281 research outputs found
Thermodynamically Stable One-Component Metallic Quasicrystals
Classical density-functional theory is employed to study finite-temperature
trends in the relative stabilities of one-component quasicrystals interacting
via effective metallic pair potentials derived from pseudopotential theory.
Comparing the free energies of several periodic crystals and rational
approximant models of quasicrystals over a range of pseudopotential parameters,
thermodynamically stable quasicrystals are predicted for parameters approaching
the limits of mechanical stability of the crystalline structures. The results
support and significantly extend conclusions of previous ground-state
lattice-sum studies.Comment: REVTeX, 13 pages + 2 figures, to appear, Europhys. Let
Lattice density-functional theory of surface melting: the effect of a square-gradient correction
I use the method of classical density-functional theory in the
weighted-density approximation of Tarazona to investigate the phase diagram and
the interface structure of a two-dimensional lattice-gas model with three
phases -- vapour, liquid, and triangular solid. While a straightforward
mean-field treatment of the interparticle attraction is unable to give a stable
liquid phase, the correct phase diagram is obtained when including a suitably
chosen square-gradient term in the system grand potential. Taken this theory
for granted, I further examine the structure of the solid-vapour interface as
the triple point is approached from low temperature. Surprisingly, a novel
phase (rather than the liquid) is found to grow at the interface, exhibiting an
unusually long modulation along the interface normal. The conventional
surface-melting behaviour is recovered only by artificially restricting the
symmetries being available to the density field.Comment: 16 pages, 6 figure
Weighted-density approximation for general nonuniform fluid mixtures
In order to construct a general density-functional theory for nonuniform
fluid mixtures, we propose an extension to multicomponent systems of the
weighted-density approximation (WDA) of Curtin and Ashcroft [Phys. Rev. A 32,
2909 (1985)]. This extension corrects a deficiency in a similar extension
proposed earlier by Denton and Ashcroft [Phys. Rev. A 42, 7312 (1990)], in that
that functional cannot be applied to the multi-component nonuniform fluid
systems with spatially varying composition, such as solid-fluid interfaces. As
a test of the accuracy of our new functional, we apply it to the calculation of
the freezing phase diagram of a binary hard-sphere fluid, and compare the
results to simulation and the Denton-Ashcroft extension.Comment: 4 pages, 4 figures, to appear in Phys. Rev. E as Brief Repor
Density-Functional Theory of Quantum Freezing: Sensitivity to Liquid-State Structure and Statistics
Density-functional theory is applied to compute the ground-state energies of
quantum hard-sphere solids. The modified weighted-density approximation is used
to map both the Bose and the Fermi solid onto a corresponding uniform Bose
liquid, assuming negligible exchange for the Fermi solid. The required
liquid-state input data are obtained from a paired phonon analysis and the
Feynman approximation, connecting the static structure factor and the linear
response function. The Fermi liquid is treated by the Wu-Feenberg cluster
expansion, which approximately accounts for the effects of antisymmetry.
Liquid-solid transitions for both systems are obtained with no adjustment of
input data. Limited quantitative agreement with simulation indicates a need for
further improvement of the liquid-state input through practical alternatives to
the Feynman approximation.Comment: IOP-TeX, 21 pages + 7 figures, to appear, J. Phys.: Condens. Matte
Polydispersity and ordered phases in solutions of rodlike macromolecules
We apply density functional theory to study the influence of polydispersity
on the stability of columnar, smectic and solid ordering in the solutions of
rodlike macromolecules. For sufficiently large length polydispersity (standard
deviation ) a direct first-order nematic-columnar transition is
found, while for smaller there is a continuous nematic-smectic and
first-order smectic-columnar transition. For increasing polydispersity the
columnar structure is stabilized with respect to solid perturbations. The
length distribution of macromolecules changes neither at the nematic-smectic
nor at the nematic-columnar transition, but it does change at the
smectic-columnar phase transition. We also study the phase behaviour of binary
mixtures, in which the nematic-smectic transition is again found to be
continuous. Demixing according to rod length in the smectic phase is always
preempted by transitions to solid or columnar ordering.Comment: 13 pages (TeX), 2 Postscript figures uuencode
Direct calculation of the hard-sphere crystal/melt interfacial free energy
We present a direct calculation by molecular-dynamics computer simulation of
the crystal/melt interfacial free energy, , for a system of hard
spheres of diameter . The calculation is performed by thermodynamic
integration along a reversible path defined by cleaving, using specially
constructed movable hard-sphere walls, separate bulk crystal and fluid systems,
which are then merged to form an interface. We find the interfacial free energy
to be slightly anisotropic with = 0.62, 0.64 and
0.58 for the (100), (110) and (111) fcc crystal/fluid
interfaces, respectively. These values are consistent with earlier density
functional calculations and recent experiments measuring the crystal nucleation
rates from colloidal fluids of polystyrene spheres that have been interpreted
[Marr and Gast, Langmuir {\bf 10}, 1348 (1994)] to give an estimate of
for the hard-sphere system of , slightly lower
than the directly determined value reported here.Comment: 4 pages, 4 figures, submitted to Physical Review Letter
Molecular dynamics study of melting of a bcc metal-vanadium II : thermodynamic melting
We present molecular dynamics simulations of the thermodynamic melting
transition of a bcc metal, vanadium using the Finnis-Sinclair potential. We
studied the structural, transport and energetic properties of slabs made of 27
atomic layers with a free surface. We investigated premelting phenomena at the
low-index surfaces of vanadium; V(111), V(001), and V(011), finding that as the
temperature increases, the V(111) surface disorders first, then the V(100)
surface, while the V(110) surface remains stable up to the melting temperature.
Also, as the temperature increases, the disorder spreads from the surface layer
into the bulk, establishing a thin quasiliquid film in the surface region. We
conclude that the hierarchy of premelting phenomena is inversely proportional
to the surface atomic density, being most pronounced for the V(111) surface
which has the lowest surface density
The low temperature interface between the gas and solid phases of hard spheres with a short-ranged attraction
At low temperature, spheres with a very short-ranged attraction exist as a
close-packed solid coexisting with an infinitely dilute gas. We find that the
ratio of the interfacial tension between these two phases to the thermal energy
diverges as the range of the attraction goes to zero. The large tensions when
the interparticle attractions are short-ranged may be why globular proteins
only crystallise over a narrow range of conditions.Comment: 6 pages, no figures (v2 has change of notation to agree with that of
Stell
Crater formation by fast ions: comparison of experiment with Molecular Dynamics simulations
An incident fast ion in the electronic stopping regime produces a track of
excitations which can lead to particle ejection and cratering. Molecular
Dynamics simulations of the evolution of the deposited energy were used to
study the resulting crater morphology as a function of the excitation density
in a cylindrical track for large angle of incidence with respect to the surface
normal. Surprisingly, the overall behavior is shown to be similar to that seen
in the experimental data for crater formation in polymers. However, the
simulations give greater insight into the cratering process. The threshold for
crater formation occurs when the excitation density approaches the cohesive
energy density, and a crater rim is formed at about six times that energy
density. The crater length scales roughly as the square root of the electronic
stopping power, and the crater width and depth seem to saturate for the largest
energy densities considered here. The number of ejected particles, the
sputtering yield, is shown to be much smaller than simple estimates based on
crater size unless the full crater morphology is considered. Therefore, crater
size can not easily be used to estimate the sputtering yield.Comment: LaTeX, 7 pages, 5 EPS figures. For related figures/movies, see:
http://dirac.ms.virginia.edu/~emb3t/craters/craters.html New version uploaded
5/16/01, with minor text changes + new figure
Effective forces in colloidal mixtures: from depletion attraction to accumulation repulsion
Computer simulations and theory are used to systematically investigate how
the effective force between two big colloidal spheres in a sea of small spheres
depends on the basic (big-small and small-small) interactions. The latter are
modeled as hard-core pair potentials with a Yukawa tail which can be both
repulsive or attractive. For a repulsive small-small interaction, the effective
force follows the trends as predicted by a mapping onto an effective
non-additive hard-core mixture: both a depletion attraction and an accumulation
repulsion caused by small spheres adsorbing onto the big ones can be obtained
depending on the sign of the big-small interaction. For repulsive big-small
interactions, the effect of adding a small-small attraction also follows the
trends predicted by the mapping. But a more subtle ``repulsion through
attraction'' effect arises when both big-small and small-small attractions
occur: upon increasing the strength of the small-small interaction, the
effective potential becomes more repulsive. We have further tested several
theoretical methods against our computer simulations: The superposition
approximation works best for an added big-small repulsion, and breaks down for
a strong big-small attraction, while density functional theory is very accurate
for any big-small interaction when the small particles are pure hard-spheres.
The theoretical methods perform most poorly for small-small attractions.Comment: submitted to PRE; New version includes an important quantitative
correction to several of the simulations. The main conclusions remain
unchanged thoug
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