooked in this approach is
that in macroscopic systems of technological relevance typically a large number
of distinct atomic scale processes take place. Which of them are decisive for
observable system properties and functions is then not only determined by the
detailed individual properties of each process alone, but in many, if not most
cases also the interplay of all processes, i.e. how they act together, plays a
crucial role. For a "predictive materials science modeling with microscopic
understanding", a description that treats the statistical interplay of a large
number of microscopically well-described elementary processes must therefore be
applied. Modern electronic structure theory methods such as DFT have become a
standard tool for the accurate description of individual molecular processes.
Here, we discuss the present status of emerging methodologies which attempt to
achieve a (hopefully seamless) match of DFT with concepts from statistical
mechanics or thermodynamics, in order to also address the interplay of the
various molecular processes. The new quality of, and the novel insights that
can be gained by, such techniques is illustrated by how they allow the
description of crystal surfaces in contact with realistic gas-phase
environments.Comment: 24 pages including 17 figures, related publications can be found at
http://www.fhi-berlin.mpg.de/th/paper.htm
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