arXiv subjects
Publications and source records attributed to Hartmut Löwen.
In a Comment [Phys. Rev. Lett. 113, 029801 (2014)] on our Letter on self-propelled asymmetric particles [Phys. Rev. Lett. 110, 198302 (2013); arXiv:1302.5787], Felderhof claims that our theory based on Langevin equations would be conceptually wrong. In this Reply we show that our theory is appropriate, consistent, and physically justified.
Magnetic elastomers are appealing materials from an application point of view: they combine the mechanical softness and deformability of polymeric substances with the addressability by external magnetic fields. In this way, mechanical deformations can be reversibly induced and elastic moduli can be reversibly adjusted from outside. So far, mainly the behavior of single-component magnetic elastomers and ferrogels has been studied. Here, we go one step further and analyze the magnetoelastic response of a bilayered material composed of two different magnetic elastomers. It turns out that, under appropriate conditions, the bilayered magnetic elastomer can show a strongly amplified deformational response in comparison to a single-component material. Furthermore, a qualitatively opposite response can be obtained, i.e.\ a contraction along the magnetic field direction (as opposed to an elongation in the single-component case). We hope that our results will further stimulate experimental and theoretical investigations directly on bilayered magnetic elastomers, or, in a further hierarchical step, on bilayered units embedded in yet another polymeric matrix.
The equilibrium structure and dynamics of a single polymer chain in a thermal solvent is by now well-understood in terms of scaling laws. Here we consider a polymer in a bacterial bath, i.e. in a solvent consisting of active particles which bring in nonequilibrium fluctuations. Using computer simulations of a self-avoiding polymer chain in two dimensions which is exposed to a dilute bath of active particles, we show that the Flory-scaling exponent is unaffected by the bath activity provided the chain is very long. Conversely, for shorter chains, there is a nontrivial coupling between the bacteria intruding into the chain which may stiffen and expand the chain in a nonuniversal way. As a function of the molecular weight, the swelling first scales faster than described by the Flory exponent, then an unusual plateau-like behaviour is reached and finally a crossover to the universal Flory behaviour is observed. As a function of bacterial activity, the chain end-to-end distance exhibits a pronounced non-monotonicity. Moreover, the mean-square displacement of the center of mass of the chain shows a ballistic behaviour at intermediate times as induced by the active solvent. Our predictions are verifiable in two-dimensional bacterial suspensions and for colloidal model chains exposed to artificial colloidal microswimmers.
We demonstrate that collective turbulent-like motion in a bacterial bath can power and steer directed transport of mesoscopic carriers through the suspension. In our experiments and simulations, a microwedge-like "bulldozer" draws energy from a bacterial bath of varied density. We obtain that a maximal transport speed is achieved in the turbulent state of the bacterial suspension. This apparent rectification of random motion of bacteria is caused by polar ordered bacteria inside the cusp region of the carrier, which is shielded from the outside turbulent fluctuations.
The ionic composition and pair correlations in fluid phases of realistically salt-free charged colloidal sphere suspensions are calculated in the primitive model. We obtain the number densities of all ionic species in suspension, including low-molecular weight microions, and colloidal macroions with acidic surface groups, from a self-consistent solution of a coupled physicochemical set of nonlinear algebraic equations and non-mean-field liquid integral equations. Here, we study suspensions of colloidal spheres with sulfonate or silanol surface groups, suspended in demineralized water that is saturated with carbon dioxide under standard atmosphere. The only input required for our theoretical scheme are the acidic dissociation constants pKa, and effective sphere diameters of all involved ions. Our method allows for an ab initio calculation of colloidal bare and effective charges, at high numerical efficiency.
Typically, in the description of active Brownian particles, a constant effective propulsion force is assumed, which is then subjected to fluctuations in orientation and translation leading to a persistent random walk with an enlarged long-time diffusion coefficient. Here, we generalize previous results for the swimming path statistics to a time-dependent and thus in many situations more realistic propulsion which is a prescribed input. We analytically calculate both the noise-free and the noise-averaged trajectories for time-periodic propulsion under the action of an additional torque. In the deterministic case, such an oscillatory microswimmer moves on closed paths that can be highly more complicated than the commonly observed straight lines and circles. When exposed to random fluctuations, the mean trajectories turn out to be self-similar curves which bear the characteristics of their noise-free counterparts. Furthermore, we consider a propulsion force which scales in time $t$ as $\propto \! t^α$ (with $α=0,1,2,\ldots$) and analyze the resulting superdiffusive behaviour. Our predictions are verifiable for diffusiophoretic artificial microswimmers with prescribed propulsion protocols.
The glass transition is investigated in three dimensions for single and double Yukawa potentials for the full range of control parameters. For vanishing screening parameter, the limit of the one-component plasma is obtained; for large screening parameters and high coupling strengths, the glass-transition properties crossover to the hard-sphere system. Between the two limits, the entire transition diagram can be described by analytical functions. Different from other potentials, the glass-transition and melting lines for Yukawa potentials are found to follow shifted but otherwise identical curves in control-parameter space.
We synthesize colloidal particles with various anisotropic shapes and track their orientationally resolved Brownian trajectories using confocal microscopy. An analysis of appropriate short-time correlation functions provides direct access to the hydrodynamic friction tensor of the particles revealing nontrivial couplings between the translational and rotational degrees of freedom. The results are consistent with calculations of the hydrodynamic friction tensor in the low-Reynolds-number regime for the experimentally determined particle shapes.
A recently introduced active phase field crystal model describes the formation of ordered resting and traveling crystals in systems of self-propelled particles. Increasing the active drive, a resting crystal can be forced to perform collectively ordered migration as a single traveling object. We demonstrate here that these ordered migrating structures are linearly stable. In other words, during migration, the single crystalline texture together with the globally ordered collective motion is preserved even on large length scales. Furthermore, we consider self-propelled particles on a substrate that are surrounded by a thin fluid film. We find that in this case the resulting hydrodynamic interactions can destabilize the order.
The kinetic separation of repulsive active Brownian particles into a dense and a dilute phase is analyzed using a systematic coarse-graining strategy. We derive an effective Cahn-Hilliard equation on large length and time scales, which implies that the separation process can be mapped onto that of passive particles. A lower density threshold for clustering is found, and using our approach we demonstrate that clustering first proceeds via a hysteretic nucleation scenario and above a higher threshold changes into a spinodal-like instability. Our results are in agreement with particle-resolved computer simulations and can be verified in experiments of artificial or biological microswimmers.
The behaviour of materials under spatial confinement is sensitively dependent on the nature of the confining boundaries. In two dimensions, confinement within a hard circular boundary inhibits the hexagonal ordering observed in bulk systems at high density. Using colloidal experiments and Monte Carlo simulations, we investigate two model systems of quasi hard discs under circularly symmetric confinement. The first system employs an adaptive circular boundary, defined experimentally using holographic optical tweezers. We show that deformation of this boundary allows, and indeed is required for, hexagonal ordering in the confined system. The second system employs a circularly symmetric optical potential to confine particles without a physical boundary. We show that, in the absence of a curved wall, near perfect hexagonal ordering is possible. We propose that the degree to which hexagonal ordering is suppressed by a curved boundary is determined by the `strictness' of that wall.
Progress in the research area of colloidal dispersions in external fields within the last years is reviewed. Colloidal dispersions play a pivotal role as model systems for phase transitions in classical statistical mechanics. In recent years the leading role of colloids to realize model systems has become evident not only for equilibrium situations but also far away from equilibrium. By using external fields (such as shear flow, electric, magnetic or laseroptical fields as well as confinement), a colloidal suspension can be brought into nonequilibrium in a controlled way. Various kinds of equilibrium and nonequilibrium phenomena explored by colloidal dispersions are described providing also a guide and summary to this special issue. Particular emphasis is put on the comparison of real-space experiments, computer simulations and statistical theories.
This mini-review is concerned with two-dimensional colloidal mixtures exposed to various kinds of external fields. By a magnetic field perpendicular to the plane, dipole moments are induced in paramagnetic particles which give rise to repulsive interactions leading to complex crystalline alloys in the composition-asymmetry diagram. A quench in the magnetic field induces complex crystal nucleation scenarios. If exposed to a gravitational field, these mixtures exhibit a brazil--nut effect and show a boundary layering which is explained in terms of a depletion bubble picture. The latter persists for time-dependent gravity ("colloidal shaking"). Finally, we summarize crystallization effects when the second species is frozen in a disordered matrix which provides obstacles for the crystallizing component.
We review recent progress in the theoretical description of anisotropic hard colloidal particles. The shapes considered range from rods and dumbbells to rounded cubes, polyhedra and to biaxial particles with arbitrary shape. Our focus is on both static and dynamical density functional theory and on computer simulations. We describe recent results for the structure, dynamics and phase behaviour in the bulk and in various confining geometries, e.g. established by two parallel walls which reduce the dimensionality of the system to two dimensions. We also include recent theoretical modelling for active particles, which are autonomously driven by some intrinsic motor, and highlight their fascinating nonequilibrium dynamics and collective behaviour.
Spherical Janus particles are one of the most prominent examples for active Brownian objects. Here, we study the diffusiophoretic motion of such microswimmers in experiment and in theory. Three stages are found: simple Brownian motion at short times, super-diffusion at intermediate times, and finally diffusive behavior again at long times. These three regimes observed in the experiments are compared with a theoretical model for the Langevin dynamics of self-propelled particles with coupled translational and rotational motion. Besides the mean square displacement also higher displacement moments are addressed. In particular, theoretical predictions regarding the non-Gaussian behavior of self-propelled particles are verified in the experiments. Furthermore, the full displacement probability distribution is analyzed, where in agreement with Brownian dynamics simulations either an extremely broadened peak or a pronounced double-peak structure is found depending on the experimental conditions.
The motion of a deformable active particle in linear shear flow is explored theoretically. Based on symmetry considerations, in two spatial dimensions, we propose coupled nonlinear dynamical equations for the particle position, velocity, deformation, and rotation. In our model, both, passive rotations induced by the shear flow as well as active spinning motions, are taken into account. Our equations reduce to known models in the two limits of vanishing shear flow and vanishing particle deformability. For varied shear rate and particle propulsion speed, we solve the equations numerically and obtain a manifold of different dynamical modes including active straight motion, periodic motions, motions on undulated cycloids, winding motions, as well as quasi-periodic and chaotic motions induced at high shear rates. The types of motion are distinguished by different characteristics in the real-space trajectories and in the dynamical behavior of the particle orientation and its deformation. Our predictions can be verified in experiments on self-propelled droplets exposed to a linear shear flow.
Motivated by recent experiments on colloidal suspensions, we study analytically and numerically a microscopic model for self-propelled particles lacking alignment interactions. In this model, even for purely repulsive interactions, a dynamical instability leading to phase separation has been reported. Starting from the many-body Smoluchowski equation, we develop a mean-field description based on a novel closure scheme and derive the effective hydrodynamic equations. We demonstrate that the microscopic origin of the instability is a force imbalance due to an anisotropic pair distribution leading to self-trapping. The phase diagram can be understood in terms of two quantities: a minimal drive and the force imbalance. At sufficiently high propulsion speeds there is a reentrance into the disordered fluid.
The pair-correlation functions for fluid ionic mixtures in arbitrary spatial dimensions are computed in hypernetted chain (HNC) approximation. In the primitive model, all ions are approximated as non-overlapping hyperspheres with Coulomb interactions. Our spectral HNC solver is based on a Fourier-Bessel transform introduced by Talman [J. Comput. Phys., 29, 35 (1978)], with logarithmically spaced computational grids. Numeric efficiency for arbitrary spatial dimensions is a commonly exploited virtue of this transform method. Here, we highlight another advantage of logarithmic grids, consisting in efficient sampling of pair-correlation functions for highly asymmetric ionic mixtures. For three-dimensional fluids, ion size- and charge-ratios larger than one thousand can be treated, corresponding to hitherto computationally not accessed micrometer-sized colloidal spheres in 1-1 electrolyte. Effective colloidal charge numbers are extracted from our primitive model results. For moderately large ion size- and charge-asymmetries, we present Molecular Dynamics simulation results that agree well with the approximate HNC pair correlations.