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Burkhard Duenweg

Publications and source records attributed to Burkhard Duenweg.

At least 19 recordsLinked to original sources

Fundamentals of the Oldroyd-B model revisited: Tensorial vs. vectorial theory

The standard derivation of the Oldroyd-B model starts from a coupled system of the momentum equation for the macroscopic flow on the one hand, and Fokker-Planck dynamics for molecular dumbbells on the other. The constitutive equation is then derived via a closure based upon the second moment of the end-to-end vector distribution. We here present an alternative closure that is rather based upon the first moment, and gives rise to an even simpler constitutive equation. We establish that both closures are physically sound, since both can be derived from (different) well-defined non-equilibrium ensembles, and both are consistent with the Second Law of thermodynamics. In contrast to the standard model, the new model has a free energy and a dissipation rate that are both regular at vanishing conformation tensor. We speculate that this might perhaps alleviate the well-known high Weissenberg number problem, i. e. severe numerical instabilities of the standard model at large flow rates. As the new model permits a trivial solution (vanishing conformation tensor, vanishing polymer stress), an extension may be needed, which includes Langevin noise in order to model thermal fluctuations.

cond-mat.soft

Systematic derivation of hydrodynamic equations for viscoelastic phase separation

(abridged) We present a detailed derivation of a simple hydrodynamic two-fluid model, which aims at the description of the phase separation of non-entangled polymer solutions, where viscoelastic effects play a role. It is directly based upon the coarse-graining of a well-defined molecular model, such that all degrees of freedom have a clear and unambiguous molecular interpretation. The considerations are based upon a free-energy functional, and the dynamics is split into a conservative and a dissipative part, where the latter satisfies the Onsager relations and the Second Law of thermodynamics. The model is therefore fully consistent with both equilibrium and non-equilibrium thermodynamics. The derivation proceeds in two steps: Firstly, we derive an extended model comprising two scalar and four vector fields, such that inertial dynamics of the macromolecules and of the relative motion of the two fluids is taken into account. In the second step, we eliminate these inertial contributions and, as a replacement, introduce phenomenological dissipative terms, which can be modeled easily by taking into account the principles of non-equilibrium thermodynamics. The final simplified model comprises the momentum conservation equation, which includes both interfacial and elastic stresses, a convection-diffusion equation where interfacial and elastic contributions occur as well, and a suitably convected relaxation equation for the end-to-end vector field. In contrast to the traditional two-scale description that is used to derive rheological equations of motion, we here treat the hydrodynamic and the macromolecular degrees of freedom on the same basis. Nevertheless, the resulting model is fairly similar, though not fully identical, to models that have been discussed previously. Notably, we find a rheological constitutive equation that differs from the standard Oldroyd-B model. ...

cond-mat.soft

Semi-automatic construction of Lattice Boltzmann models

A crucial step in constructing a Lattice Boltzmann model is the definition of a suitable set of lattice velocities, and the correct assignment of the associated weights. For high-order models, the solution of this problem requires a non-trivial effort. The paper outlines the functioning of a publicly available Python script which has been written to assist researchers in that task. The speed of sound $c_s$ is considered as a parameter, which can, within limits, be chosen at will. Under this premise, the Maxwell-Boltzmann constraint equations are a system of linear equations to determine the weights, and hence amenable to numerical solution by standard linear algebra library routines. By suitable contractions, the tensor equations are mapped to a set of equivalent scalar equations, which simplifies the treatment significantly. For a user-supplied set of velocity shells, the software first checks if a solution for the weights exists, and returns it if it also happens to be unique. In such a case, the software also calculates the range of $c_s$ values that yield positive weights. Standard models like D3Q19 with a well-defined special $c_s$ value then result as limiting cases where one of the weights vanishes. In case of an infinite set of solutions, the user may find one particular solution by supplying a $c_s$ value, and then minimizing one or several weights within the framework of standard linear programming. Some examples illustrate the feasibility and usefulness of the approach. A number of models that have been discussed in the literature are nicely reproduced, while the software has also been able to find some new models of even higher order.

physics.comp-ph

High-precision estimate of the hydrodynamic radius for self-avoiding walks

The universal asymptotic amplitude ratio between the gyration radius and the hydrodynamic radius of self-avoiding walks is estimated by high-resolution Monte Carlo simulations. By studying chains of length of up to $N = 2^{25} \approx 34 \times 10^6$ monomers, we find that the ratio takes the value $R_{\mathrm{G}}/R_{\mathrm{H}} = 1.5803940(45)$, which is several orders of magnitude more accurate than the previous state of the art. This is facilitated by a sampling scheme which is quite general, and which allows for the efficient estimation of averages of a large class of observables. The competing corrections to scaling for the hydrodynamic radius are clearly discernible. We also find improved estimates for other universal properties that measure the chain dimension. In particular, a method of analysis which eliminates the leading correction to scaling results in a highly accurate estimate for the Flory exponent of $ν= 0.58759700(40)$.

cond-mat.stat-mech

Polymer Solutions

The article provides a brief general introduction into the concepts of scaling, universality, and crossover scaling, plus the blob concept that provides an intuitive picture of crossover phenomena. We present the most important static and dynamic scaling laws for unentangled uncharged polymer solutions, together with their test and refinement by careful computer simulations. A hoard of simulation methods has been developed for these systems, and these will be briefly discussed as well.

cond-mat.soft

Consistent two-phase Lattice Boltzmann model for gas-liquid systems

A new lattice Boltzmann method for simulating multiphase flows is developed theoretically. The method is adjusted such that its continuum limit is the Navier-Stokes equation, with a driving force derived from the Cahn-Hilliard free energy. In contrast to previous work, however, the bulk and interface terms are decoupled, the former being incorporated into the model through the local equilibrium populations, and the latter through a forcing term. We focus on gas-liquid phase equilibria with the possibility to implement an arbitrary equation of state. The most novel aspect of our approach is a systematic Chapman-Enskog expansion up to the third order. Due to the third-order gradient in the interface forcing term, this is needed for full consistency with both hydrodynamics and thermodynamics. Our construction of a model that satisfies all conditions is based upon previous work by Chen, Goldhirsch, and Orszag (J. Sci. Comp. 34, 87 (2008)), and implies 59 and 21 velocities in three and two dimensions, respectively. Applying the conditions of positivity of weights, existence of a two-phase region in the phase diagram, and positivity of the bulk viscosity, we find substantial restrictions on the permitted equation of state, which can only be lifted by an even more refined model. Moreover, it turns out that it is necessary to solve a self-consistent equation for the hydrodynamic flow velocity, in order to enforce the identity of momentum density and mass current on the lattice. The analysis completely identifies all spurious terms in the Navier-Stokes equation, and thus shows how to systematically eliminate each of them, by constructing a suitable collision operator. (continued - see article PDF)

cond-mat.stat-mech

Collapse dynamics of copolymers in a poor solvent: Influence of hydrodynamic interactions and chain sequence

We investigate the dynamics of the collapse of a single copolymer chain, when the solvent quality is suddenly quenched from good to poor. We employ Brownian dynamics simulations of a bead-spring chain model and incorporate fluctuating hydrodynamic interactions via the Rotne-Prager-Yamakawa tensor. Various copolymer architectures are studied within the framework of a two-letter HP model, where monomers of type H (hydrophobic) attract each other, while all interactions involving P (polar or hydrophilic) monomers are purely repulsive. The hydrodynamic interactions are found to assist the collapse. Furthermore, the chain sequence has a strong influence on the kinetics and on the compactness and energy of the final state. The dynamics is typically characterised by initial rapid cluster formation, followed by coalescence and final rearrangement to form the compact globule. The coalescence stage takes most of the collapse time, and its duration is particularly sensitive to the details of the architecture. Long blocks of type P are identified as the main bottlenecks to find the globular state rapidly.

cond-mat.soft

Implicit and explicit solvent models for the simulation of a single polymer chain in solution: Lattice Boltzmann vs Brownian dynamics

We present a comparative study of two computer simulation methods to obtain static and dynamic properties of dilute polymer solutions. The first approach is a recently established hybrid algorithm based upon dissipative coupling between Molecular Dynamics and lattice Boltzmann (LB), while the second is standard Brownian Dynamics (BD) with fluctuating hydrodynamic interactions. Applying these methods to the same physical system (a single polymer chain in a good solvent in thermal equilibrium) allows us to draw a detailed and quantitative comparison in terms of both accuracy and efficiency. It is found that the static conformations of the LB model are distorted when the box length L is too small compared to the chain size. Furthermore, some dynamic properties of the LB model are subject to an $L^{-1}$ finite size effect, while the BD model directly reproduces the asymptotic $L \to \infty$ behavior. Apart from these finite size effects, it is also found that in order to obtain the correct dynamic properties for the LB simulations, it is crucial to properly thermalize all the kinetic modes. Only in this case, the results are in excellent agreement with each other, as expected. Moreover, Brownian Dynamics is found to be much more efficient than lattice Boltzmann as long as the degree of polymerization is not excessively large.

cond-mat.soft

Multiscale modelling strategy using the lattice Boltzmann method for polymer dynamics in a turbulent flow

Polymer dynamics in a turbulent flow is a problem spanning several orders of magnitude of length and time scales. A microscopic simulation covering all those scales from the polymer segment to the inertial scale of turbulence seems impossible within the foreseeable future. We propose a multiscale simulation strategy to enhance the spatio-temporal resolution of local Lagrangian turbulent flow by matching two different simulation techniques, i. e. direct numerical simulation for the flow as a whole, and the lattice Boltzmann method coupled to polymer dynamics at the Kolmogorov dissipation scale. Local turbulent flows sampled by Lagrangian tracer particles in the direct numerical simulation are reproduced in the lattice Boltzmann model with a finer resolution, by supplying the latter with both the correct initial condition as well as the correct time-dependent boundary condition, sampled from the former. When combined with a Molecular Dynamics simulation of a polymer chain in the lattice Boltzmann model, it provides a strategy to simulate the \emph{passive} dynamics of a polymer chain in a turbulent flow covering all those scales. While this approach allows for a fairly realistic model of the macromolecule, the back-coupling to the flow on the large scales is missing.

cond-mat.stat-mech

Lattice Boltzmann simulations of soft matter systems

This article concerns numerical simulations of the dynamics of particles immersed in a continuum solvent. As prototypical systems, we consider colloidal dispersions of spherical particles and solutions of uncharged polymers. After a brief explanation of the concept of hydrodynamic interactions, we give a general overview over the various simulation methods that have been developed to cope with the resulting computational problems. We then focus on the approach we have developed, which couples a system of particles to a lattice Boltzmann model representing the solvent degrees of freedom. The standard D3Q19 lattice Boltzmann model is derived and explained in depth, followed by a detailed discussion of complementary methods for the coupling of solvent and solute. Colloidal dispersions are best described in terms of extended particles with appropriate boundary conditions at the surfaces, while particles with internal degrees of freedom are easier to simulate as an arrangement of mass points with frictional coupling to the solvent. In both cases, particular care has been taken to simulate thermal fluctuations in a consistent way. The usefulness of this methodology is illustrated by studies from our own research, where the dynamics of colloidal and polymeric systems has been investigated in both equilibrium and nonequilibrium situations.

cond-mat.soft

Statistical Mechanics of the Fluctuating Lattice Boltzmann Equation

We propose a new formulation of the fluctuating lattice Boltzmann equation that is consistent with both equilibrium statististical mechanics and fluctuating hydrodynamics. The formalism is based on a generalized lattice-gas model, with each velocity direction occupied by many particles. We show that the most probable state of this model corresponds to the usual equilibrium distribution of the lattice Boltzmann equation. Thermal fluctuations about this equilibrium are controlled by the mean number of particles at a lattice site. Stochastic collision rules are described by a Monte Carlo process satisfying detailed balance. This allows for a straightforward derivation of discrete Langevin equations for the fluctuating modes. It is shown that all non-conserved modes should be thermalized, as first pointed out by Adhikari et al.; any other choice violates the condition of detailed balance. A Chapman-Enskog analysis is used to derive the equations of fluctuating hydrodynamics on large length and time scales; the level of fluctuations is shown to be thermodynamically consistent with the equation of state of an isothermal, ideal gas. We believe this formalism will be useful in developing new algorithms for thermal and multiphase flows.

cond-mat.soft

Electrophoresis of colloidal dispersions in the low-salt regime

We study the electrophoretic mobility of spherical charged colloids in a low-salt suspension as a function of the colloidal concentration. Using an effective particle charge and a reduced screening parameter, we map the data for systems with different particle charges and sizes, including numerical simulation data with full electrostatics and hydrodynamics and experimental data for latex dispersions, on a single master curve. We observe two different volume fraction-dependent regimes for the electrophoretic mobility that can be explained in terms of the static properties of the ionic double layer.

cond-mat.soft

Non-Fickian Interdiffusion of Dynamically Asymmetric Species: A Molecular Dynamics Study

We use Molecular Dynamics combined with Dissipative Particle Dynamics to construct a model of a binary mixture where the two species differ only in their dynamic properties (friction coefficients). For an asymmetric mixture of slow and fast particles we study the interdiffusion process. The relaxation of the composition profile is investigated in terms of its Fourier coefficients. While for weak asymmetry we observe Fickian behavior, a strongly asymmetric system exhibits clear indications of anomalous diffusion, which occurs in a crossover region between the Cases I (Fickian) and II (sharp front moving with constant velocity), and is close to the Case II limit.

cond-mat.soft

Electrophoretic mobility of a charged colloidal particle: A computer simulation study

We study the mobility of a charged colloidal particle in a constant homogeneous electric field by means of computer simulations. The simulation method combines a lattice Boltzmann scheme for the fluid with standard Langevin dynamics for the colloidal particle, which is built up from a net of bonded particles forming the surface of the colloid. The coupling between the two subsystems is introduced via friction forces. In addition explicit counterions, also coupled to the fluid, are present. We observe a non-monotonous dependence of the electrophoretic mobility on the bare colloidal charge. At low surface charge density we observe a linear increase of the mobility with bare charge, whereas at higher charges, where more than half of the ions are co-moving with the colloid, the mobility decreases with increasing bare charge.

cond-mat.soft

Coulomb Interactions via Local Dynamics: A Molecular--Dynamics Algorithm

We derive and describe in detail a recently proposed method for obtaining Coulomb interactions as the potential of mean force between charges which are dynamically coupled to a local electromagnetic field. We focus on the Molecular Dynamics version of the method and show that it is intimately related to the Car--Parrinello approach, while being equivalent to solving Maxwell's equations with freely adjustable speed of light. Unphysical self--energies arise as a result of the lattice interpolation of charges, and are corrected by a subtraction scheme based on the exact lattice Green's function. The method can be straightforwardly parallelized using standard domain decomposition. Some preliminary benchmark results are presented.

cond-mat.stat-mech

A new model for simulating colloidal dynamics

We present a new hybrid lattice-Boltzmann and Langevin molecular dynamics scheme for simulating the dynamics of suspensions of spherical colloidal particles. The solvent is modeled on the level of the lattice-Boltzmann method while the molecular dynamics is done for the solute. The coupling between the two is implemented through a frictional force acting both on the solvent and on the solute, which depends on the relative velocity. A spherical colloidal particle is represented by interaction sites at its surface. We demonstrate that this scheme quantitatively reproduces the translational and rotational diffusion of a neutral spherical particle in a liquid and show preliminary results for a charged spherical particle. We argue that this method is especially advantageous in the case of charged colloids.

cond-mat.soft

Translational Diffusion of Polymer Chains with Excluded Volume and Hydrodynamic Interactions by Brownian Dynamics Simulation

Within Kirkwood theory, we study the translational diffusion coefficient of a single polymer chain in dilute solution, and focus on the small difference between the short--time Kirkwood value $D^{(K)}$ and the asymptotic long--time value $D$. We calculate this correction term by highly accurate large--scale Brownian Dynamics simulations, and show that it is in perfect agreement with the rigorous variational result $D < D^{(K)}$, and with Fixman's Green--Kubo formula, which is re--derived. This resolves the puzzle posed by earlier numerical results (Rey {\em et al.}, Macromolecules 24, 4666 (1991)), which rather seemed to indicate $D > D^{(K)}$; the older data are shown to have insufficient statistical accuracy to resolve this question. We then discuss the Green--Kubo integrand in some detail. This function behaves very differently for pre--averaged vs. fluctuating hydrodynamics, as shown for the initial value by analytical considerations corroborated by numerical results. We also present further numerical data on the chain's statics and dynamics.

cond-mat.soft