arXiv subjects

Gerhard Jung

Publications and source records attributed to Gerhard Jung.

At least 37 records · Page 2Linked to original sources

arXiv2023

Mobility, response and transport in non-equilibrium coarse-grained models

We investigate two different types of non-Markovian coarse-grained models extracted from a linear, non-equilibrium microscopic system, featuring a tagged particle coupled to underdamped oscillators. The first model is obtained by analytically ``integrating out'' the oscillators and the second is derived using projection operator techniques. We observe that these two models behave very differently when the tagged particle is exposed to external harmonic potentials or pulling forces. Most importantly, we find that the analytic model has a well defined friction kernel and can be used to extract work, consistent with the microscopic system, while the projection model corresponds to an effective equilibrium model, which cannot be used to extract work. We apply the analysis to two popular non-equilibrium systems, time-delay feedback control and the active Ornstein-Uhlenbeck process. Finally, we highlight that our study could have important consequences for dynamic coarse-graining of non-equilibrium systems going far beyond the linear systems investigated in this manuscript.

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arXiv2023

Predicting dynamic heterogeneity in glass-forming liquids by physics-inspired machine learning

We introduce GlassMLP, a machine learning framework using physics-inspired structural input to predict the long-time dynamics in deeply supercooled liquids. We apply this deep neural network to atomistic models in 2D and 3D. Its performance is better than the state of the art while being more parsimonious in terms of training data and fitting parameters. GlassMLP quantitatively predicts four-point dynamic correlations and the geometry of dynamic heterogeneity. Transferability across system sizes allows us to efficiently probe the temperature evolution of spatial dynamic correlations, revealing a profound change with temperature in the geometry of rearranging regions.

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arXiv2023

Computer Simulations and Mode-Coupling Theory of Glass-Forming Confined Hard-Sphere Fluids

We present mode-coupling theory (MCT) results for densely packed hard-sphere fluids confined between two parallel walls and compare them quantitatively to computer simulations. The numerical solution of MCT is calculated for the first time using the full system of matrix-valued integro-differential equations. We investigate several dynamical properties of supercooled liquids including scattering functions, frequency-dependent susceptibilities and mean-square displacements. Close to the glass transition, we find quantitative agreement between the coherent scattering function predicted from theory and evaluated from simulations, which enables us to make quantitative statements on caging and relaxation dynamics of the confined hard-sphere fluid.

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arXiv2022

Structural properties of liquids in extreme confinement

We simulate a hard-sphere liquid in confined geometry where the separation of the two parallel, hard walls is smaller than two particle diameters. By systematically reducing the wall separation we analyze the behavior of structural and thermodynamic properties, such as inhomogeneous density profiles, structure factors, and compressibilities when approaching the two-dimensional limit. In agreement with asymptotic predictions, we find for quasi-two-dimensional fluids that the density profile becomes parabolic and the structure factor converges towards its two-dimensional counterpart. To extract the compressibility in polydisperse samples a perturbative expression is used which qualitatively influences the observed non-monotonic dependence of the compressibility with wall separation. We also present theoretical calculations based on fundamental-measure theory and integral-equation theory, which are in very good agreement with the simulation results.

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arXiv2021

Non-Markovian systems out of equilibrium: Exact results for two routes of coarse graining

Generalized Langevin equations (GLEs) can be systematically derived via dimensional reduction from high-dimensional microscopic systems. For linear models the derivation can either be based on projection operator techniques such as the Mori-Zwanzig (MZ) formalism or by "integrating out" the bath degrees of freedom. Based on exact analytical results we show that both routes can lead to fundamentally different GLEs and that the origin of these differences is based inherently on the non-equilibrium nature of the microscopic stochastic model. The most important conceptional difference between the two routes is that the MZ result intrinsically fulfills the generalized second fluctuation-dissipation theorem while the integration result can lead to its violation. We supplement our theoretical findings with numerical and simulation results for two popular non-equilibrium systems: Time-delayed feedback control and the active Ornstein-Uhlenbeck process.

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arXiv2021

Tagged-particle dynamics in confined colloidal liquids

We present numerical results for the tagged-particle dynamics by solving the mode-coupling theory in confined geometry for colloidal liquids (cMCT). We show that neither the microscopic dynamics nor the type of intermediate scattering function qualitatively changes the asymptotic dynamics in vicinity of the glass transition. In particular, we find similar characteristics of confinement in the low-frequency susceptibility spectrum which we interpret as footprints of parallel relaxation. We derive predictions for the localization length and the scaling of the diffusion coefficient in the supercooled regime and discover a pronounced non-monotonic dependence on the confinement length. For dilute liquids in the hydrodynamic limit we calculate an analytical expression for the intermediate scattering functions, which is in perfect agreement with event-driven Brownian dynamics simulations. From this, we derive an expression for persistent anti-correlations in the velocity autocorrelation function (VACF) for confined motion. Using numerical results of the cMCT equations for the VACF we also identify a cross-over between different scalings corresponding to a transition from unconfined to confined behaviour.

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arXiv2021

Fluctuation-Dissipation Relations Far from Equilibrium: A Case Study

Fluctuation-dissipation relations or "theorems" (FDTs) are fundamental for statistical physics and can be rigorously derived for equilibrium systems. Their applicability to non-equilibrium systems is, however, debated. Here, we simulate an active microrheology experiment, in which a spherical colloid is pulled with a constant external force through a fluid, creating near-equilibrium and far-from-equilibrium systems. We characterize the structural and dynamical properties of these systems, and reconstruct an effective generalized Langevin equation (GLE) for the colloid dynamics. Specifically, we test the validity of two FDTs: The first FDT relates the non-equilibrium response of a system to equilibrium correlation functions, and the second FDT relates the memory friction kernel in the GLE to the stochastic force. We find that the validity of the first FDT depends strongly on the strength of the external driving: it is fulfilled close to equilibrium and breaks down far from it. In contrast, we observe that the second FDT is always fulfilled. We provide a mathematical argument why this generally holds for memory kernels reconstructed from a deterministic Volterra equation for correlation functions, even for non-stationary non-equilibrium systems. Motivated by the Mori-Zwanzig formalism, we therefore suggest to impose an orthogonality constraint on the stochastic force, which is in fact equivalent to the validity of this Volterra equation. Such GLEs automatically satisfy the second FDT and are unique, which is desirable when using GLEs for coarse-grained modeling.

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arXiv2021

Tagged-particle motion in quasi-confined colloidal hard-sphere liquids

We investigate the tagged-particle motion in a strongly interacting quasi-confined liquid using periodic boundary conditions along the confining direction. Within a mode-coupling theory of the glass transition (MCT) we calculate the self-nonergodicity parameters and the self-intermediate scattering function and compare them with event-driven molecular dynamics simulations. We observe non-monotonic behavior for the in-plane mean-square displacement and further correlation functions which refer to higher mode indices encoding information about the perpendicular motion. The in-plane velocity-autocorrelation function reveals persistent anti-correlations with a negative algebraic power-law decay $t^{-2}$ at all packing fractions.

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arXiv2021

Wall slip and bulk yielding in soft particle suspensions

We simulate a dense athermal suspension of soft particles sheared between hard walls of a prescribed roughness profile, using a method that fully accounts for the fluid mechanics of the solvent between the particles, and between the particles and the walls, as well as for the solid mechanics of changes in the particle shapes. We thus capture the widely observed phenomenon of elastohydrodynamic wall slip, in which the soft particles become deformed in shear and lift away from the wall slightly, leaving behind a thin lubricating solvent layer of high shear. For imposed stresses below the material's bulk yield stress, we show the observed wall slip to be dominated by this thin solvent layer. At higher stresses, it is augmented by an additional contribution arising from a fluidisation of the first few layers of particles near the wall. By systematically varying the roughness of the walls, we quantify a suppression of slip with increasing wall roughness. For smooth walls, slip radically changes the steady state bulk flow curve of shear stress as a function of shear rate, by conferring a branch of apparent (slip-induced) flow even for $σ<σ_y$, as seen experimentally. We also elucidate the effects of slip on the dynamics of yielding following the imposition of a constant shear stress, characterising the timescales at which bulk yielding arises, and at which slip first sets in.

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arXiv2021

Model reduction techniques for the computation of extended Markov parameterizations for generalized Langevin equations

The generalized Langevin equation is a model for the motion of coarse-grained particles where dissipative forces are represented by a memory term. The numerical realization of such a model requires the implementation of a stochastic delay-differential equation and the estimation of a corresponding memory kernel. Here we develop a new approach for computing a data-driven Markov model for the motion of the particles, given equidistant samples of their velocity autocorrelation function. Our method bypasses the determination of the underlying memory kernel by representing it via up to about twenty auxiliary variables. The algorithm is based on a sophisticated variant of the Prony method for exponential interpolation and employs the Positive Real Lemma from model reduction theory to extract the associated Markov model. We demonstrate the potential of this approach for the test case of anomalous diffusion, where data are given analytically, and then apply our method to velocity autocorrelation data of molecular dynamics simulations of a colloid in a Lennard-Jones fluid. In both cases, the VACF and the memory kernel can be reproduced very accurately. Moreover, we show that the algorithm can also handle input data with large statistical noise. We anticipate that it will be a very useful tool in future studies that involve dynamic coarse-graining of complex soft matter systems.

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arXiv2020

Dynamic properties of quasi-confined colloidal hard-sphere liquids near the glass transition

The complex behavior of confined fluids arising due to a competition between layering and local packing can be disentangled by considering quasi-confined liquids, where periodic boundary conditions along the confining direction restore translational invariance. This system provides a means to investigate the interplay of the relevant length scales of the confinement and the local order. We provide a mode-coupling theory of the glass transition (MCT) for quasi-confined liquids and elaborate an efficient method for the numerical implementation. The nonergodicity parameters in MCT are compared to computer-simulation results for a hard-sphere fluid. We evaluate the nonequilibrium-state diagram and investigate the collective intermediate scattering function. For both methods, nonmonotonic behavior depending on the confinement length is observed.

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arXiv2020

An improved integration scheme for Mode-coupling-theory equations

Within the mode-coupling theory (MCT) of the glass transition, we reconsider the numerical schemes to evaluate the MCT functional. Here we propose nonuniform discretizations of the wave number, in contrast to the standard equidistant grid, in order to decrease the number of grid points without losing accuracy. We discuss in detail how the integration scheme on the new grids has to be modified from standard Riemann integration. We benchmark our approach by solving the MCT equations numerically for mono-disperse hard disks and hard spheres and by computing the critical packing fraction and the nonergodicity parameters. Our results show that significant improvements in performance can be obtained by employing a nonuniform grid.

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arXiv2020

Confinement-induced demixing and crystallization

We simulate a strongly size-disperse hard-sphere fluid confined between two parallel, hard walls. We find that confinement induces crystallization into n-layered hexagonal lattices and a novel honeycomb-shaped structure, facilitated by fractionation. The onset of freezing prevents the formation of a stable glass phase and occurs at much smaller packing fraction than in bulk. Varying the wall separation triggers solid-to-solid transitions and a systematic change of the size-distribution of crystalline particles, which we rationalize using a semi-quantitative theory. We show that the crystallization can be exploited in a wedge geometry to demix particles of different sizes.

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arXiv2020

Dynamical properties of densely packed confined hard-sphere fluids

Numerical solutions of the mode-coupling theory (MCT) equations for a hard-sphere fluid confined between two parallel hard walls are elaborated. The governing equations feature multiple parallel relaxation channels which significantly complicate their numerical integration. We investigate the intermediate scattering functions and the susceptibility spectra close to structural arrest and compare to an asymptotic analysis of the MCT equations. We corroborate that the data converge in the $β$-scaling regime to two asymptotic power laws, viz. the critical decay and the von Schweidler law. The numerical results reveal a non-monotonic dependence of the power-law exponents on the slab width and a non-trivial kink in the low-frequency susceptibility spectra. We also find qualitative agreement of these theoretical results to event-driven molecular-dynamics simulations of polydisperse hard-sphere system. In particular, the non-trivial dependence of the dynamical properties on the slab width is well reproduced.

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arXiv2020

Scaling equations for mode-coupling theories with multiple decay channels

Multiple relaxation channels often arise in the dynamics of liquids where the momentum current associated to the particle-conservation law splits into distinct contributions. Examples are strongly confined liquids for which the currents in lateral and longitudinal direction to the walls are very different, or fluids of nonspherical particles with distinct relaxation patterns for translational and rotational degrees of freedom. Here, we perform an asymptotic analysis of the slow structural relaxation close to kinetic arrest as described by mode-coupling theory (MCT) with several relaxation channels. Compared to standard MCT, the presence of multiple relaxation channels significantly changes the structure of the underlying equations of motion and leads to additional, non-trivial terms in the asymptotic solution. We show that the solution can be rescaled, and thus prove that the well-known $ β$-scaling equation of MCT remains valid even in the presence of multiple relaxation channels. The asymptotic treatment is validated using a novel schematic model. We demonstrate that the numerical solution of this schematic model can indeed be described by the derived asymptotic scaling laws close to kinetic arrest. Additionally, clear traces of the existence of two distinct decay channels are found in the low-frequency susceptibility spectrum, suggesting that clear footprints of the additional relaxation channels can in principle be detected in simulations or experiments of confined or molecular liquids.

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arXiv2018

Generalized Langevin dynamics: Construction and numerical integration of non-Markovian particle-based models

We propose a generalized Langevin dynamics (GLD) technique to construct non-Markovian particle-based coarse-grained models from fine-grained reference simulations and to efficiently integrate them. The proposed GLD model has the form of a discretized generalized Langevin equation with distance-dependent two-particle contributions to the self- and pair-memory kernels. The memory kernels are iteratively reconstructed from the dynamical correlation functions of an underlying fine-grained system. We develop a simulation algorithm for this class of non-Markovian models that scales linearly with the number of coarse-grained particles. Our GLD method is suitable for coarse-grained studies of systems with incomplete time scale separation, as is often encountered, e.g., in soft matter systems. We apply the method to a suspension of nanocolloids with frequency-dependent hydrodynamic interactions. We show that the results from GLD simulations perfectly reproduce the dynamics of the underlying fine-grained system. The effective speedup of these simulations amounts to a factor of about $10^4$. Additionally, the transferability of the coarse-grained model with respect to changes of the nanocolloid density is investigated. The results indicate that the model is transferable to systems with nanocolloid densities that differ by up to one order of magnitude from the density of the reference system.

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arXiv2018

Frequency-dependent Hydrodynamic Interaction Between Two Solid Spheres

Hydrodynamic interactions play an important role in many areas of soft matter science. In simulations with implicit solvent, various techniques such as Brownian or Stokesian dynamics explicitly include hydrodynamic interactions a posteriori by using hydrodynamic diffusion tensors derived from the Stokes equation. However, this equation assumes the interaction to be instantaneous which is an idealized approximation and only valid on long time scales. In the present paper, we go one step further and analyze the time-dependence of hydrodynamic interactions in a compressible fluid on the basis of the linearized Navier-Stokes equation. The theoretical results show that the compressibility of the fluid has a significant impact on frequency-dependent pair interactions. The predictions of the hydrodynamic theory are compared to molecular dynamics simulations of two solid spheres in a Lennard-Jones fluid. For this system we reconstruct memory functions by extending the inverse Volterra technique. The simulation data agree very well with the theory, therefore, the theory can be used to implement dynamically consistent hydrodynamic interactions in the increasingly popular field of non-Markovian modeling.

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arXiv2017

Iterative Reconstruction of Memory Kernels

In recent years, it has become increasingly popular to construct coarse-grained models with non-Markovian dynamics to account for an incomplete separation of time scales. One challenge of a systematic coarse-graining procedure is the extraction of the dynamical properties, namely, the memory kernel, from equilibrium all-atom simulations. In this article, we propose an iterative method for memory reconstruction from dynamical correlation functions. Compared to previously proposed noniterative techniques, it ensures by construction that the target correlation functions of the original fine-grained systems are reproduced accurately by the coarse-grained system, regardless of time step and discretization effects. Furthermore, we also propose a new numerical integrator for generalized Langevin equations that is significantly more accurate than the more commonly used generalization of the velocity Verlet integrator. We demonstrate the performance of the above-described methods using the example of backflow-induced memory in the Brownian diffusion of a single colloid. For this system, we are able to reconstruct realistic coarse-grained dynamics with time steps about 200 times larger than those used in the original molecular dynamics simulations.

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