arXiv subjects

Annette Zippelius

Publications and source records attributed to Annette Zippelius.

At least 73 records · Page 4Linked to original sources

arXiv2006

Translations and Rotations are correlated in Granular Gases

In a granular gas of rough particles the axis of rotation is shown to be correlated with the translational velocity of the particles. The average relative orientation of angular and linear velocities depends on the parameters which characterise the dissipative nature of the collision. We derive a simple theory for these correlations and validate it with numerical simulations for a wide range of coefficients of normal and tangential restitution. The limit of smooth spheres is shown to be singular: even an arbitrarily small roughness of the particles gives rise to orientational correlations.

cond-mat.stat-mech↗

arXiv2006

Elasticity of highly cross-linked random networks

Starting from a microscopic model of randomly cross-linked particles with quenched disorder, we calculate the Laudau-Wilson free energy S for arbitrary cross-link densities. Considering pure shear deformations, S takes the form of the elastic energy of an isotropic amorphous solid state, from which the shear modulus can be identified. It is found to be an universal quantity, not depending on any microscopic length-scales of the model.

cond-mat.soft↗

arXiv2005

Glassy correlations and microstructures in randomly crosslinked homopolymer blends

We consider a microscopic model of a polymer blend that is prone to phase separation. Permanent crosslinks are introduced between randomly chosen pairs of monomers, drawn from the Deam-Edwards distribution. Thereby, not only density but also concentration fluctuations of the melt are quenched-in in the gel state, which emerges upon sufficient crosslinking. We derive a Landau expansion in terms of the order parameters for gelation and phase separation, and analyze it on the mean-field level, including Gaussian fluctuations. The mixed gel is characterized by thermal as well as time-persistent (glassy) concentration fluctuations. Whereas the former are independent of the preparation state, the latter reflect the concentration fluctuations at the instant of crosslinking, provided the mesh size is smaller than the correlation length of phase separation. The mixed gel becomes unstable to microphase separation upon lowering the temperature in the gel phase. Whereas the length scale of microphase separation is given by the mesh size, at least close to the transition, the emergent microstructure depends on the composition and compressibility of the melt. Hexagonal structures, as well as lamellae or random structures with a unique wavelength, can be energetically favorable.

cond-mat.soft↗

arXiv2005

Heterogeneities in the Glassy State

We study heterogeneities in a binary Lennard-Jones system below the glass transition using molecular dynamics simulations. We identify mobile and immobile particles and measure their distribution of vibrational amplitudes. For temperatures near the glass transition the distribution of vibrational amplitudes obeys scaling and compares reasonably well with a mean field theory for the amorphous solid state. To investigate correlations among the immobile and mobile particles we identify clusters and analyze their size and shape. For a fixed number of immobile particles we observe that the immobile particles cluster more strongly together as the temperature is increased which allows the particles to block each other more effectively, and to therefore stay immobile. For the mobile particles, on the other hand, the clustering is most pronounced at small temperatures, indicating that mobility at low temperatures can only be sustained in cooperative motion.

cond-mat.dis-nn↗

arXiv2005

A driven two-dimensional granular gas with Coulomb friction

We study a homogeneously driven granular gas of inelastic hard particles with rough surfaces subject to Coulomb friction. The stationary state as well as the full dynamic evolution of the translational and rotational granular temperatures are investigated as a function of the three parameters of the friction model. Four levels of approximation to the (velocity-dependent) tangential restitution are introduced and used to calculate translational and rotational temperatures in a mean field theory. When comparing these theoretical results to numerical simulations of a randomly driven mono-layer of particles subject to Coulomb friction, we find that already the simplest model leads to qualitative agreement, but only the full Coulomb friction model is able to reproduce/predict the simulation results quantitatively for all magnitudes of friction. In addition, the theory predicts two relaxation times for the decay to the stationary state. One of them corresponds to the equilibration between the translational and rotational degrees of freedom. The other one, which is slower in most cases, is the inverse of the common relaxation rate of translational and rotational temperatures.

cond-mat.soft↗

arXiv2004

Dynamics of gelling liquids: a short survey

The dynamics of randomly crosslinked liquids is addressed via a Rouse- and a Zimm-type model with crosslink statistics taken either from bond percolation or Erdoes-Renyi random graphs. While the Rouse-type model isolates the effects of the random connectivity on the dynamics of molecular clusters, the Zimm-type model also accounts for hydrodynamic interactions on a preaveraged level. The incoherent intermediate scattering function is computed in thermal equilibrium, its critical behaviour near the sol-gel transition is analysed and related to the scaling of cluster diffusion constants at the critical point. Second, non-equilibrium dynamics is studied by looking at stress relaxation in a simple shear flow. Anomalous stress relaxation and critical rheological properties are derived. Some of the results contradict long-standing scaling arguments, which are shown to be flawed by inconsistencies.

cond-mat.soft↗

arXiv2004

Local heat flux and energy loss in a 2D vibrated granular gas

We performed event-driven simulations of a two-dimensional granular gas between two vibrating walls and directly measured the local heat flux and energy dissipation rate in the stationary state. Describing the local heat flux as a function of the coordinate x in the direction perpendicular to the driving walls, we use a generalization of Fourier's law, q_x(x) = kappa d_x T(x) + mu d_x rho(x), to relate the local heat flux to the local gradients of the temperature and density. This ansatz accounts for the fact that density gradients also generate heat flux, not only temperature gradients. The transport coefficients kappa and mu are assumed to be independent of x, and we check the validity of this assumption in the simulations. Both kappa and mu are determined for different system parameters, in particular, for a wide range of coefficients of restitution. We also compare our numerical results to existing hydrodynamic theories. Agreement is found for kappa for very small inelasticities only. Beyond this region, kappa and mu exhibit a striking non-monotonic behavior.

cond-mat.stat-mech↗

arXiv2004

From Vulcanization to Isotropic and Nematic Rubber Elasticity

A Landau theory is constructed for the vulcanization transition in cross-linked polymer systems with spontaneous nematic ordering. The neo-classical theory of the elasticity of nematic elastomers is derived via the minimization of this Landau free energy; this neo-classical theory contains the classical theory of rubber elasticity as its isotropic limit. Our work not only reveals the statistical-mechanical roots of these elasticity theories, but also demonstrates that they are applicable to a wide class of random solids. It also constitutes a starting-point for the investigation of sample-to-sample fluctuations in various forms of vulcanized matter.

cond-mat.soft↗

arXiv2004

Glassy states and microphase separation in cross-linked homopolymer blends

The physical properties of blends of distinct homopolymers, cross-linked beyond the gelation point, are addressed via a Landau approach involving a pair of coupled order-parameter fields: one describing vulcanisation, the other describing local phase separation. Thermal concentration fluctuations, present at the time of cross-linking, are frozen in by cross-linking, and the structure of the resulting glassy fluctuations is analysed at the Gaussian level in various regimes, determined by the relative values of certain physical length-scales. The enhancement, due to gelation, of the stability of the blend with respect to demixing is also analysed. Beyond the corresponding stability limit, gelation prevents complete demixing, replacing it by microphase separation, which occurs up to a length-scale set by the rigidity of the network, as a simple variational scheme reveals.

cond-mat.soft↗

arXiv2004

Rheology of gelling polymers in the Zimm model

In order to study rheological properties of gelling systems in dilute solution, we investigate the viscosity and the normal stresses in the Zimm model for randomly crosslinked monomers. The distribution of cluster topologies and sizes is assumed to be given either by Erd\H os-Rényi random graphs or three-dimensional bond percolation. Within this model the critical behaviour of the viscosity and of the first normal stress coefficient is determined by the power-law scaling of their averages over clusters of a given size $n$ with $n$. We investigate these Mark--Houwink like scaling relations numerically and conclude that the scaling exponents are independent of the hydrodynamic interaction strength. The numerically determined exponents agree well with experimental data for branched polymers. However, we show that this traditional model of polymer physics is not able to yield a critical divergence at the gel point of the viscosity for a polydisperse dilute solution of gelation clusters. A generally accepted scaling relation for the Zimm exponent of the viscosity is thereby disproved.

cond-mat.soft↗

arXiv2004

Local Equation of State and Velocity Distributions of a Driven Granular Gas

We present event-driven simulations of a granular gas of inelastic hard disks with incomplete normal restitution in two dimensions between vibrating walls (without gravity). We measure hydrodynamic quantities such as the stress tensor, density and temperature profiles, as well as velocity distributions. Relating the local pressure to the local temperature and local density, we construct a local constitutive equation. For strong inelasticities the local constitutive relation depends on global system parameters, like the volume fraction and the aspect ratio. For moderate inelasticities the constitutive relation is approximately independent of the system parameters and can hence be regarded as a local equation of state, even though the system is highly inhomogeneous with heterogeneous temperature and density profiles arising as a consequence of the energy injection. Concerning the local velocity distributions we find that they do not scale with the square root of the local granular temperature. Moreover the high-velocity tails are different for the distribution of the x- and the y-component of the velocity, and even depend on the position in the sample, the global volume fraction, and the coefficient of restitution.

cond-mat.stat-mech↗

arXiv2004

Goldstone-type fluctuations and their implications for the amorphous solid state

In sufficiently high spatial dimensions, the formation of the amorphous (i.e. random) solid state of matter, e.g., upon sufficent crosslinking of a macromolecular fluid, involves particle localization and, concommitantly, the spontaneous breakdown of the (global, continuous) symmetry of translations. Correspondingly, the state supports Goldstone-type low energy, long wave-length fluctuations, the structure and implications of which are identified and explored from the perspective of an appropriate replica field theory. In terms of this replica perspective, the lost symmetry is that of relative translations of the replicas; common translations remain as intact symmetries, reflecting the statistical homogeneity of the amorphous solid state. What emerges is a picture of the Goldstone-type fluctuations of the amorphous solid state as shear deformations of an elastic medium, along with a derivation of the shear modulus and the elastic free energy of the state. The consequences of these fluctuations -- which dominate deep inside the amorphous solid state -- for the order parameter of the amorphous solid state are ascertained and interpreted in terms of their impact on the statistical distribution of localization lengths, a central diagnostic of the the state. The correlations of these order parameter fluctuations are also determined, and are shown to contain information concerning further diagnostics of the amorphous solid state, such as spatial correlations in the statistics of the localization characteristics. Special attention is paid to the properties of the amorphous solid state in two spatial dimensions, for which it is shown that Goldstone-type fluctuations destroy particle localization, the order parameter is driven to zero, and power-law order-parameter correlations hold.

cond-mat.dis-nn↗

arXiv2003

Goldstone fluctuations in the amorphous solid state

Goldstone modes in the amorphous solid state, resulting from the spontaneous breaking of translational symmetry due to random localisation of particles, are discussed. Starting from a microscopic model with quenched disorder, the broken symmetry is identified to be that of relative translations of the replicas. Goldstone excitations, corresponding to pure shear deformations, are constructed from long wavelength distortions of the order parameter. The elastic free energy is computed, and it is shown that Goldstone fluctuations destroy localisation in two spatial dimensions, yielding a two-dimensional amorphous solid state characterised by power-law correlations.

cond-mat.soft↗

arXiv2003

Diffusion of gelation clusters in the Zimm model

Starting from a Zimm model we study selfdiffusion in a solution of crosslinked monomers. We focus on the effects of the hydrodynamic interaction on the dynamics and the critical behaviour at the sol-gel-point. Hydrodynamic interactions cause the clusters' diffusion constant to depend not only on the cluster's size but also on the cluster's shape -- in contrast to the Rouse model. This gives rise to a nontrivial scaling of the Kirkwood diffusion constant averaged over all clusters of fixed size $n$, ${\hat D}_n\sim n^{-{\hat b}}$ with ${\hat b}=1/d_s-1/2$ given in terms of the spectral dimension $d_s$ of critical percolation clusters. The long-time decay of the incoherent scattering function is determined by the diffusive motion of the largest clusters. This implies the critical vanishing $D_{\rm eff}\sim ε^a$ of the cluster-averaged effective diffusion constant at the gel point with exponent $a = (3/2 -τ+1/d_{s})/σ$.

cond-mat.stat-mech↗

arXiv2002

Towards finite-dimensional gelation

We consider the gelation of particles which are permanently connected by random crosslinks, drawn from an ensemble of finite-dimensional continuum percolation. To average over the randomness, we apply the replica trick, and interpret the replicated and crosslink-averaged model as an effective molecular fluid. A Mayer-cluster expansion for moments of the local static density fluctuations is set up. The simplest non-trivial contribution to this series leads back to mean-field theory. The central quantity of mean-field theory is the distribution of localization lengths, which we compute for all connectivities. The highly crosslinked gel is characterized by a one-to-one correspondence of connectivity and localization length. Taking into account higher contributions in the Mayer-cluster expansion, systematic corrections to mean-field can be included. The sol-gel transition shifts to a higher number of crosslinks per particle, as more compact structures are favored. The critical behavior of the model remains unchanged as long as finite truncations of the cluster expansion are considered. To complete the picture, we also discuss various geometrical properties of the crosslink network, e.g. connectivity correlations, and relate the studied crosslink ensemble to a wider class of ensembles, including the Deam-Edwards distribution.

cond-mat.soft↗

arXiv2001

Normal stresses at the gelation transition

A simple Rouse-type model, generalised to incorporate the effects of chemical crosslinks, is used to obtain a theoretical prediction for the critical behaviour of the normal-stress coefficients $Ψ_{1}$ and $Ψ_{2}$ at the gelation transition. While the exact calculation shows $Ψ_{2}\equiv 0$, a typical result for these types of models, an additional scaling ansatz is used to demonstrate that $Ψ_{1}$ diverges with a critical exponent $\ell = k+z$. Here, $k$ denotes the critical exponent of the shear viscosity and $z$ the exponent governing the divergence of the time scale in the Kohlrausch decay of the shear-stress relaxation function. For crosslinks distributed according to mean-field percolation, this scaling relation yields $\ell =3$, in a accordance with an exact expression for the first normal-stress coefficient based on a replica calculation. Alternatively, using three-dimensional percolation for the crosslink ensemble we find the value $\ell \approx 4.9$. Results on time-dependent normal-stress response are also presented.

cond-mat.stat-mech↗

arXiv2001

Dynamical Heterogeneities Below the Glass Transition

We present molecular dynamics simulations of a binary Lennard-Jones mixture at temperatures below the kinetic glass transition. The ``mobility'' of a particle is characterized by the amplitude of its fluctuation around its average position. The 5% particles with the largest/smallest mean amplitude are thus defined as the relatively most mobile/immobile particles. We investigate for these 5% particles their spatial distribution and find them to be distributed very heterogeneously in that mobile as well as immobile particles form clusters. The reason for this dynamic heterogeneity is traced back to the fact that mobile/immobile particles are surrounded by fewer/more neighbors which form an effectively wider/narrower cage. The dependence of our results on the length of the simulation run indicates that individual particles have a characteristic mobility time scale, which can be approximated via the non-Gaussian parameter.

cond-mat.stat-mech↗

arXiv2001

Anomalous stress relaxation in random macromolecular networks

Within the framework of a simple Rouse-type model we present exact analytical results for dynamical critical behaviour on the sol side of the gelation transition. The stress-relaxation function is shown to exhibit a stretched-exponential long-time decay. The divergence of the static shear viscosity is governed by the critical exponent $k=ϕ-β$, where $ϕ$ is the (first) crossover exponent of random resistor networks, and $β$ is the critical exponent for the gel fraction. We also derive new results on the behaviour of normal stress coefficients.

cond-mat.stat-mech↗