arXiv subjects

Matthias Fuchs

Publications and source records attributed to Matthias Fuchs.

At least 55 records · Page 3Linked to original sources

arXiv2015

Shear-thinning in dense colloidal suspensions and its effect on elastic instabilities: from the microscopic equations of motion to an approximation of the macroscopic rheology

In the vicinity of their glass transition, dense colloidal suspensions acquire elastic properties over experimental timescales. We investigate the possibility of a visco-elastic flow instability in curved geometry for such materials. To this end, we first present a general strategy extending a first-principles approach based on projections onto slow variables (so far restricted to strictly homogeneous flow) in order to handle inhomogeneities. In particular, we separate the advection of the microstructure by the flow, at the origin of a fluctuation advection term, from the intrinsic dynamics. On account of the complexity of the involved equations, we then opt for a drastic simplification of the theory, in order to establish its potential to describe instabilities. These very strong approximations lead to a constitutive equation of the White-Metzner class, whose parameters are fitted with experimental measurements of the macroscopic rheology of a glass-forming colloidal dispersion. The model properly accounts for the shear-thinning properties of the dispersions, but, owing to the approximations, the description is not fully quantitative. Finally, we perform a linear stability analysis of the flow in the experimentally relevant cylindrical (Taylor-Couette) geometry and provide evidence that shear-thinning strongly stabilises the flow, which can explain why visco-elastic instabilities are not observed in dense colloidal suspensions.

cond-mat.soft↗

arXiv2015

On the coarse-grained density and compressibility of a non-ideal crystal

The isothermal compressibility of a general crystal is derived and discussed within (classical) density functional theory. Starting from the microscopic particle density, we carefully coarse grain to obtain the thermodynamic compressibility and the long wavelength limits of the correlation functions of elasticity theory. We explicitly show that the isothermal compressibility is not the wavevector to zero limit of the (total) density correlation function. The latter also cannot be obtained from the static structure factor measured in a scattering experiment.

cond-mat.soft↗

arXiv2015

On the coarse-grained density and compressibility of non-ideal crystals: general theory and an application to cluster crystals

The isothermal compressibility of a general crystal is analyzed within classical density functional theory. Our approach can be used for homogeneous and unstrained crystals containing an arbitrarily high density of local defects. We start by coarse-graining the microscopic particle density and then obtain the long wavelength limits of the correlation functions of elasticity theory and the thermodynamic derivatives. We explicitly show that the long wavelength limit of the microscopic density correlation function differs from the isothermal compressibility. It also cannot be obtained from the static structure factor measured in a scattering experiment. We apply our theory to crystals consisting of soft particles which can multiply occupy lattice sites ('cluster crystals'). The multiple occupancy results in a strong local disorder over an extended range of temperatures. We determine the cluster crystals' isothermal compressibility, the fluctuations of the lattice occupation numbers and their correlation functions, and the dispersion relations. We also discuss their low-temperature phase diagram.

cond-mat.soft↗

arXiv2015

Nonlinear X-ray Compton Scattering

X-ray scattering is a weak linear probe of matter. It is primarily sensitive to the position of electrons and their momentum distribution. Elastic X-ray scattering forms the basis of atomic structural determination while inelastic Compton scattering is often used as a spectroscopic probe of both single-particle excitations and collective modes. X-ray free-electron lasers (XFELs) are unique tools for studying matter on its natural time and length scales due to their bright and coherent ultrashort pulses. However, in the focus of an XFEL the assumption of a weak linear probe breaks down, and nonlinear light-matter interactions can become ubiquitous. The field can be sufficiently high that even non-resonant multiphoton interactions at hard X-rays wavelengths become relevant. Here we report the observation of one of the most fundamental nonlinear X-ray-matter interactions, the simultaneous Compton scattering of two identical photons producing a single photon at nearly twice the photon energy. We measure scattered photons with an energy near 18 keV generated from solid beryllium irradiated by 8.8-9.75 keV XFEL pulses. The intensity in the X-ray focus reaches up to 4x20 W/cm2, which corresponds to a peak electric field two orders of magnitude higher than the atomic unit of field-strength and within four orders of magnitude of the quantum electrodynamic critical field. The observed signal scales quadratically in intensity and is emitted into a non-dipolar pattern, consistent with the simultaneous two-photon scattering from free electrons. However, the energy of the generated photons shows an anomalously large redshift only present at high intensities. This indicates that the instantaneous high-intensity scattering effectively interacts with a different electron momentum distribution than linear Compton scattering, with implications for the study of atomic-scale structure and dynamics of matter

physics.optics↗

arXiv2014

Transient stress evolution in repulsion and attraction dominated glasses

We present results from microscopic mode coupling theory generalized to colloidal dispersions under shear in an integration-through-transients formalism. Stress-strain curves in start-up shear, flow curves, and normal stresses are calculated with the equilibrium static structure factor as only input. Hard spheres close to their glass transition are considered, as are hard spheres with a short-ranged square-well attraction at their attraction dominated glass transition. The consequences of steric packing and physical bond formation on the linear elastic response, the stress release during yielding, and the steady plastic flow are discussed and compared to experimental data from concentrated model dispersions.

cond-mat.soft↗

arXiv2013

Nonlinear microrheology of dense colloidal suspensions: a mode-coupling theory

A mode-coupling theory for the motion of a strongly forced probe particle in a dense colloidal suspension is presented. Starting point is the Smoluchowski equation for $N$ bath and a single probe particle. The probe performs Brownian motion under the influence of a strong constant and uniform external force $\Fex$. It is immersed in a dense homogeneous bath of (different) particles also performing Brownian motion. Fluid and glass states are considered; solvent flow effects are neglected. Based on a formally exact generalized Green-Kubo relation, mode coupling approximations are performed and an integration through transients approach applied. A first-principles theory for the nonlinear velocity-force relations of the probe particle in a dense fluid and for the (de-) localized probe in a glass is obtained. It extends the mode coupling theory of the glass transition to strongly forced tracer motion and describes active microrheology experiments. A force threshold is identified which needs to be overcome to pull the probe particle free in a glass. For the model of hard sphere particles, the microscopic equations for the threshold force and the probability density of the localized probe are solved numerically. Neglecting the spatial structure of the theory, a schematic model is derived which contains two types of bifurcation, the glass transition and the force-induced delocalization, and which allows for analytical and numerical solutions. We discuss its phase diagram, forcing effects on the time-dependent correlation functions, and the friction increment. The model was successfully applied to simulations and experiments on colloidal hard sphere systems [I. Gazuz et. al., Phys. Rev. Lett. 102, 248302 (2009)], while we provide detailed information on its derivation and general properties.

cond-mat.soft↗

arXiv2013

Elastic properties of colloidal solids with disorder

Recent progress in approaches to determine the elastic constants of solids starting from the microscopic particle interactions is reviewed. On the theoretical side, density functional theory approaches are discussed and compared to more classical ones using the actual pair potentials. On the experimental side, video microscopy has been introduced to measure the elastic constants in colloidal solids. For glasses and disordered systems, the theoretical basis is given for this novel technique, and some challenges and recent advances are reviewed.

cond-mat.stat-mech↗

arXiv2012

On the Bauschinger effect in supercoooled melts under shear: results from mode coupling theory and molecular dynamics simulations

We study the nonlinear rheology of a glass-forming binary mixture under the reversal of shear flow using molecular dynamics simulations and a schematic model of the mode-coupling theory of the glass transition (MCT). Memory effects lead to a history-dependent response, as exemplified by the vanishing of a stress-overshoot phenomenon in the stress--strain curves of the sheared liquid, and a change in the apparent elastic coefficients around states with zero stress. We investigate the various retarded contributions to the stress response at a given time schematically within MCT. The connection of this macroscopic response to single-particle motion is demonstrated using molecular-dynamics simulation.

cond-mat.soft↗

arXiv2012

Overshoots in stress strain curves: Colloid experiments and schematic mode coupling theory

The stress versus strain curves in dense colloidal dispersions under start-up shear flow are investigated combining experiments on model core-shell microgels, computer simulations of hard disk mixtures, and mode coupling theory. In dense fluid and glassy states, the transient stresses exhibit first a linear increase with the accumulated strain, then a maximum ('stress overshoot') for strain values around 5%, before finally approaching the stationary value, which makes up the flow curve. These phenomena arise in well-equilibrated systems and for homogeneous flows, indicating that they are generic phenomena of the shear-driven transient structural relaxation. Microscopic mode coupling theory (generalized to flowing states by integration through the transients) derives them from the transient stress correlations, which first exhibit a plateau (corresponding to the solid-like elastic shear modulus) at intermediate times, and then negative stress correlations during the final decay. We introduce and validate a schematic model within mode coupling theory which captures all of these phenomena and handily can be used to jointly analyse linear and large-amplitude moduli, flow curves, and stress-strain curves. This is done by introducing a new strain- and time-dependent vertex into the relation between the the generalized shear modulus and the transient density correlator.

cond-mat.soft↗

arXiv2012

Glass elasticity from particle trajectories

Using positional data from video-microscopy of a two-dimensional colloidal system and from simulations of hard discs we determine the wave-vector-dependent normal mode spring constants in the supercooled fluid and glassy state, respectively. The emergence of rigidity and the existence of a displacement field in amorphous solids is clarified. Continuum elastic theory is used in the limit of long wavelengths to analyze the bulk and shear modulus of this amorphous system as a function of temperature. The onset of a finite static shear modulus upon cooling marks the fluid/solid transition. This provides an opportunity to determine the glass transition temperature $T_g$ in an intuitive and precise way.

cond-mat.soft↗

arXiv2012

Probability densities of a forced probe particle in glass: results from mode coupling theory and simulations of active microrheology

We investigate the displacements of a probe particle inside a glass, when a strong external force is applied to the probe (active nonlinear microrheology). Calculations within mode coupling theory are presented for glasses of hard spheres and compared to Langevin and Brownian dynamics simulations. Under not too strong forces where the probe remains trapped, the probe density distribution becomes anisotropic. It is shifted towards the direction of the force, develops an enhanced tail in that direction (signalled by a positive skewness), and exhibits different variances along and perpendicular to the force direction. A simple model of an harmonically trapped probe rationalizes the low force limit, with strong strain softening setting in at forces of the order of a few thermal energies per particle radius.

cond-mat.soft↗

arXiv2011

Tagged-particle motion in glassy systems under shear: Comparison of mode coupling theory and Brownian Dynamics simulations

We study the dynamics of a tagged particle in a glassy system under shear. The recently developed integration through transients approach based on mode coupling theory, is continued to arrive at the equations for the tagged particle correlators and the mean squared displacements. The equations are solved numerically for a two dimensional system, including a nonlinear stability analysis of the glass solution, the so called beta-analysis. We perform Brownian Dynamics simulations in 2-D and compare with theory. After switch on, transient glassy correlation functions show strong fingerprints of the stress overshoot scenario, including, additionally to previously studied superexponential decay, a shoulder-like slowing down after the overshoot. We also find a new type of Taylor dispersion in glassy states which has intriguing similarity to the known low density case. The theory qualitatively captures most features of the simulations with quantitative deviations concerning the shear induced timescales. We attribute these deviations to an underestimation of the overshoot scenario in the theory.

cond-mat.soft↗

arXiv2010

Schematic Models for Active Nonlinear Microrheology

We analyze the nonlinear active microrheology of dense colloidal suspensions using a schematic model of mode-coupling theory. The model describes the strongly nonlinear behavior of the microscopic friction coefficient as a function of applied external force in terms of a delocalization transition. To probe this regime, we have performed Brownian dynamics simulations of a system of quasi-hard spheres. We also analyze experimental data on hard-sphere-like colloidal suspensions [Habdas et al., Europhys. Lett., 2004, 67, 477]. The behavior at very large forces is addressed specifically.

cond-mat.soft↗

arXiv2010

Comment on "Probing the equilibrium dynamics of colloidal hard spheres above the mode-coupling glass transition"

In the Letter [PRL 102, 085703 (2009)] Brambilla, et al. claimed to observe activated dynamics in colloidal hard spheres above the critical packing fraction of mode coupling theory (MCT). By performing microscopic MCT calculations, we show that polydispersity in their system shifts the critical packing fraction above the value determined by van Megen et al. for less polydisperse samples, and that the data agree with theory except for, possibly, the highest packing fraction.

cond-mat.soft↗

arXiv2010

Displacement field and elastic constants in non-ideal crystals

In this work a periodic crystal with point defects is described in the framework of linear response theory for broken symmetry states using correlation functions and Zwanzig-Mori equations. The main results are microscopic expressions for the elastic constants and for the coarse-grained density, point-defect density, and displacement field, which are valid in real crystals, where vacancies and interstitials are present. The coarse-grained density field differs from the small wave vector limit of the microscopic density. In the long wavelength limit, we recover the phenomenological description of elasticity theory including the defect density.

cond-mat.soft↗

arXiv2009

Non-Equilibrium relation between mobility and diffusivity of interacting Brownian particles under shear

We investigate the relation between mobility and diffusivity for Brownian particles under steady shear near the glass transition, using mode coupling approximations. For the two directions perpendicular to the shear direction, the particle motion is diffusive at long times and the mobility reaches a finite constant. Nevertheless, the Einstein relation holds only for the short-time in-cage motion and is violated for long times. In order to get the relation between diffusivity and mobility, we perform the limit of small wavevector for the relations derived previously [Phys. Rev. Lett. 102 (2009), 135701], without further approximation. We find good agreement to simulation results. Furthermore, we split the extra term in the mobility in an exact way into three terms. Two of them are expressed in terms of mean squared displacements. The third is given in terms of the (less handy) force-force correlation function.

cond-mat.soft↗

arXiv2009

Nonequilibrium fluctuation dissipation relations of interacting Brownian particles driven by shear

We present a detailed analysis of the fluctuation dissipation theorem (FDT) close to the glass transition in colloidal suspensions under steady shear using mode coupling approximations. Starting point is the many-particle Smoluchowski equation. Under shear, detailed balance is broken and the response functions in the stationary state are smaller at long times than estimated from the equilibrium FDT. An asymptotically constant relation connects response and fluctuations during the shear driven decay, restoring the form of the FDT with, however, a ratio different from the equilibrium one. At short times, the equilibrium FDT holds. We follow two independent approaches whose results are in qualitative agreement. To discuss the derived fluctuation dissipation ratios, we show an exact reformulation of the susceptibility which contains not the full Smoluchowski operator as in equilibrium, but only its well defined Hermitian part. This Hermitian part can be interpreted as governing the dynamics in the frame comoving with the probability current. We present a simple toy model which illustrates the FDT violation in the sheared colloidal system.

cond-mat.soft↗

arXiv2009

A mode coupling theory for Brownian particles in homogeneous steady shear flow

A microscopic approach is presented for calculating general properties of interacting Brownian particles under steady shearing. We start from exact expressions for shear-dependent steady-state averages, such as correlation and structure functions, in the form of generalized Green-Kubo relations. To these we apply approximations inspired by the mode coupling theory (MCT) for the quiescent system, accessing steady-state properties by integration through the transient dynamics after startup of steady shear. Exact equations of motion, with memory effects, for the required transient density correlation functions are derived next; these can also be approximated within an MCT-like approach. This results in closed equations for the non-equilibrium stationary state of sheared dense colloidal dispersions, with the equilibrium structure factor of the unsheared system as the only input. In three dimensions, these equations currently require further approximation prior to numerical solution. However, some universal aspects can be analyzed exactly, including the discontinuous onset of a yield stress at the ideal glass transition predicted by MCT. Using these methods we additionally discuss the distorted microstructure of a sheared hard-sphere colloid near the glass transition, and consider how this relates to the shear stress. Time-dependent fluctuations around the stationary state are then approximated, and compared to data from experiment and simulation; the correlators for yielding glassy states obey a `time-shear-superposition' principle. The work presented here fully develops an approach first outlined previously (M. Fuchs and M. E. Cates, Phys. Rev. Lett. 89, 248304, (2002)), while incorporating a significant technical change from that work in the choice of mode coupling approximation used, whose advantages are discussed.

cond-mat.soft↗