567 research outputs found
The fluid-fluid interface in a model colloid-polymer mixture: Application of grand canonical Monte Carlo to asymmetric binary mixtures
We present a Monte Carlo method to simulate asymmetric binary mixtures in the
grand canonical ensemble. The method is used to study the colloid-polymer model
of Asakura and Oosawa. We determine the phase diagram of the fluid-fluid
unmixing transition and the interfacial tension, both at high polymer density
and close to the critical point. We also present density profiles in the
two-phase region. The results are compared to predictions of a recent density
functional theory.Comment: 4 pages, 4 figure
Electrophoretic Properties of Highly Charged Colloids: A Hybrid MD/LB Simulation Study
Using computer simulations, the electrophoretic motion of a positively
charged colloid (macroion) in an electrolyte solution is studied in the
framework of the primitive model. Hydrodynamic interactions are fully taken
into account by applying a hybrid simulation scheme, where the charged ions
(i.e. macroion and electrolyte), propagated via molecular dynamics (MD), are
coupled to a Lattice Boltzmann (LB) fluid. In a recent experiment it was shown
that, for multivalent salt ions, the mobility initially increases with
charge density , reaches a maximum and then decreases with further
increase of . The aim of the present work is to elucidate the behaviour
of at high values of . Even for the case of monovalent microions,
we find a decrease of with . A dynamic Stern layer is defined
that includes all the counterions that move with the macroion while subject to
an external electrical field. The number of counterions in the Stern layer,
, is a crucial parameter for the behavior of at high values of
. In this case, the mobility depends primarily on the ratio
(with the valency of the macroion). The previous contention that
the increase in the distortion of the electric double layer (EDL) with
increasing leads to the lowering of does not hold for high
. In fact, we show that the deformation of the EDL decreases with
increase of . The role of hydrodynamic interactions is inferred from
direct comparisons to Langevin simulations where the coupling to the LB fluid
is switched off. Moreover, systems with divalent counterions are considered. In
this case, at high values of the phenomenon of charge inversion is
found.Comment: accepted in J. Chem Phys., 10 pages, 9 figure
Tension and stiffness of the hard sphere crystal-fluid interface
A combination of fundamental measure density functional theory and Monte
Carlo computer simulation is used to determine the orientation-resolved
interfacial tension and stiffness for the equilibrium hard-sphere crystal-fluid
interface. Microscopic density functional theory is in quantitative agreement
with simulations and predicts a tension of 0.66 kT/\sigma^2 with a small
anisotropy of about 0.025 kT and stiffnesses with e.g. 0.53 kT/\sigma^2 for the
(001) orientation and 1.03 kT/\sigma^2 for the (111) orientation. Here kT is
denoting the thermal energy and \sigma the hard sphere diameter. We compare our
results with existing experimental findings
Frequency dependent specific heat of viscous silica
We apply the Mori-Zwanzig projection operator formalism to obtain an
expression for the frequency dependent specific heat c(z) of a liquid. By using
an exact transformation formula due to Lebowitz et al., we derive a relation
between c(z) and K(t), the autocorrelation function of temperature fluctuations
in the microcanonical ensemble. This connection thus allows to determine c(z)
from computer simulations in equilibrium, i.e. without an external
perturbation. By considering the generalization of K(t) to finite wave-vectors,
we derive an expression to determine the thermal conductivity \lambda from such
simulations. We present the results of extensive computer simulations in which
we use the derived relations to determine c(z) over eight decades in frequency,
as well as \lambda. The system investigated is a simple but realistic model for
amorphous silica. We find that at high frequencies the real part of c(z) has
the value of an ideal gas. c'(\omega) increases quickly at those frequencies
which correspond to the vibrational excitations of the system. At low
temperatures c'(\omega) shows a second step. The frequency at which this step
is observed is comparable to the one at which the \alpha-relaxation peak is
observed in the intermediate scattering function. Also the temperature
dependence of the location of this second step is the same as the one of the
peak, thus showing that these quantities are intimately connected to
each other. From c'(\omega) we estimate the temperature dependence of the
vibrational and configurational part of the specific heat. We find that the
static value of c(z) as well as \lambda are in good agreement with experimental
data.Comment: 27 pages of Latex, 8 figure
Non-exponential kinetic behavior of confined water
We present the results of molecular dynamics simulations of SPC/E water
confined in a realistic model of a silica pore. The single-particle dynamics
have been studied at ambient temperature for different hydration levels. The
confinement near the hydrophilic surface makes the dynamic behaviour of the
liquid strongly dependent on the hydration level. Upon decrease of the number
of water molecules in the pore we observe the onset of a slow dynamics due to
the ``cage effect''. The conventional picture of a stochastic single-particle
diffusion process thus looses its validity
Capillary Waves in a Colloid-Polymer Interface
The structure and the statistical fluctuations of interfaces between
coexisting phases in the Asakura-Oosawa (AO) model for a colloid--polymer
mixture are analyzed by extensive Monte Carlo simulations. We make use of a
recently developed grand canonical cluster move with an additional constraint
stabilizing the existence of two interfaces in the (rectangular) box that is
simulated. Choosing very large systems, of size LxLxD with L=60 and D=120,
measured in units of the colloid radius, the spectrum of capillary wave-type
interfacial excitations is analyzed in detail. The local position of the
interface is defined in terms of a (local) Gibbs surface concept. For small
wavevectors capillary wave theory is verified quantitatively, while for larger
wavevectors pronounced deviations show up. For wavevectors that correspond to
the typical distance between colloids in the colloid-rich phase, the
interfacial fluctuations exhibit the same structure as observed in the bulk
structure factor. When one analyzes the data in terms of the concept of a
wavevector-dependent interfacial tension, a monotonous decrease of this
quantity with increasing wavevector is found. Limitations of our analysis are
critically discussed.Comment: 12 pages, 15 figure
Water adsorption on amorphous silica surfaces: A Car-Parrinello simulation study
A combination of classical molecular dynamics (MD) and ab initio
Car-Parrinello molecular dynamics (CPMD) simulations is used to investigate the
adsorption of water on a free amorphous silica surface. From the classical MD
SiO_2 configurations with a free surface are generated which are then used as
starting configurations for the CPMD.We study the reaction of a water molecule
with a two-membered ring at the temperature T=300K. We show that the result of
this reaction is the formation of two silanol groups on the surface. The
activation energy of the reaction is estimated and it is shown that the
reaction is exothermic.Comment: 12 pages, 6 figures, to be published in J. Phys.: Condens. Matte
Critical phenomena in colloid-polymer mixtures: interfacial tension, order parameter, susceptibility and coexistence diameter
The critical behavior of a model colloid-polymer mixture, the so-called AO
model, is studied using computer simulations and finite size scaling
techniques. Investigated are the interfacial tension, the order parameter, the
susceptibility and the coexistence diameter. Our results clearly show that the
interfacial tension vanishes at the critical point with exponent 2\nu ~ 1.26.
This is in good agreement with the 3D Ising exponent. Also calculated are
critical amplitude ratios, which are shown to be compatible with the
corresponding 3D Ising values. We additionally identify a number of subtleties
that are encountered when finite size scaling is applied to the AO model. In
particular, we find that the finite size extrapolation of the interfacial
tension is most consistent when logarithmic size dependences are ignored. This
finding is in agreement with the work of Berg et al.[Phys. Rev. B, V47 P497
(1993)]Comment: 13 pages, 16 figure
Computer Simulations of Supercooled Liquids and Glasses
After a brief introduction to the dynamics of supercooled liquids, we discuss
some of the advantages and drawbacks of computer simulations of such systems.
Subsequently we present the results of computer simulations in which the
dynamics of a fragile glass former, a binary Lennard-Jones system, is compared
to the one of a strong glass former, SiO_2. This comparison gives evidence that
the reason for the different temperature dependence of these two types of glass
formers lies in the transport mechanism for the particles in the vicinity of
T_c, the critical temperature of mode-coupling theory. Whereas the one of the
fragile glass former is described very well by the ideal version of
mode-coupling theory, the one for the strong glass former is dominated by
activated processes. In the last part of the article we review some simulations
of glass formers in which the dynamics below the glass transition temperature
was investigated. We show that such simulations might help to establish a
connection between systems with self generated disorder (e.g. structural
glasses) and quenched disorder (e.g. spin glasses).Comment: 37 pages of Latex, 11 figures, to appear as a Topical Review article
in J. Phys.: Condens. Matte
- …