87,174 research outputs found
Carbonate Formation in Non-Aqueous Environments by Solid-Gas Carbonation of Silicates
We have produced synthetic analogues of cosmic silicates using the Sol Gel
method, producing amorphous silicates of composition Mg(x)Ca(1-x)SiO3. Using
synchrotron X-ray powder diffraction on Beamline I11 at the Diamond Light
Source, together with a newly-commissioned gas cell, real-time powder
diffraction scans have been taken of a range of silicates exposed to CO2 under
non-ambient conditions. The SXPD is complemented by other techniques including
Raman and Infrared Spectroscopy and SEM imaging.Comment: 5 pages, 3 figures. Contribution to the Proceedings of the First
European Conference on Laboratory Astrophysics (ECLA
A model colloidal fluid with competing interactions: bulk and interfacial properties
Using a simple mean-field density functional theory theory (DFT), we
investigate the structure and phase behaviour of a model colloidal fluid
composed of particles interacting via a pair potential which has a hard core of
diameter , is attractive Yukawa at intermediate separations and
repulsive Yukawa at large separations. We analyse the form of the asymptotic
decay of the bulk fluid correlation functions, comparing results from our DFT
with those from the self consistent Ornstein-Zernike approximation (SCOZA). In
both theories we find rich crossover behaviour, whereby the ultimate decay of
correlation functions changes from monotonic to long-wavelength damped
oscillatory decay on crossing certain lines in the phase diagram, or sometimes
from oscillatory to oscillatory with a longer wavelength. For some choices of
potential parameters we find, within the DFT, a -line at which the
fluid becomes unstable with respect to periodic density fluctuations. SCOZA
fails to yield solutions for state points near such a -line. The
propensity to clustering of particles, which is reflected by the presence of a
long wavelength , slowly decaying oscillatory pair correlation
function, and a structure factor that exhibits a very sharp maximum at small
but non zero wavenumbers, is enhanced in states near the -line. We
present density profiles for the planar liquid-gas interface and for fluids
adsorbed at a planar hard wall. The presence of a nearby -transition
gives rise to pronounced long-wavelength oscillations in the one-body densities
at both types of interface.Comment: 14 pages, 11 figure
Solvent mediated interactions between model colloids and interfaces: A microscopic approach
We determine the solvent mediated contribution to the effective potentials
for model colloidal or nano- particles dispersed in a binary solvent that
exhibits fluid-fluid phase separation. Using a simple density functional theory
we calculate the density profiles of both solvent species in the presence of
the `colloids', which are treated as external potentials, and determine the
solvent mediated (SM) potentials. Specifically, we calculate SM potentials
between (i) two colloids, (ii) a colloid and a planar fluid-fluid interface,
and (iii) a colloid and a planar wall with an adsorbed wetting film. We
consider three different types of colloidal particles: colloid A which prefers
the bulk solvent phase rich in species 2, colloid C which prefers the solvent
phase rich in species 1, and `neutral' colloid B which has no strong preference
for either phase, i.e. the free energies to insert the colloid into either of
the coexisting bulk phases are almost equal. When a colloid which has a
preference for one of the two solvent phases is inserted into the disfavored
phase at statepoints close to coexistence a thick adsorbed `wetting' film of
the preferred phase may form around the colloids. The presence of the adsorbed
film has a profound influence on the form of the SM potentials.Comment: 17 Pages, 13 Figures. Accepted for publication in Journal of Chemical
Physic
Is there Ornstein-Zernike equation in the canonical ensemble?
A general density-functional formalism using an extended variable-space is
presented for classical fluids in the canonical ensemble (CE). An exact
equation is derived that plays the role of the Ornstein-Zernike (OZ) equation
in the grand canonical ensemble (GCE). When applied to the ideal gas we obtain
the exact result for the total correlation function h_N. For a homogeneous
fluid with N particles the new equation only differs from OZ by 1/N and it
allows to obtain an approximate expression for h_N in terms of its GCE
counterpart that agrees with the expansion of h_N in powers of 1/N.Comment: 5 pages, RevTeX. Submitted to Phys. Rev. Let
Correlation function algebra for inhomogeneous fluids
We consider variational (density functional) models of fluids confined in
parallel-plate geometries (with walls situated in the planes z=0 and z=L
respectively) and focus on the structure of the pair correlation function
G(r_1,r_2). We show that for local variational models there exist two
non-trivial identities relating both the transverse Fourier transform G(z_\mu,
z_\nu;q) and the zeroth moment G_0(z_\mu,z_\nu) at different positions z_1, z_2
and z_3. These relations form an algebra which severely restricts the possible
form of the function G_0(z_\mu,z_\nu). For the common situations in which the
equilibrium one-body (magnetization/number density) profile m_0(z) exhibits an
odd or even reflection symmetry in the z=L/2 plane the algebra simplifies
considerably and is used to relate the correlation function to the finite-size
excess free-energy \gamma(L). We rederive non-trivial scaling expressions for
the finite-size contribution to the free-energy at bulk criticality and for
systems where large scale interfacial fluctuations are present. Extensions to
non-planar geometries are also considered.Comment: 15 pages, RevTex, 4 eps figures. To appear in J.Phys.Condens.Matte
Liquid drops on a surface: using density functional theory to calculate the binding potential and drop profiles and comparing with results from mesoscopic modelling
The contribution to the free energy for a film of liquid of thickness on
a solid surface, due to the interactions between the solid-liquid and
liquid-gas interfaces is given by the binding potential, . The precise
form of determines whether or not the liquid wets the surface. Note that
differentiating gives the Derjaguin or disjoining pressure. We develop a
microscopic density functional theory (DFT) based method for calculating
, allowing us to relate the form of to the nature of the molecular
interactions in the system. We present results based on using a simple lattice
gas model, to demonstrate the procedure. In order to describe the static and
dynamic behaviour of non-uniform liquid films and drops on surfaces, a
mesoscopic free energy based on is often used. We calculate such
equilibrium film height profiles and also directly calculate using DFT the
corresponding density profiles for liquid drops on surfaces. Comparing
quantities such as the contact angle and also the shape of the drops, we find
good agreement between the two methods. We also study in detail the effect on
of truncating the range of the dispersion forces, both those between the
fluid molecules and those between the fluid and wall. We find that truncating
can have a significant effect on and the associated wetting behaviour of
the fluid.Comment: 16 pages, 13 fig
Equivalence of two approaches for the inhomogeneous density in the canonical ensemble
In this article we show that the inhomogeneous density obtained from a
density-functional theory of classical fluids in the canonical ensemble (CE),
recently presented by White et al [Phys. Rev. Lett. 84 (2000) 1220], is
equivalent to first order to the result of the series expansion of the CE
inhomogeneous density introduced by Gonzalez et al [Phys. Rev. Lett. 79 (1997)
2466].Comment: 6 pages, RevTe
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