We investigate previously unclarified effects of fluid elasticity on shear-thickening in dilute suspensions in an Oldroyd-B viscoelastic fluid using a novel direct numerical simulation based on the smoothed profile method. Fluid elasticity is determined by the Weissenberg number Wi and by viscosity ratio $1-β=η_p/(η_s+η_p)$ which measures the coupling between the polymer stress and flow: $η_p$ and $η_s$ are the polymer and solvent viscosity, respectively.As $1-β$ increases, while the stresslet does not change significantly compared to that in the $β\to 1$ limit, the growth rate of the normalized polymer stress with Wi was suppressed.Analysis of flow and conformation dynamics around a particle for different $β$ reveals that at large $1-β$, polymer stress modulates flow, leading to suppression of polymer stretch.This effect of $β$ on polymer stress development indicates complex coupling between fluid elasticity and flow, and is essential to understand the rheology and hydrodynamic interactions in suspensions in viscoelastic media.
For the clarification of the routes to elasto-inertial turbulence (EIT), it is essential to understand how viscoelasticity modulates coherent flow structures including the longitudinal vortices. We focused on a rotating plane Couette flow that provides two-dimensional (2D) roll cells for the steady laminar Newtonian-fluid case, and we investigated how the steady longitudinal vortices are modulated by viscoelasticity at different Weissenberg numbers. The viscoelasticity was found to induce an unsteady flow state where the 2D roll-cell structure was periodically enhanced and damped with a consta…
We study numerically two-dimensional creeping viscoelastic flow past a biperiodic square array of cylinders within the Oldroyd B, FENE-CR and FENE-P constitutive models of dilute polymer solutions. Our results capture the initial mild decrease then dramatic upturn ('thickening') seen experimentally in the drag coefficient as a function of increasing Weissenberg number. By systematically varying the porosity of the flow geometry, we demonstrate two qualitatively different mechanisms underpinning this thickening effect: one that operates in the highly porous case of widely spaced obstacles, and …
The effects of viscoelasticity on the dynamics and break-up of fluid threads in microfluidic T-junctions are investigated using numerical simulations of dilute polymer solutions at changing the Capillary number ($\mbox {Ca}$), i.e. at changing the balance between the viscous forces and the surface tension at the interface, up to $\mbox{Ca} \approx 3 \times 10^{-2}$. A Navier-Stokes (NS) description of the solvent based on the lattice Boltzmann models (LBM) is here coupled to constitutive equations for finite extensible non-linear elastic dumbbells with the closure proposed by Peterlin (FENE-P …
Synchronization of two actuated sheets serves as a simple model for the interaction between flagellated microswimmers. Various factors, including inertia, sheet elasticity, and fluid viscoelasticity, have been suggested to facilitate the synchronization of two sheets; however, the importance of different contributions to this process still remains unclear. We perform a systematic investigation of competing effects of inertia, sheet elasticity, and fluid viscoelasticity on the synchronization of two sheets. Characteristic time $τ^\mathrm{s}$ for the synchronization caused by inertial effects is…
To elucidate the key factor for the quantitative prediction of the shear-thickening in suspensions in viscoelastic fluids, direct numerical simulations of many-particle suspensions in a multi-mode Oldroyd-B fluid are performed using the smoothed profile method. Suspension flow under simple shear flow is solved under periodic boundary conditions by using Lees--Edwards boundary conditions for particle dynamics and a time-dependent oblique coordinate system that evolves with mean shear flow for fluid dynamics. Semi-dilute many-particle suspensions up to a particle volume fraction of 0.1 are inves…
Predictions of the QLV (Quasi-Linear Viscoelastic) constitutive law are compared with those of the ABAQUS viscoelastic model for two simple motions in order to highlight, in particular, their very different dissipation rates and certain shortcomings of the ABAQUS model.
Ultrathin polymer films on non-wettable substrates display dynamic features which have been attributed to either viscoelastic or slip effects. Here we show that in the weak and strong slip regime effects of viscoelastic relaxation are either absent or not distinguishable from slip effects. Strong-slip modifies the fastest unstable mode in a rupturing thin film, which questions the standard approach to reconstruct the effective interface potential from dewetting experiments.
Active chiral viscoelastic materials exhibit elastic responses perpendicular to the applied stresses, referred to as odd elasticity. We use a covariant formulation of viscoelasticity combined with an entropy production analysis to show that odd elasticity is not only present in active systems but also in broad classes of passive chiral viscoelastic fluids. In addition, we demonstrate that linear viscoelastic chiral solids do require activity in order to manifest odd elastic responses. In order to model the phenomenon of passive odd viscoelasticity we propose a chiral extension of Jeffreys mode…
Many metastable complex fluids such as colloidal glasses and gels show distinct nonlinear viscoelasticity with increasing oscillatory-strain amplitude; the storage modulus decreases monotonically as the strain amplitude increases whereas the loss modulus has a distinct peak before it decreases at larger strains. We present a qualitative argument to explain this ubiquitous behavior and use mode coupling theory (MCT) to confirm it. We compare theoretical predictions to the measured nonlinear viscoelasticity in a dense hard sphere colloidal suspensions; reasonable agreement is obtained. The argum…
We show that a viscoelastic dispersion relation for shear waves in normal $^{3}$He at low temperatures follows directly from the Landau theory of normal Fermi liquids. This theoretical result is in accord with the experimental observations of propagating high frequency shear waves that identify normal $^{3}$He as a viscoelastic substance.
We consider models for elastic liquids, such as solutions of flexible polymers. They introduce a relaxation time $λ$ into the system, over which stresses relax. We study the kinematics of the problem, and clarify the relationship between Lagrangian and Eulerian descriptions, thereby showing which polymer models correspond to a nonlinear elastic deformation in the limit $λ\rightarrow\infty$. This allows us to split the change in elastic energy into reversible and dissipative parts, and thus to write an equation for the total energy, the sum of kinetic and elastic energies. As an illustration, w…
We investigate the break-up of Newtonian/viscoelastic droplets in a viscoelastic/Newtonian matrix under the hydrodynamic conditions of a confined shear flow. Our numerical approach is based on a combination of Lattice-Boltzmann models (LBM) and Finite Difference (FD) schemes. LBM are used to model two immiscible fluids with variable viscosity ratio (i.e. the ratio of the droplet to matrix viscosity); FD schemes are used to model viscoelasticity, and the kinetics of the polymers is introduced using constitutive equations for viscoelastic fluids with finitely extensible non-linear elastic dumbbe…
Many manmade and naturally occurring materials form viscoelastic solids. The increasing use of biologically inspired elastomeric material and the extreme mechanical response these elastomers offer drive the need for a better, more intuitive and quantitative understanding of the mechanical response of such continua. This is in particular important in determining the stability of viscoelastic structure over time where in lieu of robust rules we often must resort to simulations. In this work we put forward a metric description of viscoelasticity in which the continua is characterized by temporall…
Thixotropy, anti-thixotropy, and viscoelasticity are three types of time-dependent dynamics that involve fundamentally different underlying physical processes. Yet distinguishing them can be very challenging, which hinders the understanding of structure-property relations. Here we show that hysteresis is a promising technique to contrast the three dynamics by exploring signatures of the most basic thixotropic, anti-thixotropic, and nonlinear viscoelastic models. From these signatures, using shear-rate controlled ramps that begin and end at high shear rates, we identify two distinguishing featu…
This second part of paper develops a theory of linear viscoelastic nematodynamics applicable to LCP. The viscous and elastic nematic components in theory are described by using the LEP approach for viscous nematics and de Gennes free energy for weakly elastic nematic elastomers. The case of applied external magnetic field exemplifies the occurrence of non-symmetric stresses. In spite of multi- (10) parametric character of the theory, the use of nematic operators presents it in an elegant form. When the magnetic field is absent, the theory is simplified for symmetric case with 6 parameters, and…
The theory of quasi-linear viscoelasticity (QLV) is modified and developed for transversely isotropic (TI) materials under finite deformation. For the first time, distinct relaxation responses are incorporated into an integral formulation of nonlinear viscoelasticity, according to the physical mode of deformation. The theory is consistent with linear viscoelasticity in the small strain limit and makes use of relaxation functions that can be determined from small-strain experiments, given the time/deformation separability assumption. After considering the general constitutive form applicable to…
Recent experiments show a strong rotational-diffusion enhancement for self-propelled microrheological probes in colloidal glasses. Here, we provide microscopic understanding using simulations with a frictional probe-medium coupling that converts active translation into rotation. Diffusive enhancement emerges from the medium's disordered structure and peaks at a second-order transition in the number of contacts. Our results reproduce the salient features of the colloidal glass experiment and support an effective description that is applicable to a broader class of viscoelastic suspensions.
The overdamped (inertialess) dumbbell model is widely utilized to study rheological properties of polymers or other soft matters. In most cases, the effect of inertia is merely neglected because the momentum relaxation is much faster than the bond relaxation. We theoretically analyze the effect of inertia on the linear viscoelasticity of the harmonic dumbbell model. We show that the momentum and bond relaxation modes are kinetically coupled and the inertia can affect the bond relaxation if the momentum relaxation is not sufficiently fast. We derive an overdamped Langevin equation for the dumbb…
The progressive onset of slip at the wall, which corresponds to a slip length increasing with the solicitation time before reaching a plateau, has been investigated for model viscoelastic polymer solutions, allowing one to vary the longest relaxation time while keeping constant solid - fluid interactions. A hydrodynamic model based on a Maxwell fluid and the classical Navier's hypothesis of a linear response for the friction stress at the interface fully accounts for the data, without any adjustable parameter. No viscoelastic response needs be postulated for the friction, reflecting the local …
We survey the linear viscoelasticity of a new type of transient network: bridged wormlike micelles, whose structure has been characterized recently [Ramos and Ligoure, (2007)]. This composite material is obtained by adding telechelic copolymers (water-soluble chains with hydrophobic stickers at each extremity) to a solution of entangled wormlike micelles (WM). For comparison, naked WM and WM decorated by amphiphilic copolymers are also investigated. While these latter systems exhibit almost a same single ideal Maxwell behavior, solutions of bridged WM can be described as two Maxwell fluids com…
The mechanical response of active media ranging from biological gels to living tissues is governed by a subtle interplay between viscosity and elasticity. In this Letter, we generalize the canonical Kelvin-Voigt and Maxwell models to active viscoelastic media that break both parity and time-reversal symmetries. The resulting continuum theories exhibit viscous and elastic tensors that are both antisymmetric, or odd, under exchange of pairs of indices. We analyze how these parity violating viscoelastic coefficients determine the relaxation mechanisms and wave-propagation properties of odd materi…
A universal description is proposed for generic viscoelastic systems with a single relaxation time. Foliation preserving diffeomorphisms are introduced as an underlying symmetry which naturally interpolates between the two extreme limits of elasticity and fluidity. The symmetry is found to be powerful enough to determine the dynamics in the first order of strains.
Motivated by roughness-induced adhesion enhancement (toughening and strengthening) in low modulus materials, we study the detachment of a sphere from a substrate in the presence of both viscoelastic dissipation at the contact edge, and roughness in the form of a single axisymmetric waviness. We show that the roughness-induced enhancement found by Guduru and coworkers for the elastic case (i.e. at very small detachment speeds) tends to disappear with increasing speeds, where the viscoelastic effect dominates and the problem approaches that of a smooth sphere. This is in qualitative agreement wi…
We investigate the linear viscoelasticity of polymer gels produced by the dispersion of gluten proteins in water:ethanol binary mixtures with various ethanol contents, from pure water to 60% v/v ethanol. We show that the complex viscoelasticity of the gels exhibits a time/solvent composition superposition principle, demonstrating the self-similarity of the gels produced in different binary solvents. All gels can be regarded as near critical gels with characteristic rheological parameters, elastic plateau and characteristic relaxation time, which are related one to another, as a consequence of …
We consider an immersed elastic body that is actively driven through a structured fluid by a motor or an external force. The behavior of such a system generally cannot be solved analytically, necessitating the use of numerical methods. However, current numerical methods omit important details of the microscopic structure and dynamics of the fluid, which can modulate the magnitudes and directions of viscoelastic restoring forces. To address this issue, we develop a simulation platform for modeling viscoelastic media with tensorial elasticity. We build on the lattice Boltzmann algorithm and inco…
When submitted to a magnetic field, micron size wires with superparamagnetic properties behave as embedded rheometers and represent interesting sensors for micro-rheology. Here we use rotational magnetic spectroscopy to measure the shear viscosity of the cytoplasm of living cells. We address the question of whether the cytoplasm is a viscoelastic liquid or a gel. The main result of the study is the observation of a rotational instability between a synchronous and an asynchronous regime of rotation, found for murine fibroblasts and human cancer cells. For wires of susceptibility 3.6, the transi…
We describe a high-resolution, high-bandwidth technique for determining the local viscoelasticity of soft materials such as polymer gels. Loss and storage shear moduli are determined from the power spectra of thermal fluctuations of embedded micron-sized probe particles, observed with an interferometric microscope. This provides a passive, small-amplitude measurement of rheological properties over a much broader frequency range than previously accessible to microrheology. We study both F-actin biopolymer solutions and polyacrylamide (PAAm) gels, as model semiflexible and flexible systems, resp…
This is an integrated experimental and theoretical study of the dynamics and rheology of self-crosslinked, slightly charged, temperature responsive soft Poly(N-isopropylacrylamide) (pNIPAM) microgels over a wide range of concentration and temperature spanning the sharp change in particle size and intermolecular interactions across the lower critical solution temperature (LCST). Dramatic, non-monotonic changes in viscoelasticity are observed with temperature, with distinctive concentration dependences in the dense fluid, glassy, and soft-jammed states. Motivated by our experimental observations…
We have advanced our previous static theory of polymer entanglement involving an extended Cahn-Hilliard functional, to include time-dependent dynamics. We go beyond the Gaussian approximation, to the one-loop level, to compute the frequency dependent storage and loss moduli of the system. The three parameters in our theory are obtained by fitting to available experimental data on polystyrene melts of various chain lengths. This provides a physical representation of the parameters in terms of the chain length of the system. We discuss the importance of the various terms in our energy functional…
Hamburg University of Technology（汉堡工业大学）；Helmholtz-Zentrum Hereon（亥姆霍兹联合会赫尔岑研究中心）
The constitutive behavior of polymeric materials is often modeled by finite linear viscoelastic (FLV) or quasi-linear viscoelastic (QLV) models. These popular models are simplifications that typically cannot accurately capture the nonlinear viscoelastic behavior of materials. For example, the success of attempts to capture strain rate-dependent behavior has been limited so far. To overcome this problem, we introduce viscoelastic Constitutive Artificial Neural Networks (vCANNs), a novel physics-informed machine learning framework for anisotropic nonlinear viscoelasticity at finite strains. vCAN…
We develop topological methods for characterizing the relationship between polymer chain entanglement and bulk viscoelastic responses. We introduce generalized Linking Number and Writhe characteristics that are applicable to open linear chains. We investigate the rheology of polymeric chains entangled into weaves with varying topologies and levels of chain density. To investigate viscoelastic responses, we perform non-equilibrium molecular simulations over a range of frequencies using sheared Lees-Edwards boundary conditions. We show how our topological characteristics can be used to capture k…
We present a simulation study of colloidal particles having very short range attractions. In particular, we investigate the interplay between the effective attractive range and the viscoelastic properties of the gels that form when the temperature of the system is sufficiently low. Using Brownian dynamics simulations we study particles with different size and interaction range, and characterize the mechanical properties of the gels by performing small amplitude oscillatory and transient starts-up shear simulations. We found that the effective attractive range is a key parameter affecting the g…
Thermally activated transitions are ubiquitous in nature, occurring in complex environments which are typically conceived as ideal viscous fluids. We report the first direct observations of a Brownian bead transiting between the wells of a bistable optical potential in a viscoelastic fluid with a single long relaxation time. We precisely characterize both the potential and the fluid, thus enabling a neat comparison between our experimental results and a theoretical model based on the generalized Langevin equation. Our findings reveal a drastic amplification of the transition rates compared to …
Soft tissues are complex media, they display a wide range of mechanical properties such as anisotropy and non-linear stress-strain behaviour. They undergo large deformations and they exhibit a time-dependent mechanical behaviour, i.e. they are viscoelastic. In this chapter we review the foundations of the linear viscoelastic theory and the theory of Quasi-Linear Viscoelasticity (QLV) in view of developing new methods to estimate the viscoelastic properties of soft tissues through model fitting. To this aim, we consider the simple torsion of a viscoelastic Mooney-Rivlin material in two differen…
We present a theoretical framework for the linear and nonlinear visco-elastic properties of reversibly crosslinked networks of semiflexible polymers. In contrast to affine models where network strain couples to the polymer end-to-end distance, in our model strain rather serves to locally distort the network structure. This induces bending modes in the polymer filaments, the properties of wich are slaved to the surrounding network structure. Specifically, we investigate the frequency-dependent linear rheology, in particular in combination with crosslink binding/unbinding processes. We also deve…
Polymer gels behave as soft viscoelastic solids and exhibit a generic nonlinear mechanical response characterized by pronounced stiffening prior to irreversible failure, most often through macroscopic fractures. Here, we aim at capturing the latter scenario for a protein gel using a nonlinear integral constitutive equation built upon ($i$) the linear viscoelastic response of the gel, here well described by a power-law relaxation modulus, and ($ii$) the nonlinear viscoelastic properties of the gel, encoded into a "damping function". Such formalism predicts quantitatively the gel mechanical resp…
Characterizing the softness of deformable materials having partial elastic and partial viscous behaviour via soft lubrication experiments has emerged as a versatile and robust methodology in recent times. However, a straightforward extension of the classical elastohydrodynamic lubrication theory that is commonly employed for characterizing elastic materials turns out to be rather inadequate in explaining the response of such viscoelastic materials subjected to dynamic loading conditions, despite adhering to a mathematically acceptable framework via the complex Young's modulus as a material pro…
The effect of fat content in cheese curds on their rheological properties was examined using dynamic shear measurements. Surplus fat addition to milk samples caused two distinct types of changes in the temperature dependence of the viscoelastic moduli of resultant curds. The first was a significant reduction in the moduli over a wide temperature range, which is attributed to the presence of liquefied fat globules within the milk protein network. The second was the excess contribution to the low-temperature moduli owing to the reinforcing effect of solidified fat globules. An upward shift in th…
We show using Brownian dynamics simulations and theory how the shear relaxation modulus G(t) of dilute solutions of relatively stiff semiflexible polymers differs qualitatively from that of rigid rods. For chains shorter than their persistence length, G(t) exhibits three time regimes: At very early times, when the longitudinal deformation is affine, G(t) \sim t^{-3/4}. Over a broad intermediate regime, during which the chain length relaxes, G(t) \sim t^{-5/4}. At long times, $G(t) mimics that of rigid rods. A model of the polymer as an effectively extensible rod with a frequency dependent elas…
This paper discusses the possibility of identifying the shear and structure relaxation kernels in glassy materials by means of a single, simple and non-intrusive experiment. The material should be thermorheologically simple and the kernels expressed in the form of Prony series. The experiment considered consists in measuring the thickness variations over time of a flat sample cooled symmetrically from both side from a temperature above the glass transition temperature down to room temperature. The comparison of experimental observations with theoretically calculated responses allows the identi…
We have developed a new technique to measure viscoelasticity in soft materials such as polymer solutions, by monitoring thermal fluctuations of embedded probe particles using laser interferometry in a microscope. Interferometry allows us to obtain power spectra of fluctuating beads from 0.1 Hz to 20 kHz, and with sub-nanometer spatial resolution. Using linear response theory, we determined the frequency-dependent loss and storage shear moduli up to frequencies on the order of a kHz. Our technique measures local values of the viscoelastic response, without actively straining the system, and is …
Emergent odd viscoelasticity in chiral soft glassy materials
University of Göttingen（哥廷根大学）；Ecole Polytechnique de l’Université de Nantes, LTeN, U6607, Nantes Université（南特大学理工学院，LTeN，U6607）；King’s College London（伦敦国王学院）
Biological macromolecules have complex and non-trivial energy landscapes, endowing them a unique conformational adaptability and diversity in function. Hence, understanding the processes of elasticity and dissipation at the nanoscale is important to molecular biology and also emerging fields such as nanotechnology. Here we analyse single molecule fluctuations in an atomic force microscope (AFM) experiment using a generic model of biopolymer viscoelasticity that importantly includes sources of local `internal' conformational dissipation. Comparing two biopolymers, dextran and cellulose, polysac…
