Enhanced dynamics in deep thermal cycling of a model glass.

We investigate the effect of low temperature (cryogenic) thermal cycling on dynamics of a generic model glass via molecular dynamics simulations. By calculating mean squared displacements after a varying number of cycles, a pronounced enhancement of dynamics is observed. This rejuvenation effect is visible already after the first cycle and accumulates upon further cycling in an intermittent way. Our data reveal an overall deformation (buckling of the slab-shaped system) modulated by a heterogeneous deformation field due to deep cryogenic thermal cycling. It is shown via strain maps that deformation localizes in the form of shear-bands, which gradually fill the entire sample in a random and intermittent manner, very much similar to the accumulation effect observed in dynamics. While spatial organization of local strain may be connected to the specific geometry, we argue that the heterogeneity of the structure is the main cause behind rejuvenation effects observed in the present study.

Temperature Rise Inside Shear Bands in a Simple Model Glass.

One of the key factors, which hampers the application of metallic glasses as structural components, is the localization of deformation in narrow bands of a few tens up to one hundred nanometers thickness, the so-called shear bands. Processes, which occur inside shear bands are of central importance for the question whether a catastrophic failure of the material is unavoidable or can be circumvented or, at least, delayed. Via molecular dynamics simulations, this study addresses one of these processes, namely the local temperature rise due to viscous heat generation. The major contribution to energy dissipation is traced back to the plastic work performed by shear stress during steady deformation. Zones of largest strain contribute the most to this process and coincide with high-temperature domains (hottest spots) inside the sample. Magnitude of temperature rise can reach a few percent of the sample's glass transition temperature. Consequences of these observations are discussed in the context of the current research in the field.

Thin interface limit of the double-sided phase-field model with convection.

The thin interface limit of the phase-field model is extended to include transport via melt convection. A double-sided model (equal diffusivity in liquid and solid phases) is considered for the present analysis. For the coupling between phase-field and Navier-Stokes equations, two commonly used schemes are investigated using a matched asymptotic analysis: (i) variable viscosity and (ii) drag force model. While for the variable viscosity model, the existence of a thin interface limit can be shown up to the second order in the expansion parameter, difficulties arise in satisfying no-slip boundary condition at this order for the drag force model. Nevertheless, detailed numerical simulations in two dimensions show practically no difference in dendritic growth profiles in the presence of forced melt flow obtained for the two coupling schemes. This suggests that both approaches can be used for the purpose of numerical simulations. Simulation results are also compared to analytic theory, showing excellent agreement for weak flow. Deviations at higher fluid velocities are discussed in terms of the underlying theoretical assumptions. This article is part of the theme issue 'Patterns in soft and biological matters'.

Probing the Degree of Heterogeneity within a Shear Band of a Model Glass.

Recent experiments provide evidence for density variations along shear bands in metallic glasses with a length scale of a few hundred nanometers. Via molecular dynamics simulations of a generic binary glass model, here we show that this is strongly correlated with variations of composition, coordination number, viscosity, and heat generation. Individual shear events along the shear band path show a mean distance of a few nanometers, comparable to recent experimental findings on medium range order. The aforementioned variations result from these localized perturbations, mediated by elasticity.

Non-monotonic effect of additive particle size on the glass transition in polymers.

Effect of small additive molecules on the structural relaxation of polymer melts is investigated via molecular dynamics simulations. At a constant external pressure and a fixed number concentration of added molecules, the variation of the particle diameter leads to a non-monotonic change of the relaxation dynamics of the polymer melt. For non-entangled chains, this effect is rationalized in terms of an enhanced added-particle-dynamics which competes with a weaker coupling strength upon decreasing the particle size. Interestingly, cooling simulations reveal a non-monotonic effect on the glass transition temperature also for entangled chains, where the effect of additives on polymer dynamics is more intricate. This observation underlines the importance of monomer-scale packing effects on the glass transition in polymers. In view of this fact, size-adaptive thermosensitive core-shell colloids would be a promising candidate route to explore this phenomenon experimentally.

Shear-density coupling for a compressible single-component yield-stress fluid.

Flow behavior of a single-component yield stress fluid is addressed on the hydrodynamic level. A basic ingredient of the model is a coupling between fluctuations of density and velocity gradient via a Herschel-Bulkley-type constitutive model. Focusing on the limit of low shear rates and high densities, the model approximates well-but is not limited to-gently sheared hard sphere colloidal glasses, where solvent effects are negligible. A detailed analysis of the linearized hydrodynamic equations for fluctuations and the resulting cubic dispersion relation reveals the existence of a range of densities and shear rates with growing flow heterogeneity. In this regime, after an initial transient, the velocity and density fields monotonically reach a spatially inhomogeneous stationary profile, where regions of high shear rate and low density coexist with regions of low shear rate and high density. The steady state is thus maintained by a competition between shear-induced enhancement of density inhomogeneities and relaxation via overdamped sound waves. An analysis of the mechanical equilibrium condition provides a criterion for the existence of steady state solutions. The dynamical evolution of the system is discussed in detail for various boundary conditions, imposing either a constant velocity, shear rate, or stress at the walls.

Rheology of dense suspensions of elastic capsules: normal stresses, yield stress, jamming and confinement effects.

We study the shearing rheology of dense suspensions of elastic capsules, taking aggregation-free red blood cells as a physiologically relevant example. Particles are non-Brownian and interact only via hydrodynamics and short-range repulsive forces. An analysis of the different stress mechanisms in the suspension shows that the viscosity is governed by the shear elasticity of the capsules, whereas the repulsive forces are subdominant. Evidence for a dynamic yield stress above a critical volume fraction is provided and related to the elastic properties of the capsules. The shear stress is found to follow a critical jamming scenario and is rather insensitive to the tumbling-to-tank-treading transition. The particle pressure and normal stress differences display some sensitivity to the dynamical state of the cells and exhibit a characteristic scaling, following the behavior of a single particle, in the tank-treading regime. The behavior of the viscosity in the fluid phase is rationalized in terms of effective medium models. Furthermore, the role of confinement effects, which increase the overall magnitude and enhance the shear-thinning of the viscosity, is discussed.

Crossover from tumbling to tank-treading-like motion in dense simulated suspensions of red blood cells.

Via computer simulations, we provide evidence that the shear rate induced red blood cell tumbling-to-tank-treading transition also occurs at quite high volume fractions, where collective effects are important. The transition takes place as the ratio of effective suspension stress to the characteristic cell membrane stress exceeds a certain value and does not explicitly depend on volume fraction or cell deformability. This value coincides with that for a transition from an orientationally less ordered to a highly ordered phase. The average cell deformation does not show any signature of transition, but rather follows a simple scaling law independent of volume fraction.

Heterogeneous shear in hard sphere glasses.

There is growing evidence that the flow of driven amorphous solids is not homogeneous, even if the macroscopic stress is constant across the system. Via event-driven molecular dynamics simulations of a hard sphere glass, we provide the first direct evidence for a correlation between the fluctuations of the local volume fraction and the fluctuations of the local shear rate. Higher shear rates do preferentially occur at regions of lower density and vice versa. The temporal behavior of fluctuations is governed by a characteristic time scale, which, when measured in units of strain, is independent of shear rate in the investigated range. Interestingly, the correlation volume is also roughly constant for the same range of shear rates. A possible connection between these two observations is discussed.

Rejuvenation in Deep Thermal Cycling of a Generic Model Glass: A Study of Per-Particle Energy Distribution.

We investigate the effect of low temperature (cryogenic) thermal cycling on a generic model glass and observe signature of rejuvenation in terms of per-particle potential energy distributions. Most importantly, these distributions become broader and its average values successively increase when applying consecutive thermal cycles. We show that linear dimension plays a key role for these effects to become visible, since we do only observe a weak effect for a cubic system of roughly one hundred particle diameter but observe strong changes for a rule-type geometry with the longest length being two thousand particle diameters. A consistent interpretation of this new finding is provided in terms of a competition between relaxation processes, which are inherent to glassy systems, and excitation due to thermal treatment. In line with our previous report (Bruns et al., PRR 3, 013234 (2021)), it is shown that, depending on the parameters of thermal cycling, rejuvenation can be either too weak to be detected or strong enough for a clear observation.

Fluid-structure interaction simulation of tissue degradation and its effects on intra-aneurysm hemodynamics.

Tissue degradation plays a crucial role in vascular diseases such as atherosclerosis and aneurysms. Computational modeling of vascular hemodynamics incorporating both arterial wall mechanics and tissue degradation has been a challenging task. In this study, we propose a novel finite element method-based approach to model the microscopic degradation of arterial walls and its interaction with blood flow. The model is applied to study the combined effects of pulsatile flow and tissue degradation on the deformation and intra-aneurysm hemodynamics. Our computational analysis reveals that tissue degradation leads to a weakening of the aneurysmal wall, which manifests itself in a larger deformation and a smaller von Mises stress. Moreover, simulation results for different heart rates, blood pressures and aneurysm geometries indicate consistently that, upon tissue degradation, wall shear stress increases near the flow-impingement region and decreases away from it. These findings are discussed in the context of recent reports regarding the role of both high and low wall shear stress for the progression and rupture of aneurysms.

On the Size Effect of Additives in Amorphous Shape Memory Polymers.

Small additive molecules often enhance structural relaxation in polymers. We explore this effect in a thermoplastic shape memory polymer via molecular dynamics simulations. The additive-to-monomer size ratio is shown to play a key role here. While the effect of additive-concentration on the rate of shape recovery is found to be monotonic in the investigated range, a non-monotonic dependence on the size-ratio emerges at temperatures close to the glass transition. This work thus identifies the additives' size to be a qualitatively novel parameter for controlling the recovery process in polymer-based shape memory materials.

On the Potential Self-Amplification of Aneurysms Due to Tissue Degradation and Blood Flow Revealed From FSI Simulations.

Tissue degradation plays a crucial role in the formation and rupture of aneurysms. Using numerical computer simulations, we study the combined effects of blood flow and tissue degradation on intra-aneurysm hemodynamics. Our computational analysis reveals that the degradation-induced changes of the time-averaged wall shear stress (TAWSS) and oscillatory shear index (OSI) within the aneurysm dome are inversely correlated. Importantly, their correlation is enhanced in the process of tissue degradation. Regions with a low TAWSS and a high OSI experience still lower TAWSS and higher OSI during degradation. Furthermore, we observed that degradation leads to an increase of the endothelial cell activation potential index, in particular, at places experiencing low wall shear stress. These findings are robust and occur for different geometries, degradation intensities, heart rates and pressures. We interpret these findings in the context of recent literature and argue that the degradation-induced hemodynamic changes may lead to a self-amplification of the flow-induced progressive damage of the aneurysmal wall.

A Mechanical Analysis of Chemically Stimulated Linear Shape Memory Polymer Actuation.

In the present work, we study the role of programming strain (50% and 100%), end loads (0, 0.5, 1.0, and 1.5 MPa), and chemical environments (acetone, ethanol, and water) on the exploitable stroke of linear shape memory polymer (SMP) actuators made from ESTANE ETE 75DT3 (SMP­E). Dynamic mechanical thermal analysis (DMTA) shows how the uptake of solvents results in a decrease in the glass temperature of the molecular switch component of SMP-E. A novel in situ technique allows chemically studying triggered shape recovery as a function of time. It is found that the velocity of actuation decreases in the order acetone > ethanol > water, while the exploitable strokes shows the inverse tendency and increases in the order water > ethanol > acetone. The results are interpreted on the basis of the underlying chemical (how solvents affect thermophysical properties) and micromechanical processes (the phenomenological spring dashpot model of Lethersich type rationalizes the behavior). The study provides initial data which can be used for micromechanical modeling of chemically triggered actuation of SMPs. The results are discussed in the light of underlying chemical and mechanical elementary processes, and areas in need of further work are highlighted.

Multi-phase-field simulation of microstructure evolution in metallic foams.

This paper represents a model for microstructure formation in metallic foams based on the multi-phase-field approach. The model allows to naturally account for the effect of additives which prevent two gas bubbles from coalescence. By applying a non-merging criterion to the phase fields and at the same time raising the free energy penalty associated with additives, it is possible to completely prevent coalescence of bubbles in the time window of interest and thus focus on the formation of a closed porous microstructure. On the other hand, using a modification of this criterion along with lower free energy barriers we investigate with this model initiation of coalescence and the evolution of open structures. The method is validated and used to simulate foam structure formation both in two and three dimensions.

Multiple character of non-monotonic size-dependence for relaxation dynamics in polymer-particle and binary mixtures.

Adding plasticizers is a well-known procedure to reduce the glass transition temperature in polymers. It has been recently shown that this effect shows a non-monotonic dependence on the size of additive molecules (2019 J. Chem. Phys. 150 024903). In this work, we demonstrate that, as the size of the additive molecules is changed at fixed concentration, multiple extrema emerge in the dependence of the system's relaxation time on the size ratio. The effect occurs on all relevant length scales including single monomer dynamics, decay of Rouse modes and relaxation of the chain's end-to-end vector. A qualitatively similar trend is found within mode-coupling theoretical results for a binary hard-sphere mixture. An interpretation of the effect in terms of local packing efficiency and coupling between the dynamics of minority and majority species is provided.

Effects of size and elasticity on the relation between flow velocity and wall shear stress in side-wall aneurysms: A lattice Boltzmann-based computer simulation study.

Blood flow in an artery is a fluid-structure interaction problem. It is widely accepted that aneurysm formation, enlargement and failure are associated with wall shear stress (WSS) which is exerted by flowing blood on the aneurysmal wall. To date, the combined effect of aneurysm size and wall elasticity on intra-aneurysm (IA) flow characteristics, particularly in the case of side-wall aneurysms, is poorly understood. Here we propose a model of three-dimensional viscous flow in a compliant artery containing an aneurysm by employing the immersed boundary-lattice Boltzmann-finite element method. This model allows to adequately account for the elastic deformation of both the blood vessel and aneurysm walls. Using this model, we perform a detailed investigation of the flow through aneurysm under different conditions with a focus on the parameters which may influence the wall shear stress. Most importantly, it is shown in this work that the use of flow velocity as a proxy for wall shear stress is well justified only in those sections of the vessel which are close to the ideal cylindrical geometry. Within the aneurysm domain, however, the correlation between wall shear stress and flow velocity is largely lost due to the complexity of the geometry and the resulting flow pattern. Moreover, the correlations weaken further with the phase shift between flow velocity and transmural pressure. These findings have important implications for medical applications since wall shear stress is believed to play a crucial role in aneurysm rupture.

Shear stress in lattice Boltzmann simulations.

A thorough study of shear stress within the lattice Boltzmann method is provided. Via standard multiscale Chapman-Enskog expansion we investigate the dependence of the error in shear stress on grid resolution showing that the shear stress obtained by the lattice Boltzmann method is second-order accurate. This convergence, however, is usually spoiled by the boundary conditions. It is also investigated which value of the relaxation parameter minimizes the error. Furthermore, for simulations using velocity boundary conditions, an artificial mass increase is often observed. This is a consequence of the compressibility of the lattice Boltzmann fluid. We investigate this issue and derive an analytic expression for the time dependence of the fluid density in terms of the Reynolds number, Mach number, and a geometric factor for the case of a Poiseuille flow through a rectangular channel in three dimensions. Comparison of the analytic expression with results of lattice Boltzmann simulations shows excellent agreement.

Multi-phase-field model for surface and phase-boundary diffusion.

The multi-phase-field approach is generalized to treat capillarity-driven diffusion parallel to the surfaces and phase boundaries, i.e., the boundaries between a condensed phase and its vapor and the boundaries between two or multiple condensed phases. The effect of capillarity is modeled via curvature dependence of the chemical potential whose gradient gives rise to diffusion. The model is used to study thermal grooving on the surface of a polycrystalline body. Decaying oscillations of the surface profile during thermal grooving, postulated by Hillert long ago but reported only in few studies so far, are observed and discussed. Furthermore, annealing of multi-nanoclusters on a deformable free surface is investigated using the proposed model. Results of these simulations suggest that the characteristic craterlike structure with an elevated perimeter, observed in recent experiments, is a transient nonequilibrium state during the annealing process.

Non-monotonic effect of confinement on the glass transition.

The relaxation dynamics of glass forming liquids and their structure are influenced in the vicinity of confining walls. This effect has mostly been observed to be a monotonic function of the slit width. Recently, a qualitatively new behaviour has been uncovered by Mittal and coworkers, who reported that the single particle dynamics in a hard-sphere fluid confined in a planar slit varies in a non-monotonic way as the slit width is decreased from five to roughly two particle diametres (Mittal et al 2008 Phys. Rev. Lett. 100 145901). In view of the great potential of this effect for applications in those fields of science and industry, where liquids occur under strong confinement (e.g. nano-technology), the number of researchers studying various aspects and consequences of this non-monotonic behaviour has been rapidly growing. This review aims at providing an overview of the research activity in this newly emerging field. We first briefly discuss how competing mechanisms such as packing effects and short-range attraction may lead to a non-monotonic glass transition scenario in the bulk. We then analyse confinement effects on the dynamics of fluids using a thermodynamic route which relates the single particle dynamics to the excess entropy. Moreover, relating the diffusive dynamics to the Widom's insertion probability, the oscillations of the local dynamics with density at moderate densities are fairly well described. At high densities belonging to the supercooled regime, however, this approach breaks down signaling the onset of strongly collective effects. Indeed, confinement introduces a new length scale which in the limit of high densities and small pore sizes competes with the short-range local order of the fluid. This gives rise to a non-monotonic dependence of the packing structure on confinement, with a corresponding effect on the dynamics of structural relaxation. This non-monotonic effect occurs also in the case of a cone-plate type channel, where the degree of confinement varies with distance from the apex. This is a very promising issue for future research with the possibility of uncovering the existence of alternating glassy and liquid-like domains.