The toughness of a polymer material can increase significantly if two networks are combined into one material. This toughening effect is a consequence of a transition from a brittle to a ductile failure response. Although this transition and the accompanying toughening effect have been demonstrated in hydrogels first, the concept has been proven effective in elastomers and in macroscopic composites as well. This suggests that the transition is not caused by a specific molecular architecture, but rather by a general physical principle related to the mechanical interplay between two interpenetrating networks. Here we employ theory and computer simulations, inspired by this general principle, to investigate how disorder controls the brittle-to-ductile transition both at the macroscopic and the microscopic level. A random spring network model featuring two different spring types, enables us to study the joined effect of initial disorder and network-induced stress heterogeneity on this transition. We reveal that a mechanical force balance gives a good description of the brittle-to-ductile transition. In addition, the inclusion of disorder in the spring model predicts four different failure regimes along the brittle-to-ductile response in agreement with experimental findings. Finally, we show that the network structure can result in stress concentration, diffuse damage and loss of percolation depending on the failure regime. This work thus provides a framework for the design and optimization of double network materials and underlines the importance of network structure in the toughness of polymer materials.
We consider a microscopic model for the failure of soft adhesives in tension based on ideas of bond rupture under dynamic loading. Focusing on adhesive failure under loading at constant velocity, we demonstrate that bi-modal curves of stress against strain may occur due to effects of finite polymer chain or bond length and characterise the loading conditions under which such bi-modal behaviour is observed. The results of this analysis are in qualitative agreement with experiments performed on unconfined adhesives in which failure does not occur by cavitation.
With the eventual aim of describing flowing elasto-plastic materials, we focus on the elementary brick of such a flow, a plastic event, and compute the long-range perturbation it elastically induces in a medium submitted to a global shear strain. We characterize the effect of a nearby wall on this perturbation, and quantify the importance of finite size effects. Although for the sake of simplicity most of our explicit formulae deal with a 2D situation, our statements hold for 3D situations as well.
Material failure is ubiquitous, with implications from geology to everyday life and material science. It often involves sudden, unpredictable events, with little or no macroscopically detectable precursors. A deeper understanding of the microscopic mechanisms eventually leading to failure is clearly required, but experiments remain scarce. Here, we show that the microscopic dynamics of a colloidal gel, a model network-forming system, exhibit dramatic changes that precede its macroscopic failure by thousands of seconds. Using an original setup coupling light scattering and rheology, we simultan…
A recent derivation [P.H. Mott and C.M. Roland, Phys. Rev. B 80, 132104 (2009).] of the bounds on Poisson's ratio, v, for linearly elastic materials showed that the conventional lower limit, -1, is wrong, and that v cannot be less than 0.2 for classical elasticity to be valid. This is a significant result, since it is precisely for materials having small values of v that direct measurements are not feasible, so that v must be calculated from other elastic constants. Herein we measure directly Poisson's ratio for four materials, two for which the more restrictive bounds on v apply, and two havi…
We discuss a class of models for particulate gels in which the particle contacts are described by an effective interaction combining a two-body attraction and a three-body angular repulsion. Using molecular dynamics, we show how varying the model parameters allows us to sample, for a given gelation protocol, a variety of gel morphologies. For a specific set of the model parameters, we identify the local elastic structures that get interlocked in the gel network. Using the analytical expression of their elastic energy from the microscopic interactions, we can estimate their contribution to the …
The mechanical properties of soft matter are of great importance in countless applications, in addition of being an active field of academic research. Given the relative ease with which soft materials can be deformed, their non-linear behavior is of particular relevance. Large loads eventually result in material failure. In this Perspective article, we discuss recent work aiming at detecting precursors of failure by scrutinizing the microscopic structure and dynamics of soft systems under various conditions of loading. In particular, we show that the microscopic dynamics is a powerful indicato…
Selectively heating a microscopic colloidal particle embedded in a soft elastic matrix is a situation of high practical relevance. For instance, during hyperthermic cancer treatment, cell tissue surrounding heated magnetic colloidal particles is destroyed. Experiments on soft elastic polymeric matrices suggest a very long-ranged, non-decaying radial component of the thermophoretically induced displacement fields around the microscopic heat centers. We theoretically confirm this conjecture using a macroscopic hydrodynamic two-fluid description. Both, thermophoretic and elastic effects are inclu…
We describe simulations of a microscopic elastic filament immersed in a fluid and subject to a uniform external force. Our method accounts for the hydrodynamic coupling between the flow generated by the filament and the friction force it experiences. While models that neglect this coupling predict a drift in a straight configuration, our findings are very different. Notably, a force with a component perpendicular to the filament axis induces bending and perpendicular alignment. Moreover, with increasing force we observe four shape regimes, ranging from slight distortion to a state of tumbling …
A fundamental assumption in our understanding of material rheology is that when microscopic deformations are reversible, the material responds elastically to external loads. Plasticity, i.e. dissipative and irreversible macroscopic changes in a material, is assumed to be the consequence of irreversible microscopic events. Here we show direct evidence for reversible plastic events at the microscopic scale in both experiments and simulations of two-dimensional foam. In the simulations, we demonstrate a link between reversible plastic rearrangement events and pathways in the potential energy land…
The failure of brittle solids involves, before macroscopic rupture, power-law distributed avalanches of local rupture events whereby microcracks nucleate and grow, which are also observed in for an elastic interface evolving in a non-homogeneous medium. For this reason, it is tempting to relate failure to the depinning of an elastic interface. Here we compute the elastic kernel of the interface representing the damage field of a brittle solid. In the case of a damage model of rupture under compression, which implements the Mohr-Coulomb criterion at the local scale, we show that the elastic ker…
Cracks, the major vehicle for material failure, tend to accelerate to high velocities in brittle materials. In three-dimensions, cracks generically undergo a micro-branching instability at about 40% of their sonic limiting velocity. Recent experiments showed that in sufficiently thin systems cracks unprecedentedly accelerate to nearly their limiting velocity without micro-branching, until they undergo an oscillatory instability. Despite their fundamental importance and apparent similarities to other instabilities in condensed-matter physics and materials science, these dynamic fracture instabi…
Under mechanical deformation, most materials exhibit both elastic and fluid (or plastic) responses. No existing formalism derived from microscopic principles encompasses both their fluid-like and solid-like aspects. We define the {\it statistical texture tensor} to quantify the intuitive notion of stored deformation. This tensor links microscopic and macroscopic descriptions of the material, and extends the definition of elastic strain.
By mixing glass beads with a curable polymer we create a well-defined cohesive granular medium, held together by solidified, and hence elastic, capillary bridges. This material has a geometry similar to a wet packing of beads, but with an additional control over the elasticity of the bonds holding the particles together. We show that its mechanical response can be varied over several orders of magnitude by adjusting the size and stiffness of the bridges, and the size of the particles. We also investigate its mechanism of failure under unconfined uniaxial compression in combination with in situ…
We study the influence of thermal fluctuations on the fracture of elastic networks, via simulations of the uniaxial extension of central-force spring networks with varying rigidity, i.e. connectivity. Studying their failure response, both at the macroscopic and microscopic level, we find that an increase in temperature corresponds to a more homogeneous stress (re)distribution and induces thermally activated failure of springs. As a consequence, the material strength decreases upon increasing temperature, the damage is spread over larger lengthscales and a more ductile fracture process is obser…
We present a visco-elastic coupling model between caked spheres, suitable for DEM simulations, which incorporates the different loading mechanisms (tension, shear, bending, torsion) in a combined manner and allows for a derivation of elastic and failure properties on a common basis. In pull, shear, and torsion failure tests with agglomerates of up to 10000 particles, we compare the failure criterion to different approximative variants of it, with respect to accuracy and computational cost. The failure of the agglomerates, which behave according to elastic parameters derived from the contact el…
In this paper we study deformation, failure and breakage of visco-elastic thin films of aging laponite suspension under tensile deformation field. Aqueous suspension of laponite is known to undergo waiting time dependent evolution of its micro-structure, also known as aging, which is accompanied by an increase in the elastic modulus and relaxation time. In the velocity controlled tensile deformation experiments, we observed that the dependence of force and dissipated energy on velocity and initial thickness of the film is intermediate to a Newtonian fluid and a yield stress fluid. For a fixed …
Starting from a microscopic model of randomly cross-linked particles with quenched disorder, we calculate the Laudau-Wilson free energy S for arbitrary cross-link densities. Considering pure shear deformations, S takes the form of the elastic energy of an isotropic amorphous solid state, from which the shear modulus can be identified. It is found to be an universal quantity, not depending on any microscopic length-scales of the model.
We employ a first principles, force-level approach to self-consistently construct the anharmonic tube confinement field for entangled fluids of rigid needles and for primitive-path (PP) level chains in two limiting situations where chain stretching is assumed to either completely relax or remain unrelaxed. The influence of shear and extensional deformation and polymer orientation is determined in a nonlinear elastic limit where dissipative relaxation processes are intentionally neglected. For needles and PP-level chains, a Gaussian analysis of transverse polymer dynamical fluctuations predicts…
Disordered solids often change their elastic response as they slowly age. Using experiments and simulations, we study how aging disordered planar networks under an applied stress affects their nonlinear elastic response. We are able to modify dramatically the elastic properties of our systems in the non-linear regime. Using simulations, we study two models for the microscopic evolution of properties of such a material; the first considers changes in the material strength while the second considers distortions in the microscopic geometry. Both models capture different aspects of the experiments…
Randomly crosslinked macromolecules undergo a liquid-to-amorphous solid phase transition at a critical crosslink concentration. This transition has two main signatures: the random localization of a fraction of the monomers and the emergence of a nonzero static shear modulus. In this article, a semi-microscopic statistical mechanical theory of the elastic properties of the amorphous solid state is developed. This theory takes into account both quenched disorder and thermal fluctuations, and allows for the direct computation of the free energy change of the sample due to a given macroscopic shea…
In complex crystals close to melting or at finite temperatures, different types of defects are ubiquitous and their role becomes relevant in the mechanical response of these solids. Conventional elasticity theory fails to provide a microscopic basis to include and account for the motion of point-defects in an otherwise ordered crystalline structure. We study the elastic properties of a point-defect rich crystal within a first-principles theoretical framework derived from microscopic equations of motion. This framework allows us to make specific predictions pertaining to the mechanical properti…
The elastic deformation of a soft solid induced by capillary forces crucially relies on the excess stress inside the solid-liquid interface. While for a liquid-liquid interface this "surface stress" is strictly identical to the "surface free energy", the thermodynamic Shuttleworth equation implies that this is no longer the case when one of the phases is elastic. Here we develop a microscopic model that incorporates enthalpic interactions and entropic elasticity, based on which we explicitly compute the surface stress and surface free energy. It is found that the compressibility of the interfa…
Plasticity in soft amorphous materials typically involves collective deformation patterns that emerge upon intense shearing. The microscopic basis of amorphous plasticity has been commonly established through the notion of "Eshelby"-type events, localized abrupt rearrangements that induce flow in the surrounding material via non-local elastic-type interactions. This universal mechanism in flowing disordered solids has been proposed despite their diversity in terms of scales, microscopic constituents, or interactions. However, we argue that the presence of frictional interactions in granular so…
In this work a periodic crystal with point defects is described in the framework of linear response theory for broken symmetry states using correlation functions and Zwanzig-Mori equations. The main results are microscopic expressions for the elastic constants and for the coarse-grained density, point-defect density, and displacement field, which are valid in real crystals, where vacancies and interstitials are present. The coarse-grained density field differs from the small wave vector limit of the microscopic density. In the long wavelength limit, we recover the phenomenological description …
Adding perforations to a continuum sheet allows new modes of deformation, and thus modifies its elastic behavior. The failure behavior of such a perforated sheet is explored, using a model experimental system: a material containing a one-dimensional array of rectangular holes. In this model system, a transition in failure mode occurs as the spacing and aspect ratio of the holes are varied: rapid failure via a running crack is completely replaced by quasi-static failure which proceeds via the breaking of struts at random positions in the array of holes. I demonstrate that this transition can be…
In the vicinity of their glass transition, dense colloidal suspensions acquire elastic properties over experimental timescales. We investigate the possibility of a visco-elastic flow instability in curved geometry for such materials. To this end, we first present a general strategy extending a first-principles approach based on projections onto slow variables (so far restricted to strictly homogeneous flow) in order to handle inhomogeneities. In particular, we separate the advection of the microstructure by the flow, at the origin of a fluctuation advection term, from the intrinsic dynamics. O…
Unlike macroscopic multistable mechanical systems such as snap bracelets or elastic shells that must be physically manipulated into various conformations, microscopic systems can undergo spontaneous conformation switching between multistable states due to thermal fluctuations. Here we investigate the statistical mechanics of shape transitions in small elastic elliptical plates and shells driven by noise. By assuming that the effects of edges are small, which we justify exactly for plates and shells with a lenticular section, we decompose the shapes into a few geometric modes whose dynamics are…
The mechanics of cohesive or cemented granular materials is complex, combining the heterogeneous responses of granular media, like force chains, with clearly defined material properties. Here, we use a discrete element model (DEM) simulation, consisting of an assemblage of elastic particles connected by softer but breakable elastic bonds, to explore how this class of material deforms and fails under uniaxial compression. We are particularly interested in the connection between the microscopic interactions among the grains or particles and the macroscopic material response. To this end, the pro…
What characterises a solid is its way to respond to external stresses. Ordered solids, such crystals, display an elastic regime followed by a plastic one, both well understood microscopically in terms of lattice distortion and dislocations. For amorphous solids the situation is instead less clear, and the microscopic understanding of the response to deformation and stress is a very active research topic. Several studies have revealed that even in the elastic regime the response is very jerky at low temperature, resembling very much the one of disordered magnetic materials. Here we show that in…
A variety of polymeric surfaces, such as anti-corrosion coatings and polymer-modified asphalts, are prone to blistering when exposed to moisture and air. As water and oxygen diffuse through the material, dissolved species are produced, which generate osmotic pressure that deforms and debonds the coating.These mechanisms are experimentally well-supported; however, comprehensive macroscopic models capable of predicting the formation osmotic blisters, without extensive data-fitting, is scant. Here, we develop a general mathematical theory of blistering and apply it to the failure of anti-corrosio…
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…
Solid interfaces have intrinsic elasticity. However, in most experiments, this is obscured by bulk stresses. Through microscopic observations of the contact-line geometry of a partially wetting droplet on an anisotropically stretched substrate, we measure two surface-elastic constants that quantify the linear dependence of the surface stress of a soft polymer gel on its strain. With these two parameters, one can predict surface stresses for general deformations of the material in the linear-elastic limit.
In soft matter systems the local displacement field can be accessed directly by video microscopy enabling one to compute local strain fields and hence the elastic moduli using a coarse-graining procedure. We study this process for a simple triangular lattice of particles connected by harmonic springs in two-dimensions. Coarse-graining local strains obtained from particle configurations in a Monte Carlo simulation generates non-trivial, non-local strain correlations (susceptibilities), which may be understood within a generalized, Landau type elastic Hamiltonian containing up to quartic terms i…
We use molecular dynamics to study the vibrations of a thermally fluctuating two-dimensional elastic membrane clamped at both ends. We directly extract the eigenmodes from resonant peaks in the frequency domain of the time-dependent height and measure the dependence of the corresponding eigenfrequencies on the microscopic bending rigidity of the membrane, taking care also of the subtle role of thermal contraction in generating a tension when the projected area is fixed. At finite temperatures we show that the effective (macroscopic) bending rigidity tends to a constant as the bare bending rigi…
The rigidity of a network of elastic beams crucially depends on the specific details of its structure. We show both numerically and theoretically that there is a class of isotropic networks which are stiffer than any other isotropic network with same density. The elastic moduli of these \textit{stiffest elastic networks} are explicitly given. They constitute upper-bounds which compete or improve the well-known Hashin-Shtrikman bounds. We provide a convenient set of criteria (necessary and sufficient conditions) to identify these networks, and show that their displacement field under uniform lo…
Inspired by experiments on the actin driven propulsion of micrometer sized beads we develop and study a minimal mechanical model of a two-dimensional network of stiff elastic filaments grown from the surface of a cylinder. Starting out from a discrete model of the network structure and of its microscopic mechanical behavior we derive a macroscopic constitutive law by homogenization techniques. We calculate the axisymmetric equilibrium state and study its linear stability depending on the microscopic mechanical properties. We find that thin networks are linearly stable, whereas thick networks a…
In compressive fracture of dry plexiform bone, we examine the individual roles of overall mean porosity, the connectivity of the porosity network, and the elastic as well as the failure properties of the non-porous matrix, using a random spring network model. Porosity network structure is shown to reduce the compressive strength by upto 30%. However, the load bearing capacity increases with increase in either of the matrix properties - elastic modulus or failure strain threshold. To validate the porosity-based RSNM model with available experimental data, bone-specific failure strain thresholds…
Solids built out of active components can exhibit non-reciprocal elastic coefficients that give rise to non-Hermitian wave phenomena. Here, we investigate non-Hermitian effects present at the boundary of two-dimensional active elastic media obeying two general assumptions: their microscopic forces conserve linear momentum and arise only from static deformations. Using continuum equations, we demonstrate the existence of the non-Hermitian skin effect in which the boundary hosts an extensive number of localized modes. Furthermore, lattice models reveal non-Hermitian topological transitions media…
The insurgence of compression induces wrinkling in actuation devices based on EAPs thin films leading to a sudden decrease of performances up to failure. Based on the classical tension field theory for thin elastic membranes, we provide a general framework for the analysis of the insurgence of in-plane compression in membranes of electroactive polymers (EAPs). Our main result is the deduction of a (voltage-dependent) domain in the stretch space which represents tensile configurations. Under the assumption of Mooney-Rivlin materials, we obtain that for growing values of the applied voltage the …
