Biomedical subjects

H Löwen

Publications and source records attributed to H Löwen.

At least 19 recordsLinked to original sources

PubMed2006

Rhythmic cluster generation in strongly driven colloidal dispersions.

We study the response of a nematic colloidal dispersion of rods to a driven probe particle which is dragged with high speed through the dispersion perpendicular to the nematic director. In front of the dragged particle, clusters of rods are generated which rhythmically grow and dissolve by rotational motion. We find evidence for a mesoscopic cluster-cluster correlation length, independent of the imposed drag speed. Our results are based on nonequilibrium Brownian dynamics computer simulations and in line with a dynamical scaling theory.

Cluster Analysis↗

PubMed2005

Tailoring the flow of soft glasses by soft additives.

We examine the vitrification and melting of asymmetric star polymer mixtures by combining rheological measurements with mode coupling theory. We identify two types of glassy states, a single glass, in which the small component is fluid in the glassy matrix of the big one, and a double glass, in which both components are vitrified. Addition of small-star polymers leads to melting of both glasses, and the melting curve has a nonmonotonic dependence on the star-star size ratio. The phenomenon opens new ways for externally steering the rheological behavior of soft matter systems.

Computer Simulation↗

PubMed2005

Soft colloids driven and sheared by traveling wave fields.

We study the dynamics of soft colloids interacting via a Gaussian pair potential in an external moving potential which is periodic in the spatial coordinate of the direction of motion. Both dynamical density functional theory and Brownian dynamics computer simulations are used to predict the steady-state density profiles. Two different situations are investigated: the first corresponds to a light wave that travels with a constant velocity v through the quiescent solvent containing the colloidal suspension. The second setup consists of two parallel repulsive walls with a periodic topographical substructure. One of the walls is at rest relative to the solvent while the other is in motion, inducing a shearing of the suspension. In the first case, we find that the amplitude of the steady-state density behaves nonmonotonically with the traveling speed v of the wave if the shape of the wave contains an edge: for increasing v , it first grows and then decreases. In the second setup we show that a strongly confined suspension induces a shear resistance which is a nonmonotonic function of the wall velocity. These effects are verifiable in real-space experiments on colloidal suspensions exposed to external laser-optical fields. In both situations, the dynamical density functional theory is in good agreement with the Brownian dynamics simulation data.

Journal Article↗

PubMed2005

Anisotropic mean-square displacements in two-dimensional colloidal crystals of tilted dipoles.

Superparamagnetic colloidal particles confined to a flat horizontal air-water interface in an external magnetic field, which is tilted relative to the interface, form anisotropic two-dimensional crystals resulting from their mutual dipole-dipole interactions. Using real-space experiments and harmonic lattice theory we explore the mean-square displacements of the particles in the directions parallel and perpendicular to the in-plane component of the external magnetic field as a function of the tilt angle. We find that the anisotropy of the mean-square displacement behaves nonmonotonically as a function of the tilt angle and does not correlate with the structural anisotropy of the crystal.

Journal Article↗

PubMed2005

Ionic microgels as model systems for colloids with an ultrasoft electrosteric repulsion: structure and thermodynamics.

We present a theoretical analysis of the structural properties and phase behavior of spherical, loosely cross-linked ionic microgels that possess a low monomer concentration. The analysis is based on the recently derived effective interaction potential between such particles [A. R. Denton, Phys. Rev. E 67, 011804 (2003)]. By employing standard tools from the theory of the liquid state, we quantitatively analyze the pair correlations in the fluid and find anomalous behavior above the overlap concentration, similar to the cases of star-branched neutral and charged polymers. We also employ an evolutionary algorithm in order to predict the crystalline phases of the system without any a priori assumptions regarding their symmetry class. A very rich phase diagram is obtained, featuring two reentrant melting transitions and a number of unusual crystal structures. At high densities, both the Hansen-Verlet freezing criterion [J.-P. Hansen and L. Verlet, Phys. Rev. 184, 151 (1969)] and the Lindemann melting criterion [F. A. Lindemann, Phys. Z. 11, 609 (1910)] lose their validity. The topology of the phase diagram is altered when the steric interactions between the polymer segments become strong enough, in which case the lower-density reentrant melting disappears and the region of stability of the fluid is split into two disconnected domains, separated by intervening fcc and bcc regions.

Journal Article↗

PubMed2005

Polyelectrolyte-surfactant complex: phases of self-assembled structures.

We study the structure of complexes formed between ionic surfactants (SF) and a single oppositely charged polyelectrolyte (PE) chain. For our computer simulation we use the "primitive" electrolyte model: while the polyelectrolyte is modeled by a tethered chain of charged hard sphere beads, the surfactant molecules consist of a single charged head bead tethered to a tail of tethered hard spheres. A hydrophobic attraction between the tail beads is introduced by assuming a Lennard-Jones potential outside the hard-sphere diameter. As a function of the strengths of both the electrostatic and the hydrophobic interactions, we find the following scenario: switching on and increasing the electrostatic forces first leads to a stretching of the PE and then by condensation of SF to the formation of a complex. For vanishing hydrophobic forces this complex has the architecture of a molecular bottle-brush cylindrically centered around the stretched PE molecule. Upon increasing the hydrophobic attraction between the SF tails, a transition occurs inverting this structure to a spherical micelle with a neutral core of SF tails and a charged corona of SF heads with the PE molecule wrapped around. At intermediate hydrophobicity there is a competition between the two structures indicated by a non-monotonic dependence of the shape as function of the Coulomb strength, favoring the cylindrical shape for weak and the spherical micellar complex for strong interaction.

Journal Article↗

PubMed2004

Soft effective interactions between weakly charged polyelectrolyte chains.

We apply extensive molecular dynamics simulations and analytical considerations in order to study the conformations and the effective interactions between weakly charged, flexible polyelectrolyte chains in salt-free conditions. We focus on charging fractions lying below 20%, for which case there is no Manning condensation of counterions and the latter can be thus partitioned in two states: those that are trapped within the region of the flexible chain and the ones that are free in the solution. We examine the partition of counterions in these two states, the chain sizes and the monomer distributions for various chain lengths, finding that the monomer density follows a Gaussian shape. We calculate the effective interaction between the centers of mass of two interacting chains, under the assumption that the chains can be modeled as two overlapping Gaussian charge profiles. The analytical calculations are compared with measurements from molecular dynamics simulations. Good quantitative agreement is found for charging fractions below 10%, where the chains assume coil-like configurations, whereas deviations develop for charge fraction of 20%, in which case a conformational transition of the chain towards a rodlike configuration starts to take place.

Journal Article↗

PubMed2004

Reentrance effect in the lane formation of driven colloids.

Recently it has been shown that a strongly interacting colloidal mixture consisting of oppositely driven particles undergoes a nonequilibrium transition towards lane formation provided the driving strength exceeds a threshold value. We predict here a reentrance effect in lane formation: for fixed high driving force and increasing particle densities, there is first a transition towards lane formation which is followed by another transition back to a state with no lanes. Our result is obtained both by Brownian dynamics computer simulations and by a phenomenological dynamical density functional theory.

Journal Article↗

PubMed2004

Is there a reentrant glass in binary mixtures?

By employing computer simulations for a model binary mixture, we show that a reentrant glass transition upon adding a second component occurs only if the ratio alpha of the short-time mobilities between the glass-forming component and the additive is sufficiently small. For alpha approximately 1, there is no reentrant glass, even if the size asymmetry between the two components is large, in accordance with the two-component mode-coupling theory. For alpha<<1, on the other hand, the reentrant glass is observed and reproduced only by an effective one-component mode-coupling theory.

Journal Article↗

PubMed2004

Attraction between DNA molecules mediated by multivalent ions.

The effective force between two parallel DNA molecules is calculated as a function of their mutual separation for different valencies of counterion and salt ions and different salt concentrations. Computer simulations of the primitive model are used and the shape of the DNA molecules is accurately modeled using different geometrical shapes. We find that multivalent ions induce a significant attraction between the DNA molecules whose strength can be tuned by the averaged valency of the ions. The physical origin of the attraction is traced back either to electrostatics or to entropic contributions. For multivalent counterions and monovalent salt ions, we find a salt-enhanced repulsion effect: the force is first attractive but gets repulsive with increasing salt concentration. Furthermore, we show that the multivalent-ion-induced attraction does not necessarily correlate with DNA overcharging.

Binding Sites↗

PubMed2004

Phase behavior of ionic microgels.

We employ effective interaction potentials between spherical polyelectrolyte microgels in order to investigate theoretically the structure, thermodynamics, and phase behavior of ionic microgel solutions. Combining a genetic algorithm with accurate free energy calculations we are able to perform an unrestricted search of candidate crystal structures. Hexagonal, body-centered orthogonal, and trigonal crystals are found to be stable at high concentrations and charges of the microgels, accompanied by reentrant melting behavior and fluid-fcc-bcc transitions below the overlap concentration.

Journal Article↗

PubMed2003

Crystal structures of two-dimensional magnetic colloids in tilted external magnetic fields.

The stability of different crystal lattices of two-dimensional superparamagnetic suspensions that are confined to a planar liquid-gas interface and exposed to a tilted external magnetic field is studied theoretically by lattice sum minimizations. The magnetic field induces magnetic dipoles onto the colloidal particles along its direction, whose strength can be controlled by the amplitude of the external field. The mutual interaction between the colloids is governed by dipole-dipole forces and a short-ranged repulsion having its physical origin at the presence of the colloidal cores. If the direction of the magnetic field is perpendicular to the liquid-gas interface, there is a purely repulsive interaction leading to stable triangular crystals. By tilting the external field, the interaction becomes anisotropic and a mutual attraction appears upon a threshold tilt angle. We have calculated the full phase diagram at zero temperature varying the tilt angle, the colloidal density, and the strength of the magnetic field. Apart from the triangular lattice we find a variety of stable crystal lattices including rectangular, oblique, chainlike oblique, and rhombic structures. We also present the accurate derivation of the Hamiltonian of two polarizable particles of finite arbitrary geometries in external magnetic and electric fields.

Colloids↗

PubMed2003

Adsorption of monovalent and multivalent cations and anions on DNA molecules.

Adsorption of monovalent and multivalent cations and anions on a deoxyribose nucleic acid (DNA) molecule from a salt solution is investigated by computer simulation. The ions are modeled as charged hard spheres, the DNA molecule as a point charge pattern following the double-helical phosphate strands. The geometrical shape of the DNA molecules is modeled on different levels ranging from a simple cylindrical shape to structured models which include the major and minor grooves between the phosphate strands. The densities of the ions adsorbed on the phosphate strands in the major and in the minor grooves are calculated. First, we find that the adsorption pattern on the DNA surface depends strongly on its geometrical shape: counterions adsorb preferentially along the phosphate strands for a cylindrical model shape, but in the minor groove for a geometrically structured model. Second, we find that an addition of monovalent salt ions results in an increase of the charge density in the minor groove while the total charge density of ions adsorbed in the major groove stays unchanged. The adsorbed ion densities are highly structured along the minor groove while they are almost smeared along the major groove. Furthermore, for a fixed amount of added salt, the major-groove cationic charge is independent of the counterion valency. For increasing salt concentration the major groove is neutralized while the total charge adsorbed in the minor groove is constant. DNA overcharging is detected for multivalent salts. Simulations for larger ion radii, which mimic the effect of ion hydration, indicate an increased adsorbtion of cations in the major groove.

Anions↗

PubMed2003

Depletion forces in nonequilibrium.

The concept of effective depletion forces between two fixed big colloidal particles in a bath of small particles is generalized to a nonequilibrium situation where the bath of small Brownian particles is flowing around the big particles with a prescribed velocity. In striking contrast to the equilibrium case, the nonequilibrium forces violate Newton's third law; they are nonconservative and strongly anisotropic, featuring both strong attractive and repulsive domains.

Journal Article↗

PubMed2003

Nonmonotonic variation with salt concentration of the second virial coefficient in protein solutions.

The osmotic virial coefficient B2 of globular protein solutions is calculated as a function of added salt concentration at fixed pH by computer simulations of the "primitive model." The salt and counterions as well as a discrete charge pattern on the protein surface are explicitly incorporated. For parameters roughly corresponding to lysozyme, we find that B2 first decreases with added salt concentration up to a threshold concentration, then increases to a maximum, and then decreases again upon further raising the ionic strength. Our studies demonstrate that the existence of a discrete charge pattern on the protein surface profoundly influences the effective interactions and that linear and nonlinear Poisson Boltzmann theories fail for large ionic strength. The observed nonmonotonicity of B2 is compared with experiments. Implications for protein crystallization are discussed.

Journal Article↗

PubMed2003

Azimuthal frustration and bundling in columnar DNA aggregates.

The interaction between two stiff parallel DNA molecules is discussed using linear Debye-Hückel screening theory with and without inclusion of the dielectric discontinuity at the DNA surface, taking into account the helical symmetry of DNA. The pair potential furthermore includes the amount and distribution of counterions adsorbed on the DNA surface. The interaction does not only depend on the interaxial separation of two DNA molecules, but also on their azimuthal orientation. The optimal mutual azimuthal angle is a function of the DNA-DNA interaxial separation, which leads to azimuthal frustrations in an aggregate. On the basis of the pair potential, the positional and orientational order in columnar B-DNA assemblies in solution is investigated. Phase diagrams are calculated using lattice sums supplemented with the entropic contributions of the counterions in solution. A variety of positionally and azimuthally ordered phases and bundling transitions is predicted, which strongly depend on the counterion adsorption patterns.

Binding Sites↗

PubMed2002

Phase behavior of columnar DNA assemblies.

The interaction between two stiff parallel DNA molecules depends not only on the distance between their axes but also on their azimuthal orientation. The positional and orientational order in columnar B-DNA assemblies in solution is investigated, on the basis of the electrostatic pair potential that takes into account DNA helical symmetry and the amount and distribution of adsorbed counterions. A phase diagram obtained by lattice sums predicts a variety of positionally and azimuthally ordered phases and bundling transitions strongly depending on the counterion adsorption patterns.

DNA↗

PubMed2002

Effective forces in colloidal mixtures: from depletion attraction to accumulation repulsion.

Computer simulations and theory are used to systematically investigate how the effective force between two big colloidal spheres in a sea of small spheres depends on the basic (big-small and small-small) interactions. The latter are modeled as hardcore pair potentials with a Yukawa tail which can be either repulsive or attractive. For a repulsive small-small interaction, the effective force follows the trends as predicted by a mapping onto an effective nonadditive hardcore mixture: both a depletion attraction and an accumulation repulsion caused by small spheres adsorbing onto the big ones can be obtained depending on the sign of the big-small interaction. For repulsive big-small interactions, the effect of adding a small-small attraction also follows the trends predicted by the mapping. But a more subtle "repulsion through attraction" effect arises when both big-small and small-small attractions occur: upon increasing the strength of the small-small interaction, the effective potential becomes more repulsive. We have further tested several theoretical methods against our computer simulations: The superposition approximation works best for an added big-small repulsion, and breaks down for a strong big-small attraction, while density functional theory is very accurate for any big-small interaction when the small particles are pure hard spheres. The theoretical methods perform most poorly for small-small attractions.

Journal Article↗