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This is a tribute to honor Stefan U. Egelhaaf (1963-2023), a pioneer in experimental soft condensed matter physics., Comment: 4 pages, 1 figure

Laboratory realizations of 2D plasma crystals typically involve monodisperse microparticles confined into horizontal monolayers in radio-frequency (rf) plasma sheaths. This gives rise to the so-called plasma wakes beneath the microparticles. The presence of wakes renders the interactions in such systems non-reciprocal, a fact that can lead to a quite different behaviour from the one expected for their reciprocal counterparts. Here we examine the buckling of a hexagonal 2D plasma crystal, occurring as the confinement strength is decreased, taking explicitly into account the non-reciprocity of the system via a well-established point-particle wake model. We observe that for a finite wake charge, the monolayer hexagonal crystal undergoes a transition first to a bilayer hexagonal structure, unrealisable in harmonically confined reciprocal Yukawa systems, and subsequently to a bilayer square structure. Our theoretical results are confirmed by molecular dynamics simulations for experimentally relevant parameters, indicating the potential of their observation in state-of-the-art experiments with 2D complex plasmas., Comment: 13 pages, 6 figures

Despite a mounting evidence that the same gradients which active colloids use for swimming, induce important cross-interactions (phoretic interaction), they are still ignored in most many-body descriptions, perhaps to avoid complexity and a zoo of unknown parameters. Here we derive a simple model, which reduces phoretic far-field interactions to a pair-interaction whose strength is mainly controlled by one genuine parameter (swimming speed). The model suggests that phoretic interactions are generically important for autophoretic colloids (unless effective screening of the phoretic fields is strong) and should dominate over hydrodynamic interactions for the typical case of half-coating and moderately nonuniform surface mobilities. Unlike standard minimal models, but in accordance with canonical experiments, our model generically predicts dynamic clustering in active colloids at low density. This suggests that dynamic clustering can emerge from the interplay of screened phoretic attractions and active diffusion., Comment: v2,v3 discussion improved, emphasized model limitations; v4 small changes throughout, notation slightly changed, typos corrected, figure updated

We discuss recent progress in the theoretical description of chemotaxis by coupling the diffusion equation of a chemical species to equations describing the motion of sensing microorganisms. In particular, we discuss models for autochemotaxis of a single microorganism which senses its own secretion leading to phenomena such as self-localization and self-avoidance. For two heterogeneous particles, chemotactic coupling can lead to predator-prey behavior including chase and escape phenomena, and to the formation of active molecules, where motility spontaneously emerges when the particles approach each other. We close this review with some remarks on the collective behavior of many particles where chemotactic coupling induces patterns involving clusters, spirals or traveling waves., Comment: to appear as a contribution to the book "Chemical kinetics beyond the textbook"

At the triple point of a repulsive screened Coulomb system, a face-centered-cubic (fcc) crystal, a body-centered-cubic (bcc) crystal and a fluid phase coexist. At their intersection, these three phases form a liquid groove, the triple junction. Using confocal microscopy, we resolve the triple junction on a single particle level in a model system of charged PMMA colloids in a nonpolar solvent. The groove is found to be extremely deep and the incommensurate solid-solid interface to be very broad. Thermal fluctuations hence appear to dominate the solid-solid interface. This indicates a very low interfacial energy. The fcc-bcc interfacial energy is quantitatively determined based on Young's equation and, indeed, it is only about 1.3 times higher than the fcc-fluid interfacial energy close to the triple point.

Ferrogels consist of magnetic colloidal particles embedded in an elastic polymer matrix. As a consequence, their structural and rheological properties are governed by a competition between magnetic particle-particle interactions and mechanical matrix elasticity. Typically, the particles are permanently fixed within the matrix, which makes them distinguishable by their positions. Over time, particle neighbors do not change due to the fixation by the matrix. Here we present a classical density functional approach for such ferrogels. We map the elastic matrix-induced interactions between neighboring colloidal particles distinguishable by their positions onto effective pairwise interactions between indistinguishable particles similar to a "pairwise pseudopotential". Using Monte-Carlo computer simulations, we demonstrate for one-dimensional dipole-spring models of ferrogels that this mapping is justified. We then use the pseudopotential as an input into classical density functional theory of inhomogeneous fluids and predict the bulk elastic modulus of the ferrogel under various conditions. In addition, we propose the use of an "external pseudopotential" when one switches from the viewpoint of a one-dimensional dipole-spring object to a one-dimensional chain embedded in an infinitely extended bulk matrix. Our mapping approach paves the way to describe various inhomogeneous situations of ferrogels using classical density functional concepts of inhomogeneous fluids., Comment: 14 pages, 14 figures

Using liquid integral equation theory, we calculate the pair correlations of particles that interact via a smooth repulsive pair potential in d = 4 spatial dimensions. We discuss the performance of different closures for the Ornstein-Zernike equation, by comparing the results to computer simulation data. Our results are of relevance to understand crystal and glass formation in high-dimensional systems.

While the theory of diffusion of a single Brownian particle in confined geometries is well-established by now, we discuss here the theoretical framework necessary to generalize the theory of diffusion to dense suspensions of strongly interacting Brownian particles. Dynamical density functional theory (DDFT) for classical Brownian particles represents an ideal tool for this purpose. After outlining the basic ingredients to DDFT we show that it can be readily applied to flowing suspensions with time-dependent particle sources. Particle interactions lead to considerable layering in the mean density profiles, a feature that is absent in the trivial case of noninteracting, freely diffusing particles. If the particle injection rate varies periodically in time with a suitable frequency, a resonance in the layering of the mean particle density profile is predicted.

The growth of quasicrystals, i.e., aperiodic structures with long-range order, seeded from the melt is investigated using a dynamical phase field crystal model. Depending on the thermodynamic conditions, two different growth modes are detected, namely defect-free growth of the stable quasicrystal and a mode dominated by phasonic flips which are incorporated as local defects into the grown structure such that random tiling-like ordering emerges. The latter growth mode is unique to quasicrystals and can be verified in experiments on one-component mesoscopic systems.

A basic statistical mechanics analysis of many-body systems with non-reciprocal pair interactions is presented. Different non-reciprocity classes in two- and three-dimensional binary systems (relevant to real experimental situations) are investigated, where the action-reaction symmetry is broken for the interaction between different species. The asymmetry is characterized by a non-reciprocity parameter $\Delta$, which is the ratio of the non-reciprocal to reciprocal pair forces. It is shown that for the "constant" non-reciprocity (when $\Delta$ is independent of the interparticle distance $r$) one can construct a pseudo-Hamiltonian and such systems, being intrinsically non-equilibrium, can nevertheless be described in terms of equilibrium statistical mechanics and exhibit detailed balance with distinct temperatures for the different species. For a general case (when $\Delta$ is a function of $r$) the temperatures grow with time, approaching a universal power-law scaling, while their ratio is determined by an effective constant non-reciprocity which is uniquely defined for a given interaction.

We consider a two-dimensional complex plasma layer containing charged dust particles in a perpendicular magnetic field. Computer simulations of both one-component and binary systems are used to explore the equilibrium particle dynamics in the fluid state. The mobility is found to scale with the inverse of the magnetic field strength (Bohm diffusion) for strong fields. For bidisperse mixtures, the magnetic field dependence of the long-time mobility depends on the particle species providing an external control of their mobility ratio. For large magnetic fields, even a two-dimensional model porous matrix can be realized composed by the almost immobilized high-charge particles which act as obstacles for the mobile low-charge particles.

Recent studies on confined crystals of charged colloidal particles are reviewed, both in equilibrium and out of equilibrium. We focus in particular on direct comparisons of experiments (light scattering and microscopy) with lattice sum calculations and computer simulations. In equilibrium we address buckling and crystalline multilayering of charged systems in hard and soft slit confinement. We discuss also recent crystalline structures obtained for charged mixtures. Moreover, we put forward possibilities to apply external perturbations, in order to drive the system out of equilibrium. These include electrolyte gradients as well as the application of shear and electric fields., Comment: Review article, 18 pages, 5 figures

Cluster growth in a coagulating system of active particles (such as microswimmers in a solvent) is studied by theory and simulation. In contrast to passive systems, the net velocity of a cluster can have various scalings dependent on the propulsion mechanism and alignment of individual particles. Additionally, the persistence length of the cluster trajectory typically increases with size. As a consequence, a growing cluster collects neighbouring particles in a very efficient way and thus amplifies its growth further. This results in unusual large growth exponents for the scaling of the cluster size with time and, for certain conditions, even leads to "explosive" cluster growth where the cluster becomes macroscopic in a finite amount of time., Comment: 8 pages, 5 figures

Catching fish with a fishing net is typically done either by dragging a fishing net through quiescent water or by placing a stationary basket trap into a stream. We transfer these general concepts to micron-sized self-motile particles moving in a solvent at low Reynolds number and study their collective trapping behaviour by means of computer simulations of a two-dimensional system of self-propelled rods. A chevron-shaped obstacle is dragged through the active suspension with a constant speed $v$ and acts as a trapping "net". Three trapping states can be identified corresponding to no trapping, partial trapping and complete trapping and their relative stability is studied as a function of the apex angle of the wedge, the swimmer density and the drag speed $v$. When the net is dragged along the inner wedge, complete trapping is facilitated and a partially trapped state changes into a complete trapping state if the drag speed exceeds a certain value. Reversing the drag direction leads to a reentrant transition from no trapping, complete trapping, back to no trapping upon increasing the drag speed along the outer wedge contour. The transition to complete trapping is marked by a templated self-assembly of rods forming polar smectic structures anchored onto the inner contour of the wedge. Our predictions can be verified in experiments of artificial or microbial swimmers confined in microfluidic trapping devices., Comment: 10 pages, 6 figures

We introduce and investigate a coarse-grained model for quasi one-dimensional ferrogels. In our description the magnetic particles are represented by hard spheres with a magnetic dipole moment in their centers. Harmonic springs connecting these spheres mimic the presence of a cross-linked polymer matrix. A special emphasis is put on the coupling of the dipolar orientations to the elastic deformations of the matrix, where a memory effect of the orientations is included. Although the particles are displaced along one spatial direction only, the system already shows rich behavior: as a function of the magnetic dipole moment, we find a phase transition between "soft-elastic" states with finite interparticle separation and finite compressive elastic modulus on the one hand, and "hardened" states with touching particles and therefore diverging compressive elastic modulus on the other hand. Corresponding phase diagrams are derived neglecting thermal fluctuations of the magnetic particles. In addition, we consider a situation in which a spatially homogeneous magnetization is initially imprinted into the material. Depending on the strength of the magneto-mechanical coupling between the dipole orientations and the elastic deformations, the system then relaxes to a uniaxially ferromagnetic, an antiferromagnetic, or a spiral state of magnetization to minimize its energy. One purpose of our work is to provide a largely analytically solvable approach that can provide a benchmark to test future descriptions of higher complexity. From an applied point of view, our results could be exploited, for example, for the construction of novel damping devices of tunable shock absorbance., Comment: 12 pages, 12 figures

A competition of incommensurate symmetries occurs whenever a system is forced to conform to an ordering that is different from the intrinsically preferred structure of the system itself. As a model system of such a competition, we study the rivalry between the triangular ordering of hard disks and the square symmetry induced by a periodic square substrate. By using density functional theory as well as Monte Carlo computer simulations, we determine the full phase behavior for the case of one particle per minimum. We observe a rhombic preordering structure preceding the hexagonal solid as a direct consequence of the competing symmetries. Furthermore, the square-rhombic transition is reentrant with increasing substrate interaction. Our predictions can be verified in experiments of colloids in laser fields., Comment: 5 pages, 4 figures

Strongly coupled plasmas in which the interaction energy exceeds the kinetic energy play an important role in many astrophysical and laboratory systems including compact stars, laser plasmas and dusty plasmas. They exhibit many unusual collective properties, such as liquid or crystalline behaviour, peculiar oscillation spectra and transport properties. Recently, strongly coupled plasmas were studied in the presence of a strong magnetic field by computer simulations, and strong modifications of their transport properties and oscillation spectra were observed. While strong magnetization is common in stellar systems it is practically impossible to achieve in complex plasmas due to the large mass of the dust particles. Here we discuss a recently demonstrated approach to achieve very strong "magnetization" by a rotation of the neutral gas, and we present new results for macroscopic two-dimensional systems.

We propose and demonstrate a concept that mimics the magnetization of the heavy dust particles in a complex plasma while leaving the properties of the light species practically unaffected. It makes use of the frictional coupling between a complex plasma and the neutral gas, which allows to transfer angular momentum from a rotating gas column to a well-controlled rotation of the dust cloud. This induces a Coriolis force that acts exactly as the Lorentz force in a magnetic field. Experimental normal mode measurements for a small dust cluster with four particles show excellent agreement with theoretical predictions for a magnetized plasma.

Dense suspensions of self-propelled rod-like particles exhibit a fascinating variety of non-equilibrium phenomena. By means of computer simulations of a minimal model for rigid self-propelled colloidal rods with variable shape we explore the generic diagram of emerging states over a large range of rod densities and aspect ratios. The dynamics is studied using a simple numerical scheme for the overdamped noiseless frictional dynamics of a many-body system in which steric forces are dominant over hydrodynamic ones. The different emergent states are identified by various characteristic correlation functions and suitable order parameter fields. At low density and aspect ratio, a disordered phase with no coherent motion precedes a highly-cooperative swarming state at large aspect ratio. Conversely, at high densities weakly anisometric particles show a distinct jamming transition whereas slender particles form dynamic laning patterns. In between there is a large window corresponding to strongly vortical, turbulent flow. The different dynamical states should be verifiable in systems of swimming bacteria and artificial rod-like micro-swimmers., Comment: 14 pages, 8 figures

For many applications, it is important to catch collections of autonomously navigating microbes and man-made microswimmers in a controlled way. Here we propose an efficient trap to collectively capture self-propelled colloidal rods. By means of computer simulation in two dimensions, we show that a static chevron-shaped wall represents an optimal boundary for a trapping device. Its catching efficiency can be tuned by varying the opening angle of the trap. For increasing angles, there is a sequence of three emergent states corresponding to partial, complete, and no trapping. A trapping `phase diagram' maps out the trap conditions under which the capture of self-propelled particles at a given density is rendered optimal., Comment: 5 pages, 4 figures

We perform a comparative study of the free energies and the density distributions in hard sphere crystals using Monte Carlo simulations and density functional theory (employing Fundamental Measure functionals). Using a recently introduced technique (Schilling and Schmid, J. Chem. Phys 131, 231102 (2009)) we obtain crystal free energies to a high precision. The free energies from Fundamental Measure theory are in good agreement with the simulation results and demonstrate the applicability of these functionals to the treatment of other problems involving crystallization. The agreement between FMT and simulations on the level of the free energies is also reflected in the density distributions around single lattice sites. Overall, the peak widths and anisotropy signs for different lattice directions agree, however, it is found that Fundamental Measure theory gives slightly narrower peaks with more anisotropy than seen in the simulations. Among the three types of Fundamental Measure functionals studied, only the White Bear II functional (Hansen-Goos and Roth, J. Phys.: Condens. Matter 18, 8413 (2006)) exhibits sensible results for the equilibrium vacancy concentration and a physical behavior of the chemical potential in crystals constrained by a fixed vacancy concentration., Comment: 17 pages, submitted to Phys. Rev. E

We examine binary mixtures of superparamagnetic colloidal particles confined to a two-dimensional water-air interface both by real-space experiments and Monte-Carlo computer simulations at high coupling strength. In the simulations, the interaction is modelled as a pairwise dipole-dipole repulsion. While the ratio of magnetic dipole moments is fixed, the interaction strength governed by the external magnetic field and the relative composition is varied. Excellent agreement between simulation and experiment is found for the partial pair distribution functions including the fine structure of the neighbour shells at high coupling. Furthermore local crystal nuclei in the melt are identified by bond-orientational order parameters and their contribution to the pair structure is discussed.

The dynamical onset of lane formation is studied in experiments with binary complex plasmas under microgravity conditions. Small microparticles are driven and penetrate into a cloud of big particles, revealing a strong tendency towards lane formation. The observed time-resolved lane formation process is in good agreement with computer simulations of a binary Yukawa model with Langevin dynamics. The laning is quantified in terms of the anisotropic scaling index, leading to a universal order parameter for driven systems., Comment: 4 pages, 3 figures, movies available at http://www.mpe.mpg.de/pke/lane-formation/

Non-equilibrium collective behavior of self-propelled colloidal rods in a confining channel is studied using Brownian dynamics simulations and dynamical density functional theory. We observe an aggregation process in which rods self-organize into transiently jammed clusters at the channel walls. In the early stage of the process, fast-growing hedgehog-like clusters are formed which are largely immobile. At later stages, most of these clusters dissolve and mobilize into nematized aggregates sliding past the walls., Comment: 5 pages, 4 figures

As a generic model for liquid-vapour type transitions in random porous media, the Asakura-Oosawa model for colloid-polymer mixtures is studied in a matrix of quenched spheres using extensive Monte Carlo (MC) simulations. Since such systems at criticality, as well as in the two-phase region, exhibit lack of self-averaging, the analysis of MC data via finite size scaling requires special care. After presenting the necessary theoretical background and the resulting subtleties of finite size scaling in random-field Ising-type systems, we present data on the order parameter distribution (and its moments) as a function of colloid and polymer fugacities for a broad range of system sizes, and for many (thousands) realizations of the porous medium. Special attention is paid to the connected and disconnected susceptibilities, and their respective critical behavior. We show that both susceptibilities diverge at the critical point, and we demonstrate that this is compatible with the predicted scenario of random-field Ising universality., Comment: 24 pages, CODEF II conference proceedings paper, Bonn, Germany (2008)

A density functional theory for colloidal dynamics is presented which includes hydrodynamic interactions between the colloidal particles. The theory is applied to the dynamics of colloidal particles in an optical trap which switches periodically in time from a stable to unstable confining potential. In the absence of hydrodynamic interactions, the resulting density breathing mode, exhibits huge oscillations in the trap center which are almost completely damped by hydrodynamic interactions. The predicted dynamical density fields are in good agreement with Brownian dynamics computer simulations.

Using extensive Brownian dynamics computer simulations, the long-time self-diffusion coefficient is calculated for Gaussian-core particles as a function of the number density. Both spherical and rod-like particles interacting via Gaussian segments ar$ For increasing concentration we find that the translational self-diffusion behaves non-monotonically reflecting the structural reentrance effect in the equilibrium phase diagram. Both in the limits of zero and infinite concentration, it approaches its short-time value. The microscopic Medina-Noyola theory qualitatively accounts for the translational long-time diffusion. The long-time orientational diffusion coefficient for Gaussian rods, on the other hand, remains very close to its short-time counterpart for any density. Some implications of the weak translation-rotation coupling for ultrasoft rods are discussed., Comment: 5 pages, 5 figures

We show that the critical behavior of a colloid-polymer mixture inside a random porous matrix of quenched hard spheres belongs to the universality class of the random-field Ising model. We also demonstrate that random-field effects in colloid-polymer mixtures are surprisingly strong. This makes these systems attractive candidates to study random-field behavior experimentally., Comment: 4 pages, 3 figures, to appear in Phys. Rev. Lett

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, {\em independent} of the imposed drag speed. Our results are based on non-equilibrium Brownian dynamics computer simulations and in line with a dynamical scaling theory., Comment: 4 pages, 5 figures, to appear in Phys. Rev. Lett

We examine the vitrification and melting of asymmetric star polymers mixtures by combining rheological measurements with mode coupling theory. We identify two types of glassy states, a {\it single} glass, in which the small component is fluid in the glassy matrix of the big one and a {\it double} glass, in which both components are vitrified. Addition of small star polymers leads to melting of {\it both} glasses and the melting curve has a non-monotonic dependence on the star-star size ratio. The phenomenon opens new ways for externally steering the rheological behavior of soft matter systems., Comment: 4 pages, 4 figures, accepted in Phys. Rev. Lett

We show how to implement stick boundary conditions for a spherical colloid in a solvent that is coarse-grained by the method of stochastic rotation dynamics. This allows us to measure colloidal rotational velocity auto-correlation functions by direct computer simulation. We find quantitative agreement with Enskog theory for short times and with hydrodynamic mode-coupling theory for longer times. For aqueous colloidal suspensions, the Enskog contribution to the rotational friction is larger than the hydrodynamic one when the colloidal radius drops below 35nm., Comment: new version with some minor changes

The effective DNA-DNA interaction force is calculated by computer simulations with explicit tetravalent counterions and monovalent salt. For overcharged DNA molecules, the interaction force shows a double-minimum structure. The positions and depths of these minima are regulated by the counterion density in the bulk. Using two-dimensional lattice sum and free energy perturbation theories, the coexisting phases for DNA bundles are calculated. A DNA-condensation and redissolution transition and a stable mesocrystal with an intermediate lattice constant for high counterion concentration are obtained., Comment: 26 pages, 10 figures

The distance-resolved effective interaction potential between two parallel DNA molecules is calculated by computer simulations with explicit tetravalent counterions and monovalent salt. Adding counterions first yields an attractive minimum in the potential at short distances which then disappears in favor of a shallower minimum at larger separations. The resulting phase diagram includes a DNA-condensation and redissolution transition and a stable mesocrystal with an intermediate lattice constant for high counterion concentration., Comment: 4 pages, 4 figures

The onset of the Rayleigh-Taylor instability is studied a compressible Brownian Yukawa fluid mixture on the ``molecular'' length and time scales of the individual particles. As a model, a two-dimensional phase-separated symmetric binary mixture of colloidal particles of type $A$ and $B$ with a fluid-fluid interface separating an $A$-rich phase from a $B$-rich phase is investigated by Brownian computer simulations when brought into non-equilibrium via a constant external driving field which acts differently on the different particles and perpendicular to the interface. Two different scenarios are observed which occur either for high or for low interfacial free energies as compared to the driving force. In the first scenario for high interfacial tension, the critical wavelength $\lambda_c$ of the unstable interface modes is in good agreement with the classical Rayleigh-Taylor formula provided dynamically rescaled values for the interfacial tension are used. The wavelength $\lambda_{c}$ increases with time representing a self-healing effect of the interface due to a local density increase near the interface. The Rayleigh-Taylor formula is confirmed even if $\lambda_c$ is of the order of a molecular correlation length. In the second scenario for very large driving forces as compared to the interfacial line tensions, on the other hand, the particle penetrate easily the interface by the driving field and form microscopic lanes with a width different from the predictions of the classical Rayleigh-Taylor formula., Comment: 30 pages, 11 figures, submitted to Phys. Rev. E

The effective force between two parallel DNA molecules is calculated as a function of their mutual separation for different valencies of counter- and salt ions and different salt concentrations. Computer simulations of the primitive model are used and the shape of the DNA molecules is accurately modelled 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 counter- and monovalent salt ions, we find a salt-induced stabilization effect: the force is first attractive but gets repulsive for increasing salt concentration. Furthermore, we show that the multivalent-ion-induced attraction does not necessarily correlate with DNA overcharging., Comment: 51 pages and 13 figures

Adsorption of monovalent and multivalent cat- and anions on a deoxyribose nucleic acid (DNA) molecule from a salt solution is investigated by computer simulation. The ions are modelled 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 modelled 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 on 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 salt. Simulations for a larger ion radii, which mimic the effect of the ion hydration, indicate an increased adsorbtion of cations in the major groove., Comment: 34 pages with 14 figures

The influence of an external field acting differently on the two constituents of a binary colloidal mixture performing Brownian dynamics is investigated by computer simulations and a simple theory. In our model, one half of the particles ($A$-particles) are pulled by an external force ${\vec F}^{(A)}$ while the other half of them ($B$-particles) are pulled by an external force ${\vec F}^{(B)}$. If ${\vec F}^{(A)}$ and ${\vec F}^{(B)}$ are parallel and the field-free state is a mixed fluid, previous simulations (J. Dzubiella et al, Phys. Rev. E {\bf 65} 021402 (2002)) have shown a nonequilibrium pattern formation involving lanes of $A$ or $B$ particles only which are sliding against each other in the direction of the external forces. In this paper, we generalize the situation both to non-parallel external forces and to field-free crystalline states. For non-parallel forces, lane formation is also observed but with an orientation {\it tilted} with respect to the external forces. If the field-free state is crystalline, a continuous increase of the parallel external forces yields a novel {\it reentrant freezing} behavior: the crystal first melts mechanically via the external force and then recrystallizes into demixed crystalline lanes sliding against each other., Comment: 16 pages, 8 figures

The osmotic virial coefficient $B_2$ 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 counter-ions as well as a discrete charge pattern on the protein surface are explicitly incorporated. For parameters roughly corresponding to lysozyme, we find that $B_2$ 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 non-linear Poisson Boltzmann and Derjaguin-Landau-Verwey-Overbeek (DLVO) theory fail for large ionic strength. The observed non-monotonicity of $B_2$ is compared to experiments. Implications for protein crystallization are discussed., Comment: 43 pages, including 17 figures

The pair interaction between two stiff parallel linear DNA molecules depends not only on the distance between their axes but on their azimuthal orientation. The positional and orientational order in columnar B-DNA assemblies in solution is investigated, based on the DNA-DNA electrostatic pair potential that takes into account DNA helical symmetry and the amount and distribution of adsorbed counterions. A phase diagram obtained by lattice sum calculations predicts a variety of positionally and azimuthally ordered phases and bundling transitions strongly depending on the counterion adsorption patterns., Comment: 4 pages, 3 figures, submitted to PRL

The effective Coulomb interaction between globular proteins is calculated as a function of monovalent salt concentration $c_s$, by explicit Molecular Dynamics simulations of pairs of model proteins in the presence of microscopic co and counterions. For discrete charge patterns of monovalent sites on the surface, the resulting osmotic virial coefficient $B_2$ is found to be a strikingly non-monotonic function of $c_s$. The non-monotonicity follows from a subtle Coulomb correlation effect which is completely missed by conventional non-linear Poisson-Boltzmann theory and explains various experimental findings., Comment: 4 twocolumn pages with 4 figures

Using monomer-resolved Molecular Dynamics simulations and theoretical arguments based on the radial dependence of the osmotic pressure in the interior of a star, we systematically investigate the effective interactions between hard, colloidal particles and star polymers in a good solvent. The relevant parameters are the size ratio q between the stars and the colloids, as well as the number of polymeric arms f (functionality) attached to the common center of the star. By covering a wide range of q's ranging from zero (star against a flat wall) up to about 0.75, we establish analytical forms for the star-colloid interaction which are in excellent agreement with simulation results. A modified expression for the star-star interaction for low functionalities, f < 10 is also introduced., Comment: 37 pages, 14 figures, preprint-version

Using small-angle neutron scattering and liquid integral equation theory, we relate the structure factor of flexible dendrimers of 4th generation to their average shape. The shape is measured as a radial density profile of monomers belonging to a single dendrimer. From that, we derive an effective interaction of Gaussian form between pairs of dendrimers and compute the structure factor using the hypernetted chain approximation. Excellent agreement with the corresponding experimental results is obtained, without the use of adjustable parameters. The present analysis thus strongly supports the previous finding that flexible dendrimers of low generation present fluctuating structures akin to star polymers., Comment: 20 pages, 4 figures, submitted to Macromolecules on July 24, 2000

We study the effect of solvent granularity on the effective force between two charged colloidal particles by computer simulations of the primitive model of strongly asymmetric electrolytes with an explicitly added hard sphere solvent. Apart from molecular oscillating forces for nearly touching colloids which arise from solvent and counterion layering, the counterions are attracted towards the colloidal surfaces by solvent depletion providing a simple statistical description of hydration. This, in turn, has an important influence on the effective forces for larger distances which are considerably reduced as compared to the prediction based on the primitive model. When these forces are repulsive, the long-distance behaviour can be described by an effective Yukawa pair potential with a solvent-renormalized charge. As a function of colloidal volume fraction and added salt concentration, this solvent-renormalized charge behaves qualitatively similar to that obtained via the Poisson-Boltzmann cell model but there are quantitative differences. For divalent counterions and nano-sized colloids, on the other hand, the hydration may lead to overscreened colloids with mutual attraction while the primitive model yields repulsive forces. All these new effects can be accounted for through a solvent-averaged primitive model (SPM) which is obtained from the full model by integrating out the solvent degrees of freedom. The SPM was used to access larger colloidal particles without simulating the solvent explicitly., Comment: 14 pages, 16 craphics

Using computer simulations of two charged colloidal spheres with their counterions in a hard sphere solvent, we show that the granular nature of the solvent significantly influences the effective colloidal interaction. For divalent counterions, the total effective force can become attractive generated by counterion hydration, while for monovalent counterions the forces are repulsive and well-described by a solvent-induced colloidal charge renormalization. Both effects are not contained in the traditional "primitive" approaches but can be accounted for in a solvent-averaged primitive model., Comment: 4 pages, 3 figures

The effective interaction between two parallel strands of helical bio-molecules, such as deoxyribose nucleic acids (DNA), is calculated using computer simulations of the "primitive" model of electrolytes. In particular we study a simple model for B-DNA incorporating explicitly its charge pattern as a double-helix structure. The effective force and the effective torque exerted onto the molecules depend on the central distance and on the relative orientation. The contributions of nonlinear screening by monovalent counterions to these forces and torques are analyzed and calculated for different salt concentrations. As a result, we find that the sign of the force depends sensitively on the relative orientation. For intermolecular distances smaller than $6\AA$ it can be both attractive and repulsive. Furthermore we report a nonmonotonic behaviour of the effective force for increasing salt concentration. Both features cannot be described within linear screening theories. For large distances, on the other hand, the results agree with linear screening theories provided the charge of the bio-molecules is suitably renormalized., Comment: 18 pages, 18 figures included in text, 100 bibliogr

Using computer simulations we investigate the microscopic structure of the singular director field within a nematic droplet. As a theoretical model for nematic liquid crystals we take hard spherocylinders. To induce an overall topological charge, the particles are either confined to a two-dimensional circular cavity with homeotropic boundary or to the surface of a three-dimensional sphere. Both systems exhibit half-integer topological point defects. The isotropic defect core has a radius of the order of one particle length and is surrounded by free-standing density oscillations. The effective interaction between two defects is investigated. All results should be experimentally observable in thin sheets of colloidal liquid crystals., Comment: 13 pages, 16 figures, Phys. Rev. E