arXiv subjects

Matthias Schmidt

Publications and source records attributed to Matthias Schmidt.

At least 109 records · Page 6Linked to original sources

arXiv2011

First-order layering and critical wetting transitions in non-additive hard sphere mixtures

Using fundamental-measure density functional theory we investigate entropic wetting in an asymmetric binary mixture of hard spheres with positive non-additivity. We consider a general planar hard wall, where preferential adsorption is induced by a difference in closest approach of the different species and the wall. Close to bulk fluid-fluid coexistence the phase rich in the minority component adsorbs either through a series of first-order layering transitions, where an increasing number of liquid layers adsorbs sequentially, or via a critical wetting transition, where a thick film grows continuously.

cond-mat.soft↗

arXiv2011

Variational Principle of Classical Density Functional Theory via Levy's Constrained Search Method

We show that classical density functional theory can be based on the constrained search method [M. Levy, Proc. Natl. Acad. Sci. 76, 6062 (1979)]. From the Gibbs inequality one first derives a variational principle for the grand potential as a functional of a trial many-body distribution. This functional is minimized in two stages. The first step consists of a constrained search of all many-body distributions that generate a given one-body density. The result can be split into internal and external contributions to the total grand potential. In contrast to the original approach by Mermin and Evans, here the intrinsic Helmholtz free energy functional is defined by an explicit expression that does not refer to an external potential in order to generate the given one-body density. The second step consists of minimizing with respect to the one-body density. We show that this framework can be applied in a straightforward way to the canonical ensemble.

cond-mat.stat-mech↗

arXiv2011

Phase behaviour of binary mixtures of diamagnetic colloidal platelets in an external magnetic field

Using fundamental measure density functional theory we investigate paranematic-nematic and nematic-nematic phase coexistence in binary mixtures of circular platelets with vanishing thicknesses. An external magnetic field induces uniaxial alignment and acts on the platelets with a strength that is taken to scale with the platelet area. At particle diameter ratio lambda=1.5 the system displays paranematic-nematic coexistence. For lambda=2, demixing into two nematic states with different compositions also occurs, between an upper critical point and a paranematic-nematic-nematic triple point. Increasing the field strength leads to shrinking of the coexistence regions. At high enough field strength a closed loop of immiscibility is induced and phase coexistence vanishes at a double critical point above which the system is homogeneously nematic. For lambda=2.5, besides paranematic-nematic coexistence, there is nematic-nematic coexistence which persists and hence does not end in a critical point. The partial orientational order parameters along the binodals vary strongly with composition and connect smoothly for each species when closed loops of immiscibility are present in the corresponding phase diagram.

cond-mat.soft↗

arXiv2011

Computer simulations of colloidal transport on a patterned magnetic substrate

We study the transport of paramagnetic colloidal particles on a patterned magnetic substrate with kinetic Monte Carlo and Brownian dynamics computer simulations. The planar substrate is decorated with point dipoles in either parallel or zigzag stripe arrangements and exposed to an additional external magnetic field that oscillates in time. For the case of parallel stripes we find that the magnitude and direction of the particle current is controlled by the tilt angle of the external magnetic field. The effect is reliably obtained in a wide range of ratios between temperature and magnetic permeability. Particle transport is achieved only when the period of oscillation of the external field is greater than a critical value. For the case of zigzag stripes a current is obtained using an oscillating external field normal to the substrate. In this case, transport is only possible in the vertex of the zigzag, giving rise to a narrow stream of particles. The magnitude and direction of the particle current are found to be controlled by a combination of the zigzag angle and the distance of the colloids from the substrate. Metropolis Monte Carlo and Brownian dynamics simulations predict results that are in good agreement with each other. Using kinetic Monte Carlo we find that at high density the particle transport is hindered by jamming.

cond-mat.soft↗

arXiv2011

Isometric and metamorphic operations on the space of local fundamental measures

We consider symmetry operations on the four-dimensional vector space that is spanned by the local versions of the Minkowski functionals (or fundamental measures): volume, surface, integral mean curvature, and Euler characteristic, of an underlying three-dimensional geometry. A bilinear combination of the measures is used as a (pseudo) metric with ++-- signature, represented by a 4x4 matrix with unit entries on the counter diagonal. Six different types of linear automorphisms are shown to leave the metric invariant. Their generators form a Lie algebra that can be grouped into two mutually commuting triples with non-trivial structure constants. We supplement these six isometric operations by further ten transformations that have a metamorphic (altering) effect on the underlying geometry. When grouped together, four different linear combinations of the metamorphic generators form a previously obtained third-rank tensor. This is shown to describe four different types of mutually commuting "shifting" operations in fundamental measure space. The relevance for fundamental measures density functional theory is discussed briefly.

math-ph↗

arXiv2011

Density functional for hard hyperspheres from a tensorial-diagrammatic series

We represent the free energy functional by a diagrammatic series with tensorial coefficients indexed by powers of length scale. For hard cores, we obtain Percus' exact functional in one dimension and the Kierlik-Rosinberg form of fundamental measures theory in three dimensions. In five dimensions, the functional describes bulk fluids better than Percus-Yevick theory does. At planar walls density profiles oscillate with smaller periods than in lower dimensions. Our findings open up avenues for treating both more general high-dimensional systems, as well as three-dimensional mixtures via dimensional reduction.

cond-mat.soft↗

arXiv2010

The van Hove distribution function for Brownian hard spheres: dynamical test particle theory and computer simulations for bulk dynamics

We describe a test particle approach based on dynamical density functional theory (DDFT) for studying the correlated time evolution of the particles that constitute a fluid. Our theory provides a means of calculating the van Hove distribution function by treating its self and distinct parts as the two components of a binary fluid mixture, with the `self' component having only one particle, the `distinct' component consisting of all the other particles, and using DDFT to calculate the time evolution of the density profiles for the two components. We apply this approach to a bulk fluid of Brownian hard spheres and compare to results for the van Hove function and the intermediate scattering function from Brownian dynamics computer simulations. We find good agreement at low and intermediate densities using the very simple Ramakrishnan-Yussouff [Phys. Rev. B 19, 2775 (1979)] approximation for the excess free energy functional. Since the DDFT is based on the equilibrium Helmholtz free energy functional, we can probe a free energy landscape that underlies the dynamics. Within the mean-field approximation we find that as the particle density increases, this landscape develops a minimum, while an exact treatment of a model confined situation shows that for an ergodic fluid this landscape should be monotonic. We discuss possible implications for slow, glassy and arrested dynamics at high densities.

cond-mat.soft↗

arXiv2010

Binary non-additive hard sphere mixtures: Fluid demixing, asymptotic decay of correlations and free fluid interfaces

Using a fundamental measure density functional theory we investigate both bulk and inhomogeneous systems of the binary non-additive hard sphere model. For sufficiently large (positive) non-additivity the mixture phase separates into two fluid phases with different compositions. We calculate bulk fluid-fluid coexistence curves for a range of size ratios and non-additivity parameters and find that they compare well to simulation results from the literature. Using the Ornstein-Zernike equation, we investigate the asymptotic, r->infinity, decay of the partial pair correlation functions, g_ij(r). At low densities there occurs a structural crossover in the asymptotic decay between two different damped oscillatory modes with different wavelengths corresponding to the two intra-species hard core diameters. On approaching the fluid-fluid critical point there is Fisher-Widom crossover from exponentially damped oscillatory to monotonic asymptotic decay. Using the density functional we calculate the density profiles for the planar free fluid-fluid interface between coexisting fluid phases. We show that the type of asymptotic decay of g_ij(r) not only determines the asymptotic decay of the interface profiles, but is also relevant for intermediate and even short-ranged behaviour. We also determine the surface tension of the free fluid interface, finding that it increases with non-additivity, and that on approaching the critical point mean-field scaling holds.

cond-mat.soft↗

arXiv2010

Laterally driven interfaces in the three-dimensional Ising lattice gas

We study the steady state of a phase-separated driven Ising lattice gas in three dimensions using computer simulations with Kawasaki dynamics. An external force field F(z) acts in the x direction parallel to the interface, creating a lateral order parameter current j^x(z) which varies with distance z from the interface. Above the roughening temperature, our data for `shear-like' linear variation of F(z) are in agreement with the picture wherein shear acts as effective confinement in this system, thus supressing the interfacial capillary-wave fluctuations. We find sharper magnetisation profiles and reduced interfacial width as compared to equilibrium. Pair correlations are more suppressed in the vorticity direction y than in the driving direction; the opposite holds for the structure factor. Lateral transport of capillary waves occurs for those forms of F(z) for which the current j^x(z) is an odd function of z, for example the shear-like drive, and a `step-like' driving field. For a V-shaped driving force no such motion occurs, but capillary waves are suppressed more strongly than for the shear-like drive. These findings are in agreement with our previous simulation studies in two dimensions. Near and below the (equilibrium) roughening temperature the effective-confinement picture ceases to work, but the lateral motion of the interface persists.

cond-mat.stat-mech↗

arXiv2010

Bulk phase behaviour of binary hard platelet mixtures from density functional theory

We investigate isotropic-isotropic, isotropic-nematic and nematic-nematic phase coexistence in binary mixtures of circular platelets with vanishing thickness, continuous rotational degrees of freedom and radial size ratios $λ$ up to 5. A fundamental measure density functional theory, previously used for the one-component model, is proposed and results are compared against those from Onsager theory as a benchmark. For $λ\leq 1.7$ the system displays isotropic-nematic phase coexistence with a widening of the biphasic region for increasing values of $λ$. For size ratios $λ\geq 2$, we find demixing into two nematic states becomes stable and an isotropic-nematic-nematic triple point can occur. Fundamental measure theory gives a smaller isotropic-nematic biphasic region than Onsager theory and locates the transition at lower densities. Furthermore, nematic-nematic demixing occurs over a larger range of compositions at a given value of $λ$ than found in Onsager theory. Both theories predict the same topologies of the phase diagrams. The partial nematic order parameters vary strongly with composition and indicate that the larger particles are more strongly ordered than the smaller particles.

cond-mat.soft↗

arXiv2009

Lateral transport of thermal capillary waves

We demonstrate that collective motion of interfacial fluctuations can occur at the interface between two coexisting thermodynamic phases. Based on computer simulation results for driven diffusive Ising and Blume-Capel models, we conjecture that the thermal capillary waves at a planar interface travel along the interface if the lateral order parameter current j_op(y) is an odd function of the distance y from the interface and hence possesses opposite directions in the two phases. Such motion does not occur if j_op(y) is an even function of y. A discrete Gaussian interface model with effective dynamics exhibits similiar transport phenomena but with a simpler dispersion relation. These findings open up avenues for controlled interfacial transport on the nanoscale.

cond-mat.stat-mech↗

arXiv2008

Gauge Orbit Types for Theories with Classical Compact Gauge Group

We determine the orbit types of the action of the group of local gauge transformations on the space of connections in a principal bundle with structure group O(n), SO(n) or $Sp(n)$ over a closed, simply connected manifold of dimension 4. Complemented with earlier results on U(n) and SU(n) this completes the classification of the orbit types for all classical compact gauge groups over such space-time manifolds. On the way we derive the classification of principal bundles with structure group SO(n) over these manifolds and the Howe subgroups of SO(n).

hep-th↗

arXiv2008

On the algebra of quantum observables for a certain gauge model

We prove that the algebra of observables of a certain gauge model is generated by unbounded elements in the sense of Woronowicz. The generators are constructed from the classical generators of invariant polynomials by means of geometric quantization.

hep-th↗

arXiv2008

Interfaces in driven Ising models: shear enhances confinement

We use a phase-separated driven two-dimensional Ising lattice gas to study fluid interfaces exposed to shear flow parallel to the interface. The interface is stabilized by two parallel walls with opposing surface fields and a driving field parallel to the walls is applied which (i) either acts locally at the walls or (ii) varies linearly with distance across the strip. Using computer simulations with Kawasaki dynamics, we find that the system reaches a steady state in which the magnetisation profile is the same as that in equilibrium, but with a rescaled length implying a reduction of the interfacial width. An analogous effect was recently observed in sheared phase-separated colloidal dispersions. Pair correlation functions along the interface decay more rapidly with distance under drive than in equilibrium and for cases of weak drive can be rescaled to the equilibrium result.

cond-mat.stat-mech↗

arXiv2007

Non-equilibrium sedimentation of colloids on the particle scale

We investigate sedimentation of model hard sphere-like colloidal dispersions confined in horizontal capillaries using laser scanning confocal microscopy, dynamical density functional theory, and Brownian dynamics computer simulations. For homogenized initial states we obtain quantitative agreement of the results from the respective approaches for the time evolution of the one-body density distribution and the osmotic pressure on the walls. We demonstrate that single particle information can be obtained experimentally in systems that were initialized further out-of-equilibrium such that complex lateral patterns form.

cond-mat.soft↗

arXiv2006

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.

cond-mat.soft↗

arXiv2006

Phase behavior and structure of model colloid-polymer mixtures confined between two parallel planar walls

Using Gibbs ensemble Monte Carlo simulations and density functional theory we investigate the fluid-fluid demixing transition in inhomogeneous colloid-polymer mixtures confined between two parallel plates with separation distances between one and ten colloid diameters covering the complete range from quasi two-dimensional to bulk-like behavior. We use the Asakura-Oosawa-Vrij model in which colloid-colloid and colloid-polymer interactions are hard-sphere like, whilst the pair potential between polymers vanishes. Two different types of confinement induced by a pair of parallel walls are considered, namely either through two hard walls or through two semi-permeable walls that repel colloids but allow polymers to freely penetrate. For hard (semi-permeable) walls we find that the capillary binodal is shifted towards higher (lower) polymer fugacities and lower (higher) colloid fugacities as compared to the bulk binodal; this implies capillary condensation (evaporation) of the colloidal liquid phase in the slit. A macroscopic treatment is provided by a novel symmetric Kelvin equation for general binary mixtures, based on the proximity in chemical potentials of statepoints at capillary coexistence and the reference bulk coexistence. Results for capillary binodals compare well with those obtained from the classic version of the Kelvin equation due to Evans and Marini Bettolo Marconi [J. Chem. Phys. 86, 7138 (1987)], and are quantitatively accurate away from the fluid-fluid critical point, even at small wall separations. For hard walls the density profiles of polymers and colloids inside the slit display oscillations due to packing effects for all statepoints. For semi-permeable walls either similar structuring or flat profiles are found, depending on the statepoint considered.

cond-mat.soft↗

arXiv2005

Density functional theory for colloidal mixtures of hard platelets, rods, and spheres

A geometry-based density functional theory is presented for mixtures of hard spheres, hard needles and hard platelets; both the needles and the platelets are taken to be of vanishing thickness. Geometrical weight functions that are characteristic for each species are given and it is shown how convolutions of pairs of weight functions recover each Mayer bond of the ternary mixture and hence ensure the correct second virial expansion of the excess free energy functional. The case of sphere-platelet overlap relies on the same approximation as does Rosenfeld's functional for strictly two-dimensional hard disks. We explicitly control contributions to the excess free energy that are of third order in density. Analytic expressions relevant for the application of the theory to states with planar translational and cylindrical rotational symmetry, e.g. to describe behavior at planar smooth walls, are given. For binary sphere-platelet mixtures, in the appropriate limit of small platelet densities, the theory differs from that used in a recent treatment [L. Harnau and S. Dietrich, Phys. Rev. E 71, 011504 (2004)]. As a test case of our approach we consider the isotropic-nematic bulk transition of pure hard platelets, which we find to be weakly first order, with values for the coexistence densities and the nematic order parameter that compare well with simulation results.

cond-mat.soft↗