173 research outputs found
The effect of compression on the global optimization of atomic clusters
Recently, Locatelli and Schoen proposed a transformation of the potential
energy that aids the global optimization of Lennard-Jones clusters with
non-icosahedral global minima. These cases are particularly difficult to
optimize because the potential energy surface has a double funnel topography
with the global minimum at the bottom of the narrower funnel. Here we analyse
the effect of this type of transformation on the topography of the potential
energy surface. The transformation, which physically corresponds to a
compression of the cluster, firstly reduces the number of stationary points on
the potential energy surface. Secondly, we show that for a 38-atom cluster with
a face-centred-cubic global minimum the transformation causes the potential
energy surface to become increasingly dominated by the funnel associated with
the global minimum. The transformation has been incorporated in the
basin-hopping algorithm using a two-phase approach.Comment: 9 pages, 6 figures, revte
Computer simulations of the mechanism of thickness selection in polymer crystals
In this paper I describe the computer simulations that I have performed to
critically examine the Lauritzen-Hoffman and the Sadler-Gilmer theories of
polymer crystallization. In particular, I have computed the free energy profile
for nucleation of a new crystalline layer on the growth face to compare with
that assumed by the Lauritzen-Hoffman theory, I have analysed the mechanism of
thickness selection in a multi-pathway model in which some of the constraints
in the Lauritzen-Hoffman theory are relaxed, and I have re-examined the model
used by Sadler-Gilmer. These investigations have lead to a mechanism of
thickness selection of lamellar polymer crystals that differs from the two
theories that I set out to examine.Comment: 9 pages, 11 figures, revte
Structural Consequences of the Range of the Interatomic Potential: a Menagerie of Clusters
We have attempted to find the global minima of clusters containing between 20
and 80 atoms bound by the Morse potential as a function of the range of the
interatomic force. The effect of decreasing the range is to destabilize
strained structures, and hence the global minimum changes from icosahedral to
decahedral to face-centred-cubic as the range is decreased. For N>45 the global
minima associated with a long-ranged potential have polytetrahedral structures
involving defects called disclination lines. For the larger clusters the
network of disclination lines is disordered and the global minimum has an
amorphous structure resembling a liquid. The size evolution of polytetrahedral
packings enables us to study the development of bulk liquid structure in finite
systems. As many experiments on the structure of clusters only provide indirect
structural information, these results will be very useful in aiding the
interpretation of experiment. They also provide candidate structures for
theoretical studies using more specific and computationally expensive
descriptions of the interatomic interactions. Furthermore, Morse clusters
provide a rigorous testing ground for global optimization methods.Comment: 26 pages, 16 figures, revtex. Unabridged version of paper accepted by
J. Chem. Soc., Faraday Tran
Lead clusters: different potentials, different structures
The lowest-energy structures of lead clusters interacting via a Gupta
potential are obtained for N<151. Structures based on Marks decahedra dominate
at the larger sizes. These results are very different from those obtained
previously using a lead glue potential, and the origins of the differences are
related back to differences in the potential.Comment: 6 pages, 4 figures, TAMC4 proceeding
The effect of temperature jumps during polymer crystallization
Temperature changes during the growth of lamellar polymer crystals give rise
to steps on the surface of the crystals. It has recently been suggested that
these steps could provide important insights into the mechanism of polymer
crystallization. In particular, a characterization of the profiles of these
steps might reveal the fixed-point attractor that underlies a recently proposed
crystallization mechanism. Here we examine this hypothesis by performing
simulations of such temperature jumps using the Sadler-Gilmer model. We find
that for this model the step profiles do reveal the fixed-point attractor.
However, for temperature decreases they also reflect the rounding of the
crystal edge that occurs in this model and for temperature increases they also
reflect the fluctuations in the thickness present in the crystal. We discuss
the implications of these results for the interpretation of experimental step
profiles.Comment: 8 pages, 7 figures, revte
The Dynamics of Structural Transitions in Sodium Chloride Clusters
In recent experiments on sodium chloride clusters structural transitions
between nanocrystals with different cuboidal shapes were detected. Here we
presents results for the thermodynamics and dynamics of one of these clusters,
(NaCl)35Cl-. As the time scales for the structural transitions can be much
longer than those accessible by conventional dynamics simulations, we use a
master equation to describe the probability flow within a large sample of
potential energy minima. We characterize the processes contributing to
probability flow between the different nanocrystals, and obtain rate constants
and activation energies for comparison with the experimental values.Comment: 11 pages, 8 figures, revte
Global Minima for Transition Metal Clusters Described by Sutton-Chen Potentials
Using a Monte Carlo minimization approach we report the global minima for
metal clusters modelled by the Sutton-Chen family of potentials with N<81,
where N is the number of atoms. The resulting structures are discussed in the
light of both experimental and theoretical data for clusters of the appropriate
elements.Comment: 16 pages, 7 figures, revte
On the Thermodynamics of Global Optimization
Theoretical design of global optimization algorithms can profitably utilize
recent statistical mechanical treatments of potential energy surfaces (PES's).
Here we analyze a particular method to explain its success in locating global
minima on surfaces with a multiple-funnel structure, where trapping in local
minima with different morphologies is expected. We find that a key factor in
overcoming trapping is the transformation applied to the PES which broadens the
thermodynamic transitions. The global minimum then has a significant
probability of occupation at temperatures where the free energy barriers
between funnels are surmountable.Comment: 4 pages, 3 figures, revte
The mechanism of thickness selection in the Sadler-Gilmer model of polymer crystallization
Recent work on the mechanism of polymer crystallization has led to a proposal
for the mechanism of thickness selection which differs from those proposed by
the surface nucleation theory of Lauritzen and Hoffman and the entropic barrier
model of Sadler and Gilmer. This has motivated us to reexamine the model used
by Sadler and Gilmer. We again find a fixed-point attractor which describes the
dynamical convergence of the crystal thickness to a value just larger than the
minimum stable thickness, l_min. This convergence arises from the combined
effect of two constraints on the length of stems in a layer: it is unfavourable
for a stem to be shorter than l_min and for a stem to overhang the edge of the
previous layer. The relationship between this new mechanism and the explanation
given by Sadler and Gilmer in terms of an entropic barrier is discussed. We
also examine the behaviour of the Sadler-Gilmer model when an energetic
contribution from chain folds is included.Comment: 15 pages, 13 figures, revte
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