288 research outputs found
Structural and energetic properties of nickel clusters:
The four most stable structures of Ni clusters with from 2 to 150
have been determined using a combination of the embedded-atom method in the
version of Daw, Baskes and Foiles, the {\it variable metric/quasi-Newton}
method, and our own {\it Aufbau/Abbau} method. A systematic study of
energetics, structure, growth, and stability of also larger clusters has been
carried through without more or less severe assumptions on the initial
geometries in the structure optimization, on the symmetry, or on bond lengths.
It is shown that cluster growth is predominantly icosahedral with of
{\it fcc}, {\it tetrahedral} and {\it decahedral} growth. For the first time in
unbiased computations it is found that Ni is the multilayer (third
Mackay) icosahedron. Further, we point to an enhanced ability of {\it fcc}
clusters to compete with the icosahedral and decahedral structures in the
vicinity of N=79. In addition, it is shown that conversion from the {\it
hcp}/anti-Mackay kind of icosahedral growth to the {\it fcc}/Mackay one occurs
within a transition layer including several cluster sizes. Moreover, we present
and apply different analytical tools in studying structural and energetic
properties of such a large class of clusters. These include means for
identifying the overall shape, the occurrence of atomic shells, the similarity
of the clusters with, e.g., fragments of the {\it fcc} crystal or of a large
icosahedral cluster, and a way of analysing whether the -atom cluster can be
considered constructed from the -atom one by adding an extra atom. In
addition, we compare in detail with results from chemical-probe experiment.
Maybe the most central result is that first for clusters with above 80
general trends can be identified.Comment: 37 pages, 11 figure
Diffusion-limited reactions on a two-dimensional lattice with binary disorder
Reaction-diffusion systems where transition rates exhibit quenched disorder
are common in physical and chemical systems. We study pair reactions on a
periodic two-dimensional lattice, including continuous deposition and
spontaneous desorption of particles. Hopping and desorption are taken to be
thermally activated processes. The activation energies are drawn from a binary
distribution of well depths, corresponding to `shallow' and `deep' sites. This
is the simplest non-trivial distribution, which we use to examine and explain
fundamental features of the system. We simulate the system using kinetic Monte
Carlo methods and provide a thorough understanding of our findings. We show
that the combination of shallow and deep sites broadens the temperature window
in which the reaction is efficient, compared to either homogeneous system. We
also examine the role of spatial correlations, including systems where one type
of site is arranged in a cluster or a sublattice. Finally, we show that a
simple rate equation model reproduces simulation results with very good
accuracy.Comment: 9 pages, 5 figure
Effects of jamming on non-equilibrium transport times in nano-channels
Many biological channels perform highly selective transport without direct
input of metabolic energy and without transitions from a 'closed' to an 'open'
state during transport. Mechanisms of selectivity of such channels serve as an
inspiration for creation of artificial nano-molecular sorting devices and
bio-sensors. To elucidate the transport mechanisms, it is important to
understand the transport on the single molecule level in the experimentally
relevant regime when multiple particles are crowded in the channel. In this
paper we analyze the effects of inter-particle crowding on the non-equilibrium
transport times through a finite-length channel by means of analytical theory
and computer simulations
Efficiency of Rejection-Free Methods for Dynamic Monte Carlo Studies of Off-lattice Interacting Particles
We calculate the efficiency of a rejection-free dynamic Monte Carlo method
for -dimensional off-lattice homogeneous particles interacting through a
repulsive power-law potential . Theoretically we find the algorithmic
efficiency in the limit of low temperatures and/or high densities is
asymptotically proportional to with
the particle density and the temperature . Dynamic Monte Carlo
simulations are performed in 1-, 2- and 3-dimensional systems with different
powers , and the results agree with the theoretical predictions.Comment: revtex4, 4 pages, 6 figure
The Decay Properties of the Finite Temperature Density Matrix in Metals
Using ordinary Fourier analysis, the asymptotic decay behavior of the density
matrix F(r,r') is derived for the case of a metal at a finite electronic
temperature. An oscillatory behavior which is damped exponentially with
increasing distance between r and r' is found. The decay rate is not only
determined by the electronic temperature, but also by the Fermi energy. The
theoretical predictions are confirmed by numerical simulations
Smoluchowski ripening of Ag islands on Ag(100)
Using scanning tunneling microscopy, we study the post-deposition coarsening of distributions of large, two-dimensional Ag islands on a perfect Ag(100) surface at 295 K. The coarsening process is dominated by diffusion, and subsequent collision and coalescence of these islands. To obtain a comprehensive characterization of the coarsening kinetics, we perform tailored families of experiments, systematically varying the initial value of the average island size by adjusting the amount of Ag deposited (up to 0.25 ML). Results unambiguously indicate a strong decrease in island diffusivity with increasing island size. An estimate of the size scaling exponent follows from a mean-field Smoluchowski rate equation analysis of experimental data. These rate equations also predict a rapid depletion in the initial population of smaller islands. This leads to narrowing of the size distribution scaling function from its initial form, which is determined by the process of island nucleation and growth during deposition. However, for later times, a steady increase in the width of this scaling function is predicted, consistent with observed behavior. Finally, we examine the evolution of Ag adlayers on a strained Ag(100) surface, and find significantly enhanced rates for island diffusion and coarsening
Changing shapes in the nanoworld
What are the mechanisms leading to the shape relaxation of three dimensional
crystallites ? Kinetic Monte Carlo simulations of fcc clusters show that the
usual theories of equilibration, via atomic surface diffusion driven by
curvature, are verified only at high temperatures. Below the roughening
temperature, the relaxation is much slower, kinetics being governed by the
nucleation of a critical germ on a facet. We show that the energy barrier for
this step linearly increases with the size of the crystallite, leading to an
exponential dependence of the relaxation time.Comment: 4 pages, 5 figures. Accepted by Phys Rev Let
Fragmentation pathways of nanofractal structures on surface
We present a detailed systematical theoretical analysis of the post-growth
processes occurring in nanofractals grown on surface. For this study we
developed a method which accounts for the internal dynamics of particles in a
fractal. We demonstrate that particle diffusion and detachment controls the
shape of the emerging stable islands on surface. We consider different
scenarios of fractal post-growth relaxation and analyze the time evolution of
the island's morphology. The results of our calculations are compared with
available experimental observations, and experiments in which the post-growth
relaxation of deposited nanostructures can be probed are suggested.Comment: 34 pages, 11 figure
Rate theory for correlated processes: Double-jumps in adatom diffusion
We study the rate of activated motion over multiple barriers, in particular
the correlated double-jump of an adatom diffusing on a missing-row
reconstructed Platinum (110) surface. We develop a Transition Path Theory,
showing that the activation energy is given by the minimum-energy trajectory
which succeeds in the double-jump. We explicitly calculate this trajectory
within an effective-medium molecular dynamics simulation. A cusp in the
acceptance region leads to a sqrt{T} prefactor for the activated rate of
double-jumps. Theory and numerical results agree
Event-based relaxation of continuous disordered systems
A computational approach is presented to obtain energy-minimized structures
in glassy materials. This approach, the activation-relaxation technique (ART),
achieves its efficiency by focusing on significant changes in the microscopic
structure (events). The application of ART is illustrated with two examples:
the structure of amorphous silicon, and the structure of Ni80P20, a metallic
glass.Comment: 4 pages, revtex, epsf.sty, 3 figure
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