arXiv subjects

Sabine H. L. Klapp

Publications and source records attributed to Sabine H. L. Klapp.

At least 73 records · Page 4Linked to original sources

arXiv2017

Coarse-graining strategy for molecular pair interactions: A reaction coordinate study for two- and three-dimensional systems

We investigate and provide optimal sets of reaction coordinates for mixed pairs of molecules displaying polar, uniaxial, or spherical symmetry in two and three dimensions. These coordinates are non-redundant, i.e., they implicitly involve the molecules' symmetries. By tabulating pair interactions in these coordinates, resulting tables are thus minimal in length and require a minimal memory space. The intended fields of application are computer simulations of large ensembles of molecules or colloids with rather complex interactions in a fluid or liquid crystalline phase at low densities. Using effective interactions directly in the form of tables can help bridging the time and length scales without introducing errors stemming from any modeling procedure. Finally, we outline an exemplary computational methodology for gaining an effective pair potential in these coordinates, based on the Boltzmann inversion principle, by providing a step-by-step recipe.

cond-mat.stat-mech↗

arXiv2017

Shear-induced laning transition in a confined colloidal film

Using Brownian dynamics (BD) simulations we investigate a dense system of charged colloids exposed to shear flow in a confined (slit-pore) geometry. The equilibrium system at zero flow consists of three, well-pronounced layers with square-like crystalline in-plane structure. We demonstrate that, for sufficiently large shear rates, the middle layer separates into two sublayers where the particles organize into moving lanes with opposite velocities. The formation of this micro-laned state results in a destruction of the applied shear profile. It has a strong impact not only on the structure of the system, but also on its rheology as measured by the stress tensor. At higher shear rates we observe a disordered state and finally a recrystallization reminiscent of the behavior of bilayer films. We expect the shear-induced laning to be a generic feature of thin films with three or more layers.

cond-mat.soft↗

arXiv2016

Depinning and heterogeneous dynamics of colloidal crystal layers under shear flow

Using Brownian dynamics (BD) simulations and an analytical approach we investigate the shear-induced, nonequilibrium dynamics of dense colloidal suspensions confined to a narrow slit-pore. Focusing on situations where the colloids arrange in well-defined layers with solidlike in-plane structure, the confined films display complex, nonlinear behavior such as collective depinning and local transport via density excitations. These phenomena are reminiscent of colloidal monolayers driven over a periodic substrate potential. In order to deepen this connection, we present an effective model which maps the dynamics of the shear-driven colloidal layers to the motion of a single particle driven over an effective substrate potential. This model allows to estimate the critical shear rate of the depinning transition based on the equilibrium configuration, revealing the impact of important parameters such as the slit-pore width and the interaction strength. We then turn to heterogeneous systems where a layer of small colloids is sheared with respect to bottom layers of large particles. For these incommensurate systems we find that the particle transport is dominated by density excitations resembling the so-called "kink" solutions of the Frenkel-Kontorova (FK) model. In contrast to the FK model, however, the corresponding "antikinks" do not move.

cond-mat.soft↗

arXiv2016

Non-equilibrium surface growth in a hybrid inorganic-organic system

Using kinetic Monte Carlo simulations, we show that molecular morphologies found in non-equilibrium growth can be strongly different from those at equilibrium. We study the prototypical hybrid inorganic-organic system 6P on ZnO(10-10) during thin film adsorption, and find a wealth of phenomena including re-entrant growth, a critical adsorption rate and observables that are non-monotonous with the adsorption rate. We identify the transition from lying to standing molecules with a critical cluster size and discuss the competition of time scales during growth in terms of a rate equation approach. Our results form a basis for understanding and predicting collective orientational ordering during growth in hybrid material systems.

cond-mat.soft↗

arXiv2016

A minimal model for short-time diffusion in periodic potentials

We investigate the dynamics of a single, overdamped colloidal particle, which is driven by a constant force through a one-dimensional periodic potential. We focus on systems with large barrier heights where the lowest-order cumulants of the density field, that is, average position and the mean-squared displacement, show nontrivial (non-diffusive) short-time behavior characterized by the appearance of plateaus. We demonstrate that this "cage-like" dynamics can be well described by a discretized master equation model involving two states (related to two positions) within each potential valley. Non-trivial predictions of our approach include analytic expressions for the plateau heights and an estimate of the "de-caging time" obtained from the study of deviations from Gaussian behaviour. The simplicity of our approach means that it offers a minimal model to describe the short-time behavior of systems with hindered dynamics.

cond-mat.stat-mech↗

arXiv2016

Shear banding in nematogenic fluids with oscillating orientational dynamics

We investigate the occurrence of shear banding in nematogenic fluids under planar Couette flow, based on mesoscopic dynamical equations for the orientational order parameter and the shear stress. We focus on parameter values where the sheared homogeneous system exhibits regular oscillatory orientational dynamics, whereas the equilibrium system is either isotropic (albeit close to the isotropic--nematic transition) or deep in its nematic phase. The numerical calculations are restricted to spatial variations in shear gradient direction. We find several new types of shear banded states characterized by regions with regular oscillatory orientational dynamics. In all cases shear banding is accompanied by a non--monotonicity of the flow curve of the homogeneous system; however, only in the case of the initially isotropic system this curve has the typical $S$--like shape. We also analyze the influence of different orientational boundary conditions and of the spatial correlation length.

cond-mat.soft↗

arXiv2016

Angle-resolved effective potentials for disk-shaped molecules

We present an approach for calculating coarse-grained angle-resolved effective pair potentials for uniaxial molecules. For integrating out the intramolecular degrees of freedom we apply umbrella sampling and steered dynamics techniques in atomistically-resolved molecular dynamics (MD) computer simulations. Throughout this study we focus on disk-like molecules such as coronene. To develop the methods we focus on integrating out the van-der-Waals and intramolecular interactions, while electrostatic charge contributions are neglected. The resulting coarse-grained pair potential reveals a strong temperature and angle dependence. In the next step we fit the numerical data with various Gay-Berne-like potentials to be used in more efficient simulations on larger scales. The quality of the resulting coarse-grained results is evaluated by comparing their pair and many-body structure as well as some thermodynamic quantities self-consistently to the outcome of atomistic MD simulations of many-particle systems. We find that angle-resolved potentials are essential not only to accurately describe crystal structures but also for fluid systems where simple isotropic potentials start to fail already for low to moderate packing fractions. Further, in describing these states it is crucial to take into account the pronounced temperature dependence arising in selected pair configurations due to bending fluctuations.

cond-mat.soft↗

arXiv2016

Coarse-grained electrostatic interactions of coronene: Towards the crystalline phase

In this article we present and compare two different, coarse-grained approaches to model electrostatic interactions of disc-shaped aromatic molecules, specifically coronene. Our study builds on previous work [J. Chem. Phys. 141, 214110 (2014)] where we proposed, based on a systematic coarse-graining procedure starting from the atomistic level, an anisotropic effective (Gay-Berne-like) potential capable of describing van-der-Waals contributions to the interaction energy. To take into account electrostatics, we introduce, first, a linear quadrupole moment along the symmetry axis of the coronene disc. The second approach takes into account the fact that the partial charges within the molecules are distributed in a ring-like fashion. We then reparametrize the effective Gay-Berne-like potential such that it matches, at short distances, the ring-ring potential. To investigate the validity of these two approaches, we perform many-particle Molecular Dynamics (MD) simulations, focusing on the crystalline phase (karpatite) where electrostatic interaction effects are expected to be particularly relevant for the formation of tilted stacked columns. Specifically, we investigate various structural parameters as well as the melting transition. We find that the second approach yields consistent results with those from experiments despite the fact that the underlying potential decays with the wrong distance dependence at large molecule separations. Our strategy can be transferred to a broader class of molecules, such as benzene or hexabenzocoronene.

cond-mat.soft↗

arXiv2016

Equilibrium structures of anisometric, quadrupolar particles confined to a monolayer

We investigate the structural properties of a two-dimensional system of ellipsoidal particles carrying a linear quadrupole moment in their center. These particles represent a simple model for a variety of uncharged, non-polar conjugated organic molecules. Using optimization tools based on ideas of Evolutionary Algorithms, we first examine the ground state structures as we vary the aspect ratio of the particles and the pressure. Interestingly, we find, besides the intuitively expected T-like configurations, a variety of complex structures, characterized with up to three different particle orientations. In an effort to explore the impact of thermal fluctuations, we perform constant-pressure Molecular Dynamics simulations within a range of rather low temperatures. We observe that ground state structures formed by particles with a large aspect ratio are in particular suited to withstand fluctuations up to rather high temperatures. Our comprehensive investigations allow for a deeper understanding of molecular or colloidal monolayer arrangements under the influence of a typical electrostatic interaction on a coarse-grained level.

cond-mat.soft↗

arXiv2016

Collective dynamics of dipolar and multipolar colloids: from passive to active systems

This article reviews recent research on the collective dynamical behavior of colloids with dipolar or multipolar interactions. Indeed, whereas equilibrium structures and static self-assembly of such systems are now rather well understood, the past years have seen an explosion of interest in understanding dynamicals aspects, from the relaxation dynamics of strongly correlated dipolar networks over systems driven by time-dependent, electric or magnetic fields, to pattern formation and dynamical control of active, self-propelled systems. Unraveling the underlying mechanisms is crucial for a deeper understanding of self-assembly in and out of equilibrium and the use of such particles as functional devices. At the same time, the complex dynamics of dipolar colloids poses challenging physical questions and puts forward their role as model systems for nonlinear behavior in condensed matter physics. Here we attempt to give an overview of these developments, with an emphasis on theoretical and simulation studies.

cond-mat.soft↗

arXiv2015

Binary mixtures of rod-like colloids under shear: microscopically-based equilibrium theory and order--parameter dynamics

This paper is concerned with the dynamics of a binary mixture of rod--like, repulsive colloidal particles driven out of equilibrium by means of a steady shear flow (Couette geometry). To this end we first derive, starting from a microscopic density functional in Parsons--Lee approximation, a mesoscopic free energy functional whose main variables are the orientational order parameter tensors. Based on this mesoscopic functional we then explore the stability of isotropic and nematic equilibrium phases in terms of composition and rod lengths. Second, by combining the equilibrium theory with the Doi--Hess approach for the order parameter dynamics under shear, we investigate the orientational dynamics of binary mixtures for a range of shear rates and coupling parameters. We find a variety of dynamical states, including synchronized oscillatory states of the two components, but also symmetry breaking behavior where the components display different in--plane oscillatory states.

cond-mat.soft↗

arXiv2015

Self-assembly of three-dimensional ensembles of magnetic particles with laterally shifted dipoles

We consider a model of colloidal spherical particles carrying a permanent dipole moment which is laterally shifted out of the particles' geometrical centres, i.e. the dipole vector is oriented perpendicular to the radius vector of the particles. Varying the shift $δ$ from the centre, we analyze ground state structures for two, three and four hard spheres, using a simulated annealing procedure. We also compare to earlier ground state results. We then consider a bulk system at finite temperatures and different densities. Using Molecular Dynamics simulations, we examine the equilibrium self-assembly properties for several shifts. Our results show that the shift of the dipole moment has a crucial impact on both, the ground state configurations as well as the self-assembled structures at finite temperatures.

cond-mat.soft↗

arXiv2015

Hydrodynamic length-scale selection and effective viscosity in microswimmer suspensions

A universal characteristic of mesoscale turbulence in active suspensions is the emergence of a typical vortex length scale, distinctly different from the scale-invariance of turbulent high-Reynolds number flows. Collective length-scale selection has been observed in bacterial fluids, endothelial tissue and active colloides, yet the physical origins of this phenomenon remain elusive. Here, we systematically derive an effective fourth-order field theory from a generic microscopic model that allows us to predict the typical vortex size in microswimmer suspensions. Building on a self-consistent closure condition, the derivation shows that the vortex length scale is determined by the competition between local alignment forces and intermediate-range hydrodynamic interactions. Vortex structures found in simulations of the theory agree with recent measurements in Bacillus subtilis suspensions. Moreover, our approach correctly predicts an effective viscosity enhancement (reduction), as reported experimentally for puller (pusher) microorganisms.

cond-mat.soft↗

arXiv2015

Enhancement of mobility in an interacting colloidal system under feedback control

Feedback control schemes are a promising way to manipulate transport properties of driven colloidal suspensions. In the present article we suggest a feedback scheme to enhance the collective transport of colloidal particles with repulsive interactions through a one-dimensional tilted washboard potential. The control is modelled by a harmonic confining potential, mimicking an optical "trap", with the center of this trap moving with the (instantaneous) mean particle position. Our theoretical analysis is based on the Smoluchowski equation combined with Dynamical Density Functional Theory (DDFT) for systems with hard-core or ultra-soft (Gaussian) interactions. For either type of interaction we find that the feedback control can lead to an enhancement of the mobility by several orders of magnitude relative to the uncontrolled case. The largest effects occur for intermediate stiffness of the trap and large particle numbers. Moreover, in some regions of the parameter space the feedback control induces oscillations of the mean velocity. Finally, we show that the enhancement of mobility is robust against a small time delay in implementing the feedback control.

cond-mat.soft↗

arXiv2015

Generic model for tunable colloidal aggregation in multidirectional fields

Based on Brownian Dynamics computer simulations in two dimensions we investigate aggregation scenarios of colloidal particles with directional interactions induced by multiple external fields. To this end we propose a model which allows continuous change in the particle interactions from point-dipole-like to patchy-like (with four patches). We show that, as a result of this change, the non-equilibrium aggregation occurring at low densities and temperatures transforms from conventional diffusion-limited cluster aggregation (DLCA) to slippery DLCA involving rotating bonds; this is accompanied by a pronounced change of the underlying lattice structure of the aggregates from square-like to hexagonal ordering. Increasing the temperature we find a transformation to a fluid phase, consistent with results of a simple mean-field density functional theory.

cond-mat.soft↗

arXiv2015

Tunable structures of mixtures of magnetic particles in liquid-crystalline matrices

We investigate the self-organization of a binary mixture of similar sized rods and dipolar soft spheres by means of Monte-Carlo simulations. We model the interparticle interactions by employing anisotropic Gay-Berne, dipolar and soft-sphere interactions. In the limit of vanishing magnetic moments we obtain a variety of fully miscible liquid crystalline phases including nematic, smectic and lamellar phases. For the magnetic mixture, we find that the liquid crystalline matrix supports the formation of orientationally ordered ferromagnetic chains. Depending on the relative size of the species the chains align parallel or perpendicular to the director of the rods forming uniaxial or biaxial nematic, smectic and lamellar phases. As an exemplary external perturbation we apply a homogeneous magnetic field causing uniaxial or biaxial ordering to an otherwise isotropic state.

cond-mat.soft↗

arXiv2015

Spontaneous ordering of magnetic particles in liquid crystals: From chains to biaxial lamellae

Using Monte Carlo (MC) computer simulations we explore the self-assembly and ordering behavior of a hybrid, soft magnetic system consisting of small magnetic nano-spheres in a liquid-crystalline (LC) matrix. Inspired by recent experiments with colloidal rod-matrices we focus on conditions where the sphere and rod diameters are comparable. Already in the absence of a magnetic field, the nematic ordering of the LC can stabilize formation of magnetic chains along the nematic or smectic director, yielding a state with local (yet no macroscopic) magnetic order. The chains, in turn, increase the overall nematic order, reflecting the complex interplay of the structure formation of the two components. Increasing the sphere diameter the spontaneous uniaxial ordering is replaced by biaxial lamellar morphologies characterized by alternating layers of rods and magnetic chains oriented perpendicular to the rod's director. These novel ordering scenarios at zero field suggest complex response of the resulting hybrid to external stimuli such as magnetic fields and shear forces.

cond-mat.soft↗

arXiv2015

Lane formation in a system of dipolar microswimmers

Using Brownian Dynamics (BD) simulations we investigate the non-equilibrium structure formation of a two-dimensional (2D) binary system of dipolar colloids propelling in opposite directions. Despite of a pronounced tendency for chain formation, the system displays a transition towards a laned state reminiscent of lane formation in systems with isotropic repulsive interactions. However, the anisotropic dipolar interactions induce novel features: First, the lanes have themselves a complex internal structure characterized by chains or clusters. Second, laning occurs only in a window of interaction strengths. We interprete our findings by a phase separation process and simple force balance arguments.

cond-mat.soft↗