1,796 research outputs found
Dynamical density functional theory: phase separation in a cavity and the influence of symmetry
Consider a fluid composed of two species of particles, where the
interparticle pair potentials . On confining an
equal number of particles from each species in a cavity, one finds that the
average one body density profiles of each species are constrained to be exactly
the same due to the symmetry, when both external cavity potentials are the
same. For a binary fluid of Brownian particles interacting via repulsive
Gaussian pair potentials that exhibits phase separation, we study the dynamics
of the fluid one body density profiles on breaking the symmetry of the external
potentials, using the dynamical density functional theory of Marconi and
Tarazona [{\it J. Chem. Phys.}, {\bf 110}, 8032 (1999)]. On breaking the
symmetry we see that the fluid one body density profiles can then show the
phase separation that is present.Comment: 7 pages, 4 figures. Accepted for the proceedings of the Liquid Matter
conference 2005, to be publication in J. Phys.: Condens. Matte
Solidification in soft-core fluids: disordered solids from fast solidification fronts
Using dynamical density functional theory we calculate the speed of
solidification fronts advancing into a quenched two-dimensional model fluid of
soft-core particles. We find that solidification fronts can advance via two
different mechanisms, depending on the depth of the quench. For shallow
quenches, the front propagation is via a nonlinear mechanism. For deep
quenches, front propagation is governed by a linear mechanism and in this
regime we are able to determine the front speed via a marginal stability
analysis. We find that the density modulations generated behind the advancing
front have a characteristic scale that differs from the wavelength of the
density modulation in thermodynamic equilibrium, i.e., the spacing between the
crystal planes in an equilibrium crystal. This leads to the subsequent
development of disorder in the solids that are formed. For the one-component
fluid, the particles are able to rearrange to form a well-ordered crystal, with
few defects. However, solidification fronts in a binary mixture exhibiting
crystalline phases with square and hexagonal ordering generate solids that are
unable to rearrange after the passage of the solidification front and a
significant amount of disorder remains in the system.Comment: 18 pages, 14 fig
Modelling the evaporation of thin films of colloidal suspensions using Dynamical Density Functional Theory
Recent experiments have shown that various structures may be formed during
the evaporative dewetting of thin films of colloidal suspensions. Nano-particle
deposits of strongly branched `flower-like', labyrinthine and network
structures are observed. They are caused by the different transport processes
and the rich phase behaviour of the system. We develop a model for the system,
based on a dynamical density functional theory, which reproduces these
structures. The model is employed to determine the influences of the solvent
evaporation and of the diffusion of the colloidal particles and of the liquid
over the surface. Finally, we investigate the conditions needed for
`liquid-particle' phase separation to occur and discuss its effect on the
self-organised nano-structures
Mean-field dynamical density functional theory
We examine the out-of-equilibrium dynamical evolution of density profiles of
ultrasoft particles under time-varying external confining potentials in three
spatial dimensions. The theoretical formalism employed is the dynamical density
functional theory (DDFT) of Marini Bettolo Marconi and Tarazona [J. Chem. Phys.
{\bf 110}, 8032 (1999)], supplied by an equilibrium excess free energy
functional that is essentially exact. We complement our theoretical analysis by
carrying out extensive Brownian Dynamics simulations. We find excellent
agreement between theory and simulations for the whole time evolution of
density profiles, demonstrating thereby the validity of the DDFT when an
accurate equilibrium free energy functional is employed.Comment: 8 pagers, 4 figure
Modelling the evaporation of nanoparticle suspensions from heterogeneous surfaces
We present a Monte Carlo (MC) grid-based model for the drying of drops of a
nanoparticle suspension upon a heterogeneous surface. The model consists of a
generalised lattice-gas in which the interaction parameters in the Hamiltonian
can be varied to model different properties of the materials involved. We show
how to choose correctly the interactions, to minimise the effects of the
underlying grid so that hemispherical droplets form. We also include the
effects of surface roughness to examine the effects of contact-line pinning on
the dynamics. When there is a `lid' above the system, which prevents
evaporation, equilibrium drops form on the surface, which we use to determine
the contact angle and how it varies as the parameters of the model are changed.
This enables us to relate the interaction parameters to the materials used in
applications. The model has also been applied to drying on heterogeneous
surfaces, in particular to the case where the suspension is deposited on a
surface consisting of a pair of hydrophilic conducting metal surfaces that are
either side of a band of hydrophobic insulating polymer. This situation occurs
when using inkjet printing to manufacture electrical connections between the
metallic parts of the surface. The process is not always without problems,
since the liquid can dewet from the hydrophobic part of the surface, breaking
the bridge before the drying process is complete. The MC model reproduces the
observed dewetting, allowing the parameters to be varied so that the conditions
for the best connection can be established. We show that if the hydrophobic
portion of the surface is located at a step below the height of the
neighbouring metal, the chance of dewetting of the liquid during the drying
process is significantly reduced.Comment: 14 pages, 14 figure
Dynamical density functional theory for the dewetting of evaporating thin films of nanoparticle suspensions exhibiting pattern formation
Recent experiments have shown that the striking structure formation in
dewetting films of evaporating colloidal nanoparticle suspensions occurs in an
ultrathin `postcursor' layer that is left behind by a mesoscopic dewetting
front. Various phase change and transport processes occur in the postcursor
layer, that may lead to nanoparticle deposits in the form of labyrinthine,
network or strongly branched `finger' structures. We develop a versatile
dynamical density functional theory to model this system which captures all
these structures and may be employed to investigate the influence of
evaporation/condensation, nanoparticle transport and solute transport in a
differentiated way. We highlight, in particular, the influence of the subtle
interplay of decomposition in the layer and contact line motion on the observed
particle-induced transverse instability of the dewetting front.Comment: 5 pages, 5 figure
Criticality and phase separation in a two-dimensional binary colloidal fluid induced by the solvent critical behavior
We present an experimental and theoretical study of the phase behavior of a
binary mixture of colloids with opposite adsorption preferences in a critical
solvent. As a result of the attractive and repulsive critical Casimir forces,
the critical fluctuations of the solvent lead to a further critical point in
the colloidal system, i.e. to a critical colloidal-liquid--colloidal-liquid
demixing phase transition which is controlled by the solvent temperature. Our
experimental findings are in good agreement with calculations based on a simple
approximation for the free energy of the system.Comment: 5 pages, 5 figures, to be published in Europhysics Letter
Dynamics in inhomogeneous liquids and glasses via the test particle limit
We show that one may view the self and the distinct part of the van Hove
dynamic correlation function of a simple fluid as the one-body density
distributions of a binary mixture that evolve in time according to dynamical
density functional theory. For a test case of soft core Brownian particles the
theory yields results for the van Hove function that agree quantitatively with
those of our Brownian dynamics computer simulations. At sufficiently high
densities the free energy landscape underlying the dynamics exhibits a barrier
as a function of the mean particle displacement, shedding new light on the
nature of glass formation. For hard spheres confined between parallel planar
walls the barrier height oscillates in-phase with the local density, implying
that the mobility is maximal between layers, which should be experimentally
observable in confined colloidal dispersions.Comment: 4 pages, 3 figure
Dynamic density functional study of a driven colloidal particle in polymer solutions
The Dynamic Density Functional (DDF) theory and standard Brownian dynamics
simulations (BDS) are used to study the drifting effects of a colloidal
particle in a polymer solution, both for ideal and interacting polymers. The
structure of the stationary density distributions and the total induced current
are analyzed for different drifting rates. We find good agreement with the BDS,
which gives support to the assumptions of the DDF theory. The qualitative
aspect of the density distribution are discussed and compared to recent results
for driven colloids in one-dimensional channels and to analytical expansions
for the ideal solution limit
Dynamical density functional theory for dense atomic liquids
Starting from Newton's equations of motion, we derive a dynamical density
functional theory (DDFT) applicable to atomic liquids. The theory has the
feature that it requires as input the Helmholtz free energy functional from
equilibrium density functional theory. This means that, given a reliable
equilibrium free energy functional, the correct equilibrium fluid density
profile is guaranteed. We show that when the isothermal compressibility is
small, the DDFT generates the correct value for the speed of sound in a dense
liquid. We also interpret the theory as a dynamical equation for a coarse
grained fluid density and show that the theory can be used (making further
approximations) to derive the standard mode coupling theory that is used to
describe the glass transition. The present theory should provide a useful
starting point for describing the dynamics of inhomogeneous atomic fluids.Comment: 14 pages, accepted for publication in J. Phys.: Condens. Matte
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