arXiv subjects

Marcus Müller

Publications and source records attributed to Marcus Müller.

At least 19 recordsLinked to original sources

arXiv2026

Coupling Complementary Simulations for Combined Performance and Energy Optimization

Polymer simulations are among the most computationally demanding workloads in soft-matter research, often requiring days of execution and high energy consumption to achieve physically meaningful results. In this work, we address these challenges through the coupling and optimization of two complementary simulation frameworks: the Uneyama-Doi Model (UDM) and the SOft coarse-grained Monte Carlo Acceleration (SOMA). UDM efficiently propagates concentration fields at the continuum level, while SOMA resolves chain-scale thermal fluctuations via particle-based Monte Carlo dynamics. Each model was individually optimized for GPU execution using kernel fusion, memory coalescing, asynchronous random-number generation yielding up to 70% (UDM) and 80% (SOMA) performance improvement. The coupling is performed through our proposed coordinator library that orchestrates data exchange and synchronizes time-stepping across multiple GPUs. Further management of coupling workload distribution enabled a 13x overall speedup and 24.5x reduction in total energy usage compared to the SOMA baseline, i. e., 96% energy saving. The proposed hybrid approach maintains the same scientific fidelity while drastically reducing the computational and energy footprint, showcasing the potential of energy-aware, cross-application co-design for sustainable high-performance simulations

cs.DC↗

arXiv2025

Thermal conductivity of commodity polymers under high pressures

Understanding the thermal conductivity of polymers under high-pressure conditions is essential for a range of applications, from aerospace and deep-sea engineering to common lubricants. However, the complex relationship between pressure, $P$, the thermal transport coefficient, $\kappa$, and polymer architecture poses substantial challenges to both experimental and theoretical investigations. In this work, we study the pressur-dependent thermal transport properties of a widely used commodity polymer -- poly(methyl methacrylate) (PMMA) -- using a combination of all-atom molecular dynamics simulations and semi-analytical approaches. While we report both classical and quantum-corrected estimates of $\kappa$, the latter approach reveals that as the pressure increases from 1 atm to 10 GPa, $\kappa$ rises by up to a factor of four -- from 0.21 W m$^{-1}$ K$^{-1}$ to 0.80 W m$^{-1}$ K$^{-1}$. To better understand the mechanisms behind this increase, we disentangle the contributions from bonded and nonbonded monomer interactions. Our analysis shows that nonbonded energy-transfer rates increase by a factor of six over the pressure range, while bonded interactions show a more modest increase -- about a factor of three. This observation further consolidates the fact that the nonbonded interactions play the dominant role in dictating the microscopic heat flow in polymers. These individual energy-transfer rates are also incorporated into a simplified heat diffusion model to predict $\kappa$. The results obtained from different approaches show internal consistency and align well with available experimental data. Additionally, some data for polylactic acid (PLA) are presented.

cond-mat.soft↗

arXiv2025

Machine-learned domain partitioning for computationally efficient coupling of continuum and particle simulations of membrane fabrication

All simulation approaches eventually face limits in computational scalability when applied to large spatiotemporal domains. This challenge becomes especially apparent in molecular-level particle simulations, where high spatial and temporal resolution leads to rapidly increasing computational demands. To overcome these limitations, hybrid methods that combine simulations with different levels of resolution offer a promising solution. In this context, we present a machine learning-based decision model that dynamically selects between simulation methods at runtime. The model is built around a Multilayer perceptron (MLP) that predicts the expected discrepancy between particle and continuum simulation results, enabling the localized use of high-fidelity particle simulations only where they are expected to add value. This concurrent approach is applied to the simulation of membrane fabrication processes, where a particle simulation is coupled with a continuum model. This article describes the architecture of the decision model and its integration into the simulation workflow, enabling efficient, scalable, and adaptive multiscale simulations.

physics.comp-ph↗

arXiv2025

Computing finite--temperature elastic constants with noise cancellation

Elastic constants are central material properties, frequently reported in experimental and theoretical studies. While their computation is straightforward in the absence of thermal fluctuations, finite--temperature methods often suffer from poor signal--to--noise ratios or the presence of strong anharmonic effects. Here, we show how to compute elastic constants in thermal ordered and disordered systems by generalizing a noise--cancellation method originally developed for piezoelectric coupling coefficients. A slight strain is applied to an equilibrated solid. Simulations of both the strained and unstrained (or oppositely strained) reference systems are performed using identical thermostatting schemes. As demonstrated theoretically and with generic one--dimensional models, this allows stress differences to be evaluated and elastic constants to be determined with much reduced thermal noise. We then apply this approach across a diverse set of systems, spanning crystalline argon, ordered silicon as well as amorphous silicon, poly(methyl methacrylate), and cellulose derivatives.

cond-mat.mtrl-sci↗

arXiv2025

Mechanisms of Chain Exchange in Diblock Copolymer Micelles

We investigate the mechanism of chain exchange in diblock copolymer micelles using two distinct yet complementary simulation techniques. First, enhanced sampling method is combined with coarse-grained molecular dynamics to compute a two-dimensional free energy surface for the chain expulsion process in the strong segregation regime. To facilitate chain expulsion, a distance-based collective variable is biased, and the end-to-end distance of the core block is also biased to ensure sufficient sampling of chain conformations. The free energy surface reveals a bimodal distribution of chain conformations along the effective reaction coordinate. The minimum free energy pathway qualitatively aligns with the Halperin-Alexander budding-like mechanism. The free energy barrier along this pathway is calculated for core block lengths ranging from $N_\textrm{core}=4$-$100$, and the barrier is shown to scale as $\beta\Delta F_\textrm{barr} \sim N_\textrm{core}^{2/3}$, consistent with the Halperin-Alexander prediction for a globular transition state. Notably, the free energy surface also reveals a nearly degenerate alternative pathway in which the chain escapes by extending out bead-by-bead, in agreement with previous simulations. We also study the case of a dense copolymer melt, where the core-block shrinks but does not collapse into a dry compact globule in the opposite phase. To examine the kinetic pathway, a simplified model is introduced in which a single chain escapes from a planar interface within a mean-field background. Forward flux sampling calculations yield a linear scaling of the barrier, $\beta\Delta F_\textrm{barr} \sim N_\textrm{core}$, in agreement with experimental observations and prior simulations. Moreover, analysis of successful escape trajectories highlights an extended chain conformation at the transition state.

cond-mat.soft↗

arXiv2025

Stochastic bubble dynamics in phase-separated scalar active matter

In ABP systems, phase separation is accompanied by the emergence of vapor bubbles within liquid domains. Using large-scale particle-based simulations, we study the stochastic dynamics of these bubbles and find that most nucleate, grow, and dissolve within liquid domains. We show that their area dynamics can be described by a Langevin equation with a constant negative drift and noise proportional to the perimeter, fully characterizing bubble area and lifetime statistics. Additionally, we develop a lattice gas model that captures the morphological properties, including the decrease in bubble asphericity with increasing area. These findings provide new insights into phase separation in active matter and highlight limitations in current continuum theories.

cond-mat.soft↗

arXiv2023

Reaction-driven Diffusiophoresis of Liquid Condensates: Mechanisms for Intra-cellular Organization

The cellular environment, characterized by its intricate composition and spatial organization, hosts a variety of organelles, ranging from membrane-bound ones to membraneless structures that are formed through liquid-liquid phase separation. Cells show precise control over the position of such condensates. We demonstrate that organelle movement in external concentration gradients, diffusiophoresis, is distinct from the one of colloids because fluxes can remain finite inside the liquid-phase droplets and movement of the latter arises from incompressibility. Within cellular domains diffusiophoresis naturally arises from biochemical reactions that are driven by a chemical fuel and produce waste. Simulations and analytical arguments within a minimal model of reaction-driven phase separation reveal that the directed movement stems from two contributions: Fuel and waste are refilled or extracted locally, resulting in concentration gradients, which (i) induce product fluxes via incompressibility and (ii) result in an asymmetric forward reaction in the droplet's surroundings (as well as asymmetric backward reaction inside the droplet), thereby shifting the droplet's position. We show that the former contribution dominates and sets the direction of the movement, away from or towards fuel source and waste sink, depending on the product molecules' affinity towards fuel and waste, respectively. The mechanism thus provides a simple means to organize condensates with different composition. Particle-based simulations and systems with more complex reaction cycles corroborate the robustness and universality of this mechanism.

cond-mat.soft↗

arXiv2023

Fractional Chirp-Slope-Shift-Keying for SDR-based Search and Rescue Applications

The use of modern software-defined radio (SDR) devices enables the implementation of efficient communication systems in numerous scenarios. Such technology comes especially handy in the context of search and rescue (SAR) systems, enabling the incorporation of additional communication data transmission into the otherwise sub-optimally used SAR bands at 121.5 and 243~MHz. In this work, we propose a novel low-complexity, energy-efficient modulation scheme that allows transmission of additional data within chirped homing signals, while still meeting the standards of international SAR systems such as COSPAS-SARSAT. The proposed method modulates information onto small deviations of the chirp slope with respect to the required unmodulated chirp, which can be easily detected at the receiver side using digital signal processing.

eess.SP↗

arXiv2023

Morphology-Dependent Influences on the Performance of Battery Cells with a Hierarchically Structured Positive Electrode

The rising demand for high-performing batteries requires new technological concepts. To facilitate fast charge and discharge, hierarchically structured electrodes offer short diffusion paths in the active material. However, there are still gaps in understanding the influences on the cell performance of such electrodes. Here, we employed a cell model to demonstrate that the morphology of the hierarchically structured electrode determines which electrochemical processes dictate the cell performance. The potentially limiting processes include electronic conductivity within the porous secondary particles, solid diffusion within the primary particles, and ionic transport in the electrolyte surrounding the secondary particles. Our insights enable a goal-oriented tailoring of hierarchically structured electrodes for high-power applications.

cond-mat.mtrl-sci↗

arXiv2022

Switchable Wetting of Stimulus Responsive Polymer Brushes by Lipid Vesicles: Experiments and Simulations

We grafted polyacrylic acid brushes containing cysteine side chains at a defined surface density on planar lipid membranes. Specular X-ray reflectivity data indicated that the addition of Cd2+ ions induces the compaction of the polymer brush layer and modulates the adhesion of lipid vesicles. The critical threshold level inducing the switch from non-wetting to partial wetting state, [Cd2+] = 0.25 mM, was determined by microinterferometry. The interactions between vesicles and brushes were evaluated by height fluctuations of the membrane in contact with brushes and the shape of vesicles near the surface. To analyze these experiments, we have studied adhesion of axially symmetric vesicles for finite-range membrane-substrate interaction and buoyancy through simulations. We found that the local transversality condition that relates the maximal curvature at the edge of the adhesion zone to the adhesion strength remains rather accurate. Thus, although it is not experimentally possible to prepare vesicles at zero buoyancy, we can use the transversality condition to estimate the adhesion strength. However, the adhesion diagram is significantly modified by a finite range of membrane-substrate interaction and buoyancy. For downward buoyancy, vesicles merely sediment onto the substrate and there is no mean-field adhesion transition. For upward buoyancy, adhered vesicles are metastable at best. Thus, a mean-field adhesion transition can only occur at vanishing buoyancy. Only for zero-range membrane-substrate interaction does a second-order adhesion transition occur at finite interaction strength. For any finite-range interaction, the transition occurs when the membrane-substrate interaction changes from repulsive to attractive. We present a adhesion diagram as a function of adhesion strength and buoyancy and compare the adhesion behavior of vesicles to the wetting behavior of droplets of liquids.

cond-mat.soft↗

arXiv2021

Dynamics and Rheology of Polymer Melts via Hierarchical Atomistic, Coarse-grained, and Slip-spring Simulations

A hierarchical (triple scale) simulation methodology is presented for the prediction of the dynamical and rheological properties of high molecular weight entangled polymer melts. The methodology consists of atomistic, moderately coarse-grained (mCG), and highly coarse-grained slip-spring (SLSP) simulations. At the mCG level, a few chemically bonded atoms are lumped into one coarse-grained bead. At this level, the chemical identity of the atomistic system, and the interchain topological constraints (entanglements) are preserved. The mCG potentials are derived by matching local structural distributions of the mCG model to those of the atomistic model through iterative Boltzmann inversion. For matching mCG and atomistic dynamics, the mCG time is scaled by a time scaling factor, which compensates for the lower monomeric friction coefficient of the mCG model than that of the atomistic one. At the SLSP level, multiple Kuhn segments of a polymer chain are represented by one coarse-grained bead. The very soft nonbonded interactions between beads do not prevent chain crossing and, hence, can not capture entanglements. The topological constraints are represented by slip-springs. A compensating pair potential is used in the SLSP model, to keep the static macromolecular properties unaltered upon the introduction of slip-springs. The static and kinetic parameters of the SLSP model are determined based on the lower level simulation models. Particularly, matching the orientational autocorrelation of the end-to-end vector, we determine the number of slip-springs and calibrate the timescale of the SLSP model. As the test case, the hierarchical methodology is applied to $cis$-1,4-polybutadiene (cPB) at 413 K. Dynamical properties of cPB melts are calculated for a broad range of molecular weights. The calculations are compared, and found in good agreement, with experimental data from the literature.

cond-mat.soft↗

arXiv2020

Dynamics and Structure of Monolayer Polymer Crystallites on Graphene

Graphene-based nanostructured systems and van-der-Waals heterostructures comprise a material class of growing technological and scientific importance. Joining materials with vastly different properties, polymer-graphene heterosystems promise diverse applications in surface- and nanotechnology, including photovoltaics or nanotribology. Fundamentally, molecular adsorbates are prototypical systems to study confinement-induced phase transitions exhibiting intricate dynamics, which require a comprehensive understanding of the dynamical and static properties on molecular time and length scales. Here, we investigate the dynamics and the structure of a single polyethylene chain on free-standing graphene by means of molecular dynamics simulations. In equilibrium, the adsorbed polymer is orientationally linked to the graphene as two-dimensional folded-chain crystallites or, at elevated temperatures, as a floating solid. The associated superstructure can be reversibly melted on a picosecond time scale upon quasi-instantaneous substrate heating, involving ultrafast heterogeneous melting via a transient floating phase. Our findings elucidate time-resolved molecular-scale ordering and disordering phenomena in individual polymers interacting with solids, yielding complementary information to collective friction and viscosity, and linking to recent experimental observables from ultrafast electron diffraction. We anticipate that the approach will help in resolving non-equilibrium phenomena of hybrid polymeric systems over a broad range of time and length scales.

cond-mat.soft↗

arXiv2019

Interface repulsion and lamellar structures in thin films of homopolymer blends due to thermal oscillations

In equilibrium the interface potential that describes the interaction between two AB interfaces in a binary blend of A and B homopolymers is attractive at all distances, resulting in coarsening of the blend morphology even in the absence of interface curvature. We demonstrate that the dissipative assembly in response to a time-periodic variation of the blend incompatibility qualitatively alters this behavior, i.e., for suitable parameters the interface potential exhibits a periodic spatial modulation and AB interfaces adopt a well-defined distance. We explore for which oscillation periods and amplitudes an interface repulsion occurs and demonstrate that we can control the preferred interface distance over a wide range by varying the oscillation period. Using particle-based simulations we explicitly demonstrate that this dissipative assembly of a homopolymer blend results in a lamellar structure with multiple planar interfaces in a thin film geometry.

cond-mat.soft↗

arXiv2018

Multi-Architecture Monte-Carlo (MC) Simulation of Soft Coarse-Grained Polymeric Materials: SOft coarse grained Monte-carlo Acceleration (SOMA)

Multi-component polymer systems are important for the development of new materials because of their ability to phase-separate or self-assemble into nano-structures. The Single-Chain-in-Mean-Field (SCMF) algorithm in conjunction with a soft, coarse-grained polymer model is an established technique to investigate these soft-matter systems. Here we present an im- plementation of this method: SOft coarse grained Monte-carlo Accelera- tion (SOMA). It is suitable to simulate large system sizes with up to billions of particles, yet versatile enough to study properties of different kinds of molecular architectures and interactions. We achieve efficiency of the simulations commissioning accelerators like GPUs on both workstations as well as supercomputers. The implementa- tion remains flexible and maintainable because of the implementation of the scientific programming language enhanced by OpenACC pragmas for the accelerators. We present implementation details and features of the program package, investigate the scalability of our implementation SOMA, and discuss two applications, which cover system sizes that are difficult to reach with other, common particle-based simulation methods.

physics.comp-ph↗

arXiv2013

Directed transport of polymer drops on vibrating superhydrophobic substrates: A Molecular Dynamics study

Using Molecular Dynamics simulations of a coarse-grained polymer liquid we investigate the transport of droplets on asymmetrically structured (saw-tooth shaped), vibrating substrates. Due to a continuous supply of power by substrate vibrations and the asymmetry of its topography, the droplets are driven in a preferred direction. We study this directed motion as a function of the size of the droplets, the linear dimensions of the substrate corrugation, and the period of vibrations. Two mechanisms of driven transport are identified: (i) one that relies on the droplet's contact lines and (ii), in a range of vibration periods, the entire contact area contributes to the driving. In this latter regime, the set-up may be used in experiments for sorting droplets according to their size. Additionally, we show that the linear dimension of the substrate corrugation affects the flux inside the droplet. While on a substrate with a fine corrugation droplets mostly slide, on a more coarsely corrugated substrate the flux may exhibit an additional rotation pattern.

cond-mat.soft↗

arXiv2013

Correlation between surface topography and slippage: a Molecular Dynamics study

Using Molecular Dynamics simulations of a polymer liquid flowing past flat and patterned surfaces, we investigate the influence of corrugation, wettability and pressure on slippage and friction at the solid-liquid interface. For one-dimensional, rectangular grooves, we observe a gradual crossover between the Wenzel state, where the liquid fills the grooves, and the Cassie state, where the corrugation supports the liquid and the grooves are filled with vapor. Using two independent flow set-ups, we characterize the near-surface flow by the slip length, $δ$, and the position, $z_\textrm{h}$, at which viscous and frictional stresses are balanced according to Navier's partial slip boundary condition. This hydrodynamic boundary position depends on the pressure inside the channel and may be located above the corrugated surface. In the Cassie state, we observe that the edges of the corrugation contribute to the friction.

cond-mat.soft↗

arXiv2013

Parameter passing between Molecular Dynamics and continuum models for droplets on solid substrates - The static case

We study equilibrium properties of polymer films and droplets on a solid substrate employing particle-based simulation techniques (Molecular Dynamics) and a continuum description. Parameter-passing techniques are explored that facilitate a detailed comparison of the two models. In particular, the liquid-vapor, solid-liquid and solid-vapor interface tensions, and the Derjaguin or disjoining pressure are determined by Molecular Dynamics simulations. This information is then introduced into continuum descriptions accounting for (i) the full curvature and (ii) a long-wave approximation of the curvature (thin film model). A comparison of the dependence of the contact angle on droplet size indicates that the theories agree well if the contact angles are defined in a compatible manner.

cond-mat.soft↗

arXiv2012

Test of a scaling hypothesis for the structure factor of disordered diblock copolymer melts

Coarse-grained theories of dense polymer liquids such as block copolymer melts predict a universal dependence of equilibrium properties on a few dimensionless parameters. For symmetric diblock copolymer melts, such theories predict a universal dependence on only chi N and Nbar, where chi is an effective interaction parameter, N is a degree of polymerization, and Nbar is a measure of overlap. We test whether simulation results for the structure factor S(q) obtained from several different simulation models are consistent with this two-parameter scaling hypothesis. We compare results from three models: (1) a lattice Monte Carlo model, the bond-fluctuation model, (2) a bead-spring model with harsh repulsive interactions, similar to that of Kremer and Grest, and (3) a bead-spring model with very soft repulsion between beads, and strongly overlapping beads. We compare results from pairs of simulations of different models that have been designed to have matched values of Nbar, over a range of values of chi N and N, and devise methods to test the scaling hypothesis without relying on any prediction for how the phenomenological interaction parameter chi depends on more microscopic parameters. The results strongly support the scaling hypothesis, even for rather short chains, confirming that it is indeed possible to give an accurate universal description of simulation models that differ in many details.

cond-mat.soft↗