arXiv subjects

Thomas Speck

Publications and source records attributed to Thomas Speck.

At least 55 records · Page 3Linked to original sources

arXiv2019

Dynamical coexistence in moderately polydisperse hard-sphere glasses

We perform extensive numerical simulations of a paradigmatic model glass former, the hard-sphere fluid with 10% polydispersity. We sample from the ensemble of trajectories with fixed observation time, whereby single trajectories are generated by event-driven molecular dynamics. We show that these trajectories can be characterized in terms of local structure, and we find a dynamical-structural (active-inactive) phase transition between two dynamical phases: one dominated by liquid-like trajectories with low degree of local order and one dominated by glassy-like trajectories with a high degree of local order. We show that both phases coexist and are separated by a spatiotemporal interface. Sampling exceptionally long trajectories allows to perform a systematic finite-size scaling analysis. We find excellent agreement with Binder's scaling theory for first-order transitions. Interestingly, the coexistence region narrows at higher densities, supporting the idea of a critical point controlling the dynamic arrest.

cond-mat.stat-mech↗

arXiv2019

From scalar to polar active matter: Connecting simulations with mean-field theory

We study numerically the phase behavior of self-propelled elliptical particles interacting through the "hard" repulsive Gay-Berne potential at infinite Péclet number. Changing a single parameter, the aspect ratio, allows to continuously go from discoid active Brownian particles to elongated polar rods. Discoids show phase separation, which changes to a cluster state of polar domains, which then form polar bands as the aspect ratio is increased. From the simulations, we identify and extract the two effective parameters entering the mean-field description: the force imbalance coefficient and the effective coupling to the local polarization. These two coefficients are sufficient to obtain a complete and consistent picture, unifying the paradigms of scalar and polar active matter.

cond-mat.stat-mech↗

arXiv2019

Quorum-sensing active particles with discontinuous motility

We develop a dynamic mean-field theory for polar active particles that interact through a self-generated field, in particular one generated through emitting a chemical signal. While being a form of chemotactic response, it is different from conventional chemotaxis in that particles discontinuously change their motility when the local concentration surpasses a threshold. The resulting coupled equations for density and polarization are linear and can be solved analytically for simple geometries, yielding inhomogeneous density profiles. Specifically, here we consider a planar and circular interface. Our theory thus explains the observed coexistence of dense aggregates with an active gas. There are, however, differences to the more conventional picture of liquid-gas coexistence based on a free energy, most notably the absence of a critical point. We corroborate our analytical predictions by numerical simulations of active particles under confinement and interacting through volume exclusion. Excellent quantitative agreement is reached through an effective translational diffusion coefficient. We finally show that an additional response to the chemical gradient direction is sufficient to induce vortex clusters. Our results pave the way to engineer motility responses in order to achieve aggregation and collective behavior even at unfavorable conditions.

cond-mat.stat-mech↗

arXiv2019

Thermodynamic Approach to the Self-Diffusiophoresis of Colloidal Janus Particles

Most available theoretical predictions for the self-diffusiophoretic motion of colloidal particles are based on the hydrodynamic thin boundary layer approximation in combination with a solvent body force due to a self-generated local solute gradient. This gradient is enforced through specifying boundary conditions, typically without accounting for the thermodynamic cost to maintain the gradient. Here we present an alternative thermodynamic approach that exploits a direct link between dynamics and entropy production: the local detailed balance condition. We study two cases: First, we revisit self-propulsion in a demixing binary solvent. At variance with a slip velocity, we find that propulsion is due to forces at the poles that are perpendicular to the particle surface. Second, for catalytic swimmers driven through liberating chemical free energy we recover previous expressions. In both cases we argue that propulsion is due to asymmetric dissipation and not simply due to an asymmetric concentration of molecular solutes.

cond-mat.soft↗

arXiv2019

Classical Nucleation Theory for the Crystallization Kinetics in Sheared Liquids

While statistical mechanics provides a comprehensive framework for the understanding of equilibrium phase behavior, predicting the kinetics of phase transformations remains a challenge. Classical nucleation theory (CNT) provides a thermodynamic framework to relate the nucleation rate to thermodynamic quantities such as pressure difference and interfacial tension through the nucleation work necessary to spawn critical nuclei. However, it remains unclear whether such an approach can be extended to the crystallization of driven melts that are subjected to mechanical stresses and flows. Here, we demonstrate numerically for hard spheres that the impact of simple shear on the crystallization rate can be rationalized within the CNT framework by an additional elastic work proportional to the droplet volume. We extract the local stress and strain inside solid droplets, which yield size-dependent values for the shear modulus that are about half of the bulk value. Finally, we show that for a complete description one also has to take into account the change of interfacial work between the strained droplet and the sheared liquid. From scaling reasons, we expect this extra contribution to dominate the work formation of small nuclei but become negligible compared to the elastic work for droplets composed of a few hundreds particles.

cond-mat.stat-mech↗

arXiv2019

Dynamic facilitation theory: A statistical mechanics approach to dynamic arrest

The modeling of supercooled liquids approaching dynamic arrest has a long tradition, which is documented through a plethora of competing theoretical approaches. Here, we review the modeling of supercooled liquids in terms of dynamic "defects", also called excitations or soft spots, that are able to sustain motion. To this end, we consider a minimal statistical mechanics description in terms of active regions with the order parameter related to their typical size. This is the basis for both Adam-Gibbs and dynamical facilitation theory, which differ in their relaxation mechanism as the liquid is cooled: collective motion of more and more particles vs. concerted hierarchical motion over larger and larger length scales. For the latter, dynamic arrest is possible without a growing static correlation length, and we sketch the derivation of a key result: the parabolic law for the structural relaxation time. We critically discuss claims in favor of a growing static length and argue that the resulting scenarios for pinning and dielectric relaxation are in fact compatible with dynamic facilitation.

cond-mat.stat-mech↗

arXiv2019

Spontaneous Spatiotemporal Ordering of Shape Oscillations Enhances Cell Migration

The migration of cells is relevant for processes such as morphogenesis, wound healing, and invasion of cancer cells. In order to move, single cells deform cyclically. However, it is not understood how these shape oscillations influence collective properties. Here we demonstrate, using numerical simulations, that the interplay of directed motion, shape oscillations, and excluded volume enables cells to locally "synchronize" their motion and thus enhance collective migration. Our model captures elongation and contraction of crawling ameboid cells controlled by an internal clock with a fixed period, mimicking the internal cycle of biological cells. We show that shape oscillations are crucial for local rearrangements that induce ordering of internal clocks between neighboring cells even in the absence of signaling and regularization. Our findings reveal a novel, purely physical mechanism through which the internal dynamics of cells influences their collective behavior, which is distinct from well known mechanisms like chemotaxis, cell division, and cell-cell adhesion.

physics.bio-ph↗

arXiv2019

Non-equilibrium Markov state modeling of periodically driven biomolecules

Molecular dynamics simulations allow to study the structure and dynamics of single biomolecules in microscopic detail. However, many processes occur on time scales beyond the reach of fully atomistic simulations and require coarse-grained multiscale models. While systematic approaches to construct such models have become available, these typically rely on microscopic dynamics that obey detailed balance. In vivo, however, biomolecules are constantly driven away from equilibrium in order to perform specific functions and thus break detailed balance. Here we introduce a method to construct Markov state models for systems that are driven through periodically changing one (or several) external parameter. We illustrate the method for alanine dipeptide, a widely used benchmark molecule for computational methods, exposed to a time-dependent electric field.

cond-mat.stat-mech↗

arXiv2018

Aggregation and sedimentation of active Brownian particles at constant affinity

We study the motility-induced phase separation of active particles driven through the interconversion of two chemical species controlled by ideal reservoirs (chemiostats). As a consequence, the propulsion speed is non-constant and depends on the actual inter-particle forces, enhancing the positive feedback between increased density and reduced motility that is responsible for the observed inhomogeneous density. For hard discs, we find that this effect is negligible and that the phase separation is controlled by the average propulsion speed. For soft particles and large propulsion speeds, however, we predict an observable impact on the collective behavior. We briefly comment on the reentrant behavior found for soft discs. Finally, we study the influence of non-constant propulsion on the sedimentation profile of non-interacting active particles.

cond-mat.stat-mech↗

arXiv2018

Active Brownian particles driven by constant affinity

Experimental realizations of self-propelled colloidal Janus particles exploit the conversion of free energy into directed motion. One route are phoretic mechanisms that can be modeled schematically as the interconversion of two chemical species. Here we consider the situation when the difference of chemical potential between the two species (the driving affinity) can be assumed to be constant, and we derive the thermodynamically consistent equations of motion. In contrast to the standard model of active Brownian particles parametrized by a constant self-propulsion speed, this yields a non-constant speed that depends on the potential energy of the suspension. This approach allows to consistently model the breaking of detailed balance and the accompanying entropy production without non-conservative forces.

cond-mat.stat-mech↗

arXiv2018

Devitrification of the Kob-Andersen glass former: Competition with the locally favored structure

Supercooled liquids are kinetically trapped materials in which the transition to a thermodynamically more stable state with long-range order is strongly suppressed. To assess the glass-forming abilities of a liquid empirical rules exist, but a comprehensive microscopic picture of devitrification is still missing. Here we study the crystallization of a popular model glass former, the binary Kob-Andersen mixture, in small systems. We perform trajectory sampling employing the population of the locally favored structure as order parameter. While for large population a dynamical phase transition has been reported, here we show that biasing towards a small population of locally favored structures induces crystallization, and we estimate the free energy difference. This result sheds new light on the competition between local and global structure in glass-forming liquids and its implications for crystallization.

cond-mat.stat-mech↗

arXiv2018

Is directed percolation in colloid-polymer mixtures linked to dynamic arrest?

Using computer simulations, we study the dynamic arrest in a schematic model of colloid-polymer mixtures combining short-ranged attractions with long-ranged repulsions. The arrested gel is a dilute rigid network of colloidal particles bonded due to the strong attractions. Without repulsions, the gel forms at the spinodal through arrested phase separation. In the ergodic suspension at sufficiently high densities, colloidal clusters form temporary networks that percolate space. Recently [Nat. Commun. 7, 11817 (2016)], it has been proposed that the transition of these networks to directed percolation coincides with the onset of the dynamic arrest, thus linking structure to dynamics. Here, we evaluate for various screening lengths the underlying gas-liquid binodal and the percolation transitions. We find that directed percolation shifts the continuous percolation line to larger densities, but even beyond this line the suspension remains ergodic. Only when approaching the spinodal does dynamic arrest occur. Competing repulsions thus do not modify the qualitative scenario for non-equilibrium gelation, although the structure of the emerging percolating network shows some differences.

cond-mat.soft↗

arXiv2018

Transmission of torque at the nanoscale

In macroscopic mechanical devices torque is transmitted through gearwheels and clutches. In the construction of devices at the nanoscale, torque and its transmission through soft materials will be a key component. However, this regime is dominated by thermal fluctuations leading to dissipation. Here we demonstrate the principle of torque transmission for a disc-like colloidal assembly exhibiting clutch-like behaviour, driven by $27$ particles in optical traps. These are translated on a circular path to form a rotating boundary that transmits torque to additional particles confined to the interior. We investigate this transmission and find that it is determined by solid-like or fluid-like behaviour of the device and a stick-slip mechanism reminiscent of macroscopic gearwheels slipping. The transmission behaviour is predominantly governed by the rotation rate of the boundary and the density of the confined system. We determine the efficiency of our device and thus optimise conditions to maximise power output.

cond-mat.soft↗

arXiv2018

Highly controlled optical transport of cold atoms into a hollow-core fiber

We report on an efficient and highly controlled cold atom hollow-core fiber interface, suitable for quantum simulation, information, and sensing. The main focus of this manuscript is a detailed study on transporting cold atoms into the fiber using an optical conveyor belt. We discuss how we can precisely control the spatial, thermal, and temporal distribution of the atoms by, e.g., varying the speed at which the atoms are transported or adjusting the depth of the transport potential according to the atomic position. We characterize the transport of atoms to the fiber tip for these different parameters. In particular, we show that by adapting the transport potential we can lower the temperature of the transported atoms by a factor of 6, while reducing the transport efficiency only by a factor 2. For atoms transported inside the fiber, we can obtain a transport efficiency into the fiber of more than 40% and we study the influence of the different transport parameters on the time-dependent optical depth signal. When comparing our measurements to the results of a classical transport simulation, we find a good qualitative agreement.

physics.atom-ph↗

arXiv2018

Crystallization of hard spheres revisited. II. Thermodynamic modeling, nucleation work, and the surface of tension

Combining three numerical methods (forward flux sampling, seeding of droplets, and finite size droplets), we probe the crystallization of hard spheres over the full range from close to coexistence to the spinodal regime. We show that all three methods allow to sample different regimes and agree perfectly in the ranges where they overlap. By combining the nucleation work calculated from forward flux sampling of small droplets and the nucleation theorem, we show how to compute the nucleation work spanning three orders of magnitude. Using a variation of the nucleation theorem, we show how to extract the pressure difference between the solid droplet and ambient liquid. Moreover, combining the nucleation work with the pressure difference allows us to calculate the interfacial tension of small droplets. Our results demonstrate that employing bulk quantities yields inaccurate results for the nucleation rate.

cond-mat.soft↗

arXiv2018

Geometric view of stochastic thermodynamics for non-equilibrium steady states

We explore the idea that non-equilibrium steady states breaking detailed balance are obtained by deforming trajectories (lines in space-time) that have been sampled in a reference system with stochastic dynamics obeying detailed balance, and we ask for the work required to perform this task. These geometric deformations are not arbitrary but arise through interactions with the environment, either the manipulation of conserved quantities by an external agent, or by their exchange with a work reservoir. This view allows to consistently model the breaking of detailed balance and the accompanying entropy production without non-conservative forces, and to systematically extend the notion of thermodynamic ensembles to non-equilibrium steady states. We illustrate the usefulness of this approach by applying it to suspensions of active colloidal particles and deriving their thermodynamically consistent equations of motion.

cond-mat.stat-mech↗

arXiv2018

Structural-dynamical transition in the Wahnström mixture

In trajectory space, dynamical heterogeneities in glass-forming liquids correspond to the emergence of a dynamical phase transition between an active phase poor in local structure and an inactive phase which is rich in local structure. We support this scenario with the study of a model additive mixture of Lennard-Jones particles, quantifying how the choice of the relevant structural and dynamical observable affects the transition in trajectory space. We find that the low mobility, structure-rich phase is dominated by icosahedral order. Applying a nonequilibrium rheological protocol, we connect local order to the emergence of mechanical rigidity.

cond-mat.soft↗

arXiv2018

Crystallization of hard spheres revisited. I. Extracting kinetics and free energy landscape from forward flux sampling

We investigate the kinetics and the free energy landscape of the crystallization of hard spheres from a supersaturated metastable liquid though direct simulations and forward flux sampling. In this first paper, we describe and test two different ways to reconstruct the free energy barriers from the sampled steady state probability distribution of cluster sizes without sampling the equilibrium distribution. The first method is based on mean first passage times, the second on splitting probabilities. We verify both methods for a single particle moving in a double-well potential. For the nucleation of hard spheres, these methods allow to probe a wide range of supersaturations, and to reconstruct the kinetics and the free energy landscape from the same simulation. Results are consistent with the scaling predicted by classical nucleation theory although a quantitative fit requires a rather large, effective interfacial tension.

cond-mat.soft↗