1,209 research outputs found
Fractionation effects in phase equilibria of polydisperse hard sphere colloids
The equilibrium phase behaviour of hard spheres with size polydispersity is
studied theoretically. We solve numerically the exact phase equilibrium
equations that result from accurate free energy expressions for the fluid and
solid phases, while accounting fully for size fractionation between coexisting
phases. Fluids up to the largest polydispersities that we can study (around
14%) can phase separate by splitting off a solid with a much narrower size
distribution. This shows that experimentally observed terminal polydispersities
above which phase separation no longer occurs must be due to non-equilibrium
effects. We find no evidence of re-entrant melting; instead, sufficiently
compressed solids phase separate into two or more solid phases. Under
appropriate conditions, coexistence of multiple solids with a fluid phase is
also predicted. The solids have smaller polydispersities than the parent phase
as expected, while the reverse is true for the fluid phase, which contains
predominantly smaller particles but also residual amounts of the larger ones.
The properties of the coexisting phases are studied in detail; mean diameter,
polydispersity and volume fraction of the phases all reveal marked
fractionation. We also propose a method for constructing quantities that
optimally distinguish between the coexisting phases, using Principal Component
Analysis in the space of density distributions. We conclude by comparing our
predictions to perturbative theories for near-monodisperse systems and to Monte
Carlo simulations at imposed chemical potential distribution, and find
excellent agreement.Comment: 21 pages, 23 figures, 2 table
Incorporation of excluded volume correlations into Poisson-Boltzmann theory
We investigate the effect of excluded volume interactions on the electrolyte
distribution around a charged macroion. First, we introduce a criterion for
determining when hard-core effects should be taken into account beyond standard
mean field Poisson-Boltzmann (PB) theory. Next, we demonstrate that several
commonly proposed local density functional approaches for excluded volume
interactions cannot be used for this purpose. Instead, we employ a non-local
excess free energy by using a simple constant weight approach. We compare the
ion distribution and osmotic pressure predicted by this theory with Monte Carlo
simulations. They agree very well for weakly developed correlations and give
the correct layering effect for stronger ones. In all investigated cases our
simple weighted density theory yields more realistic results than the standard
PB approach, whereas all local density theories do not improve on the PB
density profiles but on the contrary, deviate even more from the simulation
results.Comment: 23 pages, 7 figures, 1 tabl
A cluster theory for a Janus fluid
Recent Monte Carlo simulations on the Kern and Frenkel model of a Janus fluid
have revealed that in the vapour phase there is the formation of preferred
clusters made up of a well-defined number of particles: the micelles and the
vesicles. A cluster theory is developed to approximate the exact clustering
properties stemming from the simulations. It is shown that the theory is able
to reproduce the micellisation phenomenon.Comment: 27 pages, 8 figures, 6 table
Density Functional for Anisotropic Fluids
We propose a density functional for anisotropic fluids of hard body
particles. It interpolates between the well-established geometrically based
Rosenfeld functional for hard spheres and the Onsager functional for elongated
rods. We test the new approach by calculating the location of the the
nematic-isotropic transition in systems of hard spherocylinders and hard
ellipsoids. The results are compared with existing simulation data. Our
functional predicts the location of the transition much more accurately than
the Onsager functional, and almost as good as the theory by Parsons and Lee. We
argue that it might be suited to study inhomogeneous systems.Comment: To appear in J. Physics: Condensed Matte
Phase separation in mixtures of colloids and long ideal polymer coils
Colloidal suspensions with free polymer coils which are larger than the
colloidal particles are considered. The polymer-colloid interaction is modeled
by an extension of the Asakura-Oosawa model. Phase separation occurs into
dilute and dense fluid phases of colloidal particles when polymer is added. The
critical density of this transition tends to zero as the size of the polymer
coils diverges.Comment: 5 pages, 3 figure
Nodal quasiparticle meltdown in ultra-high resolution pump-probe angle-resolved photoemission
High- cuprate superconductors are characterized by a strong
momentum-dependent anisotropy between the low energy excitations along the
Brillouin zone diagonal (nodal direction) and those along the Brillouin zone
face (antinodal direction). Most obvious is the d-wave superconducting gap,
with the largest magnitude found in the antinodal direction and no gap in the
nodal direction. Additionally, while antinodal quasiparticle excitations appear
only below , superconductivity is thought to be indifferent to nodal
excitations as they are regarded robust and insensitive to . Here we
reveal an unexpected tie between nodal quasiparticles and superconductivity
using high resolution time- and angle-resolved photoemission on optimally doped
BiSrCaCuO. We observe a suppression of the nodal
quasiparticle spectral weight following pump laser excitation and measure its
recovery dynamics. This suppression is dramatically enhanced in the
superconducting state. These results reduce the nodal-antinodal dichotomy and
challenge the conventional view of nodal excitation neutrality in
superconductivity.Comment: 7 pages, 3 figure. To be published in Nature Physic
Mode-coupling theory for multiple-time correlation functions of tagged particle densities and dynamical filters designed for glassy systems
The theoretical framework for higher-order correlation functions involving
multiple times and multiple points in a classical, many-body system developed
by Van Zon and Schofield [Phys. Rev. E 65, 011106 (2002)] is extended here to
include tagged particle densities. Such densities have found an intriguing
application as proposed measures of dynamical heterogeneities in structural
glasses. The theoretical formalism is based upon projection operator techniques
which are used to isolate the slow time evolution of dynamical variables by
expanding the slowly-evolving component of arbitrary variables in an infinite
basis composed of the products of slow variables of the system. The resulting
formally exact mode-coupling expressions for multiple-point and multiple-time
correlation functions are made tractable by applying the so-called N-ordering
method. This theory is used to derive for moderate densities the leading mode
coupling expressions for indicators of relaxation type and domain relaxation,
which use dynamical filters that lead to multiple-time correlations of a tagged
particle density. The mode coupling expressions for higher order correlation
functions are also succesfully tested against simulations of a hard sphere
fluid at relatively low density.Comment: 15 pages, 2 figure
Multiple-Point and Multiple-Time Correlations Functions in a Hard-Sphere Fluid
A recent mode coupling theory of higher-order correlation functions is tested
on a simple hard-sphere fluid system at intermediate densities. Multi-point and
multi-time correlation functions of the densities of conserved variables are
calculated in the hydrodynamic limit and compared to results obtained from
event-based molecular dynamics simulations. It is demonstrated that the mode
coupling theory results are in excellent agreement with the simulation results
provided that dissipative couplings are included in the vertices appearing in
the theory. In contrast, simplified mode coupling theories in which the
densities obey Gaussian statistics neglect important contributions to both the
multi-point and multi-time correlation functions on all time scales.Comment: Second one in a sequence of two (in the first, the formalism was
developed). 12 pages REVTeX. 5 figures (eps). Submitted to Phys.Rev.
Ninth and Tenth Order Virial Coefficients for Hard Spheres in D Dimensions
We evaluate the virial coefficients B_k for k<=10 for hard spheres in
dimensions D=2,...,8. Virial coefficients with k even are found to be negative
when D>=5. This provides strong evidence that the leading singularity for the
virial series lies away from the positive real axis when D>=5. Further analysis
provides evidence that negative virial coefficients will be seen for some k>10
for D=4, and there is a distinct possibility that negative virial coefficients
will also eventually occur for D=3.Comment: 33 pages, 12 figure
Pressure Dependence of Born Effective Charges, Dielectric Constant and Lattice Dynamics in SiC
The pressure dependence of the Born effective charge, dielectric constant and
zone-center LO and TO phonons have been determined for -SiC by a linear
response method based on the linearized augmented plane wave calculations
within the local density approximation. The Born effective charges are found to
increase nearly linearly with decreasing volume down to the smallest volume
studied, , corresponding to a pressure of about 0.8 Mbar. This
seems to be in contradiction with the conclusion of the turnover behavior
recently reported by Liu and Vohra [Phys.\ Rev.\ Lett.\ {\bf 72}, 4105 (1994)]
for -SiC. Reanalyzing their procedure to extract the pressure dependence of
the Born effective charges, we suggest that the turnover behavior they obtained
is due to approximations in the assumed pressure dependence of the dielectric
constant , the use of a singular set of experimental data
for the equation of state, and the uncertainty in measured phonon frequencies,
especially at high pressure.Comment: 25 pages, revtex, 5 postscript figures appended, to be published in
Phys. Rev.
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