arXiv subjects

Matthias Schmidt

Publications and source records attributed to Matthias Schmidt.

At least 55 records · Page 3Linked to original sources

arXiv2023

Inhomogeneous steady shear dynamics of a three-body colloidal gel former

We investigate the stationary flow of a colloidal gel under an inhomogeneous external shear force using adaptive Brownian dynamics simulations. The interparticle forces are derived from the Stillinger-Weber potential, where the three-body term is tuned to enable network formation and gelation in equilibrium. When subjected to the shear force field, the system develops remarkable modulations in the one-body density profile. Depending on the shear magnitude, particles accumulate either in quiescent regions or in the vicinity of maximum net flow, and we deduce this strong non-equilibrium response to be characteristic of the gel state. Studying the components of the internal force parallel and perpendicular to the flow direction reveals that the emerging flow and structure of the stationary state are driven by significant viscous and structural superadiabatic forces. Thereby, the magnitude and nature of the observed non-equilibrium phenomena differs from the corresponding behavior of simple fluids. We demonstrate that a simple power functional theory reproduces accurately the viscous force profile, giving a rationale of the complex dynamical behavior of the system.

cond-mat.soft↗

arXiv2022

Sedimentation path theory for mass-polydisperse colloidal systems

Both polydispersity and the presence of a gravitational field are inherent to essentially any colloidal experiment. While several theoretical works have focused on the effect of polydispersity on the bulk phase behavior of a colloidal system, little is known about the effect of a gravitational field on a polydisperse colloidal suspension. We extend here sedimentation path theory to study sedimentation-diffusion-equilibrium of a mass-polydisperse colloidal system: the particles possess different buoyant masses but they are otherwise identical. The model helps to understand the interplay between gravity and polydispersity on sedimentation experiments. Since the theory can be applied to any parent distribution of buoyant masses, it can be also used to study sedimentation of monodisperse colloidal systems. We find that mass-polydispersity has a strong influence in colloidal systems near density matching for which the bare density of the colloidal particles equals the solvent density. To illustrate the theory, we study crystallization in sedimentation-diffusion-equilibrium of a suspension of mass-polydisperse hard spheres.

cond-mat.soft↗

arXiv2022

Force balance in thermal quantum many-body systems from Noether's theorem

We address the consequences of invariance properties of the free energy of spatially inhomogeneous quantum many-body systems. We consider a specific position-dependent transformation of the system that consists of a spatial deformation and a corresponding locally resolved change of momenta. This operator transformation is canonical and hence equivalent to a unitary transformation on the underlying Hilbert space of the system. As a consequence, the free energy is an invariant under the transformation. Noether's theorem for invariant variations then allows to derive an exact sum rule, which we show to be the locally resolved equilibrium one-body force balance. For the special case of homogeneous shifting, the sum rule states that the average global external force vanishes in thermal equilibrium.

cond-mat.stat-mech↗

arXiv2022

Variance of fluctuations from Noether invariance

The strength of fluctuations, as measured by their variance, is paramount in the quantitative description of a large class of physical systems, ranging from simple and complex liquids to active fluids and solids. Fluctuations originate from the irregular motion of thermal degrees of freedom and statistical mechanics facilitates their description. Here we demonstrate that fluctuations are constrained by the inherent symmetries of the given system. For particle-based classical many-body systems, Noether invariance at second order in the symmetry parameter leads to exact sum rules. These identities interrelate the global force variance with the mean potential energy curvature. Noether invariance is restored by an exact balance between these distinct mechanisms. The sum rules provide a practical guide for assessing and constructing theories, for ensuring self-consistency in simulation work, and for providing a systematic pathway to the theoretical quantification of fluctuations.

cond-mat.stat-mech↗

arXiv2022

Power functional theory for many-body dynamics

The rich and diverse dynamics of particle-based systems ultimately originates from the coupling of their degrees of freedom via internal interactions. To arrive at a tractable approximation of such many-body problems, coarse-graining is often an essential step. Power functional theory provides a unique and microscopically sharp formulation of this concept. The approach is based on an exact one-body variational principle to describe the dynamics of both overdamped and inertial classical and quantum many-body systems. In equilibrium, density functional theory is recovered, and hence spatially inhomogeneous systems are described correctly. The dynamical theory operates on the level of time-dependent one-body correlation functions. Two- and higher-body correlation functions are accessible via the dynamical test particle limit and the nonequilibrium Ornstein-Zernike route. We describe the structure of this functional approach to many-body dynamics, including much background as well as applications to a broad range of dynamical situations, such as the van Hove function in liquids, flow in nonequilibrium steady states, motility-induced phase separation of active Brownian particles, lane formation in binary colloidal mixtures, and both steady and transient shear phenomena.

cond-mat.soft↗

arXiv2022

Dynamic Decay and Superadiabatic Forces in the van Hove Dynamics of Bulk Hard Sphere Fluids

We study the dynamical decay of the van Hove function of Brownian hard spheres using event-driven Brownian dynamics simulations and dynamic test particle theory. Relevant decays mechanisms include deconfinement of the self particle, decay of correlation shells, and shell drift. Comparison to results for the Lennard-Jones system indicates the generality of these mechanisms for dense overdamped liquids. We use dynamical density functional theory on the basis of the Rosenfeld functional with self interaction correction. Superadiabatic forces are analysed using a recent power functional approximation. The power functional yields a modified Einstein long-time self diffusion coefficient in good agreement with simulation data.

cond-mat.soft↗

arXiv2022

Why Noether's Theorem applies to Statistical Mechanics

Noether's Theorem is familiar to most physicists due its fundamental role in linking the existence of conservation laws to the underlying symmetries of a physical system. Typically the systems are described in the particle-based context of classical mechanics or on the basis of field theory. We have recently shown [Commun. Phys. $\textbf{4}$, 176 (2021)] that Noether's reasoning also applies to thermal systems, where fluctuations are paramount and one aims for a statistical mechanical description. Here we give a pedagogical introduction based on the canonical ensemble and apply it explicitly to ideal sedimentation. The relevant mathematical objects, such as the free energy, are viewed as functionals. This vantage point allows for systematic functional differentiation and the resulting identities express properties of both macroscopic average forces and molecularly resolved correlations in many-body systems, both in and out-of-equilibrium, and for active Brownian particles. To provide further background, we briefly describe the variational principles of classical density functional theory, of power functional theory, and of classical mechanics.

cond-mat.stat-mech↗

arXiv2021

Self-bound dipolar droplets and supersolids in molecular Bose-Einstein condensates

We numerically study the many-body physics of molecular Bose-Einstein condensates with strong dipole-dipole interactions. We observe the formation of self-bound droplets, and explore phase diagrams that feature a variety of exotic supersolid states. In all of these cases, the large and tunable molecular dipole moments enable the study of unexplored regimes and phenomena, including liquid-like density saturation and universal stability scaling laws for droplets, as well as pattern formation and the limits of droplet supersolidity. We discuss a realistic experimental approach to realize both the required collisional stability of the molecular gases and the independent tunability of their contact and dipolar interaction strengths. Our work provides both a blueprint and a benchmark for near-future experiments with bulk molecular Bose-Einstein condensates.

cond-mat.quant-gas↗

arXiv2021

Gravity-induced phase phenomena in plate-rod colloidal mixtures

Gravity can affect colloidal suspensions since for micrometer-sized particles gravitational and thermal energies can be comparable over vertical length scales of a few millimeters. In mixtures, each species possesses a different buoyant mass, which can make experimental results counter-intuitive and difficult to interpret. Here, we revisit from a theoretical perspective iconic sedimentation-diffusion-equilibrium experiments on colloidal plate-rod mixtures by van der Kooij and Lekkerkerker. We reproduce their findings, including the observation of five different mesophases in a single cuvette. Using sedimentation path theory, we incorporate gravity into a microscopic theory for the bulk of a plate-rod mixture. We also show how to disentangle the effects of gravity from sedimentation experiments to obtain the bulk behavior and make predictions that can be experimentally tested. These include changes in the sequence by altering the sample height. We demonstrate that both buoyant mass ratio and sample height form control parameters to study bulk phase behavior.

cond-mat.soft↗

arXiv2021

Noether's Theorem in Statistical Mechanics

Noether's calculus of invariant variations yields exact identities from functional symmetries. The standard application to an action integral allows to identify conservation laws. Here we rather consider generating functionals, such as the free energy and the power functional, for equilibrium and driven many-body systems. Translational and rotational symmetry operations yield mechanical laws. These global identities express vanishing of total internal and total external forces and torques. We show that functional differentiation then leads to hierarchies of local sum rules that interrelate density correlators as well as static and time direct correlation functions, including memory. For anisotropic particles, orbital and spin motion become systematically coupled. The theory allows us to shed new light on the spatio-temporal coupling of correlations in complex systems. As applications we consider active Brownian particles, where the theory clarifies the role of interfacial forces in motility-induced phase separation. For active sedimentation, the center-of-mass motion is constrained by an internal Noether sum rule.

cond-mat.stat-mech↗

arXiv2021

Adaptive Brownian Dynamics

A framework for performant Brownian Dynamics (BD) many-body simulations with adaptive timestepping is presented. Contrary to the Euler-Maruyama scheme in common non-adaptive BD, we employ an embedded Heun-Euler integrator for the propagation of the overdamped coupled Langevin equations of motion. This enables the derivation of a local error estimate and the formulation of criteria for the acceptance or rejection of trial steps and for the control of optimal stepsize. Introducing erroneous bias in the random forces is avoided by Rejection Sampling with Memory (RSwM) due to Rackauckas and Nie, which makes use of the Brownian bridge theorem and guarantees the correct generation of a specified random process even when rejecting trial steps. For test cases of Lennard-Jones fluids in bulk and in confinement, it is shown that adaptive BD solves performance and stability issues of conventional BD, already outperforming the latter even in standard situations. We expect this novel computational approach to BD to be especially helpful in long-time simulations of complex systems, e.g. in non-equilibrium, where concurrent slow and fast processes occur.

cond-mat.stat-mech↗

arXiv2021

Chemomechanical simulation of microtubule dynamics with explicit lateral bond dynamics

We introduce and parameterize a chemomechanical model of microtubule dynamics on the dimer level, which is based on the allosteric tubulin model and includes attachment, detachment and hydrolysis of tubulin dimers as well as stretching of lateral bonds, bending at longitudinal junctions, and the possibility of lateral bond rupture and formation. The model is computationally efficient such that we reach sufficiently long simulation times to observe repeated catastrophe and rescue events at realistic tubulin concentrations and hydrolysis rates, which allows us to deduce catastrophe and rescue rates. The chemomechanical model also allows us to gain insight into microscopic features of the GTP-tubulin cap structure and microscopic structural features triggering microtubule catastrophes and rescues. Dilution simulations show qualitative agreement with experiments. We also explore the consequences of a possible feedback of mechanical forces onto the hydrolysis process and the GTP-tubulin cap structure.

q-bio.SC↗

arXiv2021

Phase separation of active Brownian particles in two dimensions: Anything for a quiet life

Active Brownian particles display self-propelled movement, which can be modelled as arising from a one-body force. Although their interparticle interactions are purely repulsive, for strong self propulsion the swimmers phase separate into dilute and dense phases. We describe in detail a recent theory (Phys. Rev. E 100, 052604 (2019); Phys. Rev. Lett. 128, 26802 (2019)) for such motility induced phase-separation. Starting from the continuity equation and the force density balance, the description is based on four superadiabatic contributions to the internal force density. Here the superadiabatic forces are due to the flow in the system and they act on top of the adiabatic forces that arise from the equilibrium free energy. Phase coexistence is described by bulk state functions and agrees quantitatively with Brownian dynamics simulation results from the literature. We describe in detail all analytical steps to fully resolve the spatial and orientational dependence of the one-body density and current. The decomposition into angular Fourier series leads to coupling of total density, polarization and all higher modes. We describe the power functional approach, including the kinematic dependence of the superadiabatic force fields and the quiet life effect that pushes particles from fast to slow regions, and hence induces the phase separation.

cond-mat.soft↗

arXiv2021

Roton Excitations in an Oblate Dipolar Quantum Gas

We observe signatures of radial and angular roton excitations around a droplet crystallization transition in dipolar Bose-Einstein condensates. In situ measurements are used to characterize the density fluctuations near this transition. The static structure factor is extracted and used to identify the radial and angular roton excitations by their characteristic symmetries. These fluctuations peak as a function of interaction strength indicating the crystallization transition of the system. We compare our observations to a theoretically calculated excitation spectrum allowing us to connect the crystallization mechanism with the softening of the angular roton modes.

cond-mat.quant-gas↗

arXiv2021

Custom Flow in Molecular Dynamics

Driving an inertial many-body system out of equilibrium generates complex dynamics due to memory effects and the intricate relationships between the external driving force, internal forces, and transport effects. Understanding the underlying physics is challenging and often requires carrying out case-by-case analysis. To systematically study the interplay between all types of forces that contribute to the dynamics, a method to generate prescribed flow patterns could be of great help. We develop a custom flow method to numerically construct the external force field required to obtain the desired time evolution of an inertial many-body system, as prescribed by its one-body current and density profiles. We validate the custom flow method in a Newtonian system of purely repulsive particles by creating a slow motion dynamics of an out-of-equilibrium process and by prescribing the full time evolution between two distinct equilibrium states. The method can also be used with thermostat algorithms to control the temperature.

cond-mat.soft↗

arXiv2021

Universality in Driven and Equilibrium Hard Sphere Liquid Dynamics

We demonstrate that the time evolution of the van Hove dynamical pair correlation function is governed by adiabatic forces that arise from the free energy and by superadiabatic forces that are induced by the flow of the van Hove function. The superadiabatic forces consist of drag, viscous, and structural contributions, as occur in active Brownian particles, in liquids under shear and in lane forming mixtures. For hard sphere liquids we present a power functional theory that predicts these universal force fields in quantitative agreement with our Brownian dynamics simulation results.

cond-mat.soft↗

arXiv2020

Fluctuation profiles in inhomogeneous fluids

Three one-body profiles that correspond to local fluctuations in energy, in entropy, and in particle number are used to describe the equilibrium properties of inhomogeneous classical many-body systems. Local fluctuations are obtained from thermodynamic differentiation of the density profile or equivalently from average microscopic covariances. The fluctuation profiles follow from functional generators and they satisfy Ornstein-Zernike relations. Computer simulations reveal markedly different fluctuations in confined fluids with Lennard-Jones, hard sphere, and Gaussian core interactions.

cond-mat.soft↗

arXiv2020

Dynamic Pair Correlations and Superadiabatic Forces in a Dense Brownian Liquid

We study dynamic two-body correlation functions, i.e. the two-body density, the current-density correlator or van Hove current, and the current-current correlator in Brownian dynamics computer simulations of a dense Lennard-Jones bulk liquid. The dynamic decay of the correlation shells of the two-body density is examined in detail. Inner correlation shells decay faster than outer correlation shells, whereas outer correlation shells remain stable for increasing times. Within a dynamic test particle picture the mechanism is assumed to be triggered by the dislocation of the self particle, which releases the confinement of the surrounding correlation shells. We present a division of the van Hove current into an adiabatic and a superadiabatic contribution. The magnitude of the adiabatic van Hove current is found to exceed that of the total van Hove current, which is consistent with dynamic density functional theory overestimating the speed of the dynamics. The direction of the superadiabatic van Hove current opposes that of the total van Hove current. The current-current correlator reveals detailed insight in the collisions of the particles. We find a large static nearest-neighbor peak, which results from colliding particles and different dynamic peaks, that are attributed to consecutive collisions.

cond-mat.soft↗