Disordered spring networks are a useful paradigm to examine macroscopic mechanical properties of amorphous materials. Here, we study the elastic behavior of under-constrained spring networks, i.e.\ networks with more degrees of freedom than springs. While such networks are usually floppy, they can be rigidified by applying external strain. Recently, an analytical formalism has been developed to predict the mechanical network properties close to this rigidity transition. Here we numerically show that these predictions apply to many different classes of spring networks, including phantom triangular, Delaunay, Voronoi, and honeycomb networks. The analytical predictions further imply that the shear modulus $G$ scales linearly with isotropic stress $T$ close to the rigidity transition; however, this seems to be at odds with recent numerical studies suggesting an exponent between $G$ and $T$ that is smaller than one for some network classes. Using increased numerical precision and shear stabilization, we demonstrate here that close to the transition linear scaling, $G\sim T$, holds independent of the network class. Finally, we show that our results are not or only weakly affected by finite-size effects, depending on the network class.
Gels are an increasingly important class of soft materials with applications ranging from regenerative medicine to commodity materials. A major drawback of gels is their relative mechanical weakness, which worsens further under strain. We report a new class of responsive gels with latent crosslinking moieties that exhibit strain-stiffening behavior. This property results from the lability of disulfides, initially isolated in a protected state, then activated to crosslink on-demand. The active thiol groups are induced to form inter-chain crosslinks when subjected to mechanical compression, resu…
Spider silk possesses unique mechanical properties like large extensibility, high tensile strength, super-contractility, etc. Understanding these mechanical responses require characterization of the rheological properties of silk beyond the simple force-extension relations which are widely reported. Here we study the linear and non-linear viscoelastic properties of dragline silk obtained from social spiders Stegodyphus sarasinorum using a Micro-Extension Rheometer that we have developed. Unlike continuous extension data, our technique allows for the probing of the viscoelastic response by appl…
Random packings of granular chains are presented as a model polymer system to investigate the contribution of entanglements to strain-stiffening in the absence of Brownian motion. The chain packings are sheared in triaxial compression experiments. For short chain lengths, these packings yield when the shear stress exceeds a the scale of the confining pressure, similar to packings of spherical particles. In contrast, packings of chains which are long enough to form loops exhibit strain-stiffening, in which the effective stiffness of the material increases with strain, similar to many polymer ma…
Strain stiffening of protein networks is explored by means of a finite strain analysis of a two-dimensional network model of cross-linked semiflexible filaments. The results show that stiffening is caused by non-affine network rearrangements that govern a transition from a bending dominated response at small strains to a stretching dominated response at large strains. Thermally-induced filament undulations only have a minor effect; they merely postpone the transition.
Strain-stiffening is a well-documented behavior in soft biological materials such as liver and brain tissue. Measuring and characterizing this nonlinear response, which is commonly considered as a mechanism for damage prevention, is of great interest to engineers for design of better biomimetic materials, and to physicians for diagnostic purposes. However, probing the elastic response of soft or biological materials at large deformation in their natural habitat, is an arduous task. Here, we present the Volume Controlled Cavity Expansion (VCCE) technique as an in-vivo measurement method that of…
Packings of macroscopic granular chains capture some of the essential aspects of molecular polymer systems and have been suggested as a paradigm to understand the physics on a molecular scale. However, here we demonstrate that the interparticle friction $μ$ in granular chain packings, which has no counterpart in polymer systems, leads to a nontrivial yielding and rheological response. Based on discrete element simulations we study the nonlinear rheology of random packings of granular chains under large amplitude oscillatory shear. We find that the maximum stress and the penetration depth of th…
Filamentous bio-materials such as fibrin or collagen networks exhibit an enormous stiffening of their elastic moduli upon large deformations. This pronounced nonlinear behavior stems from a significant separation between the stiffnesses scales associated with bending vs. stretching the material's constituent elements. Here we study a simple model of such materials - floppy networks of hinged rigid bars embedded in an elastic matrix - in which the effective ratio of bending to stretching stiffnesses vanishes identically. We introduce a theoretical framework and build upon it to construct a nume…
We have studied the elastic response of actin networks with both compliant and rigid crosslinks by modeling molecular motors as force dipoles. Our finite element simulations show that for compliant crosslinkers such as filamin A, the network can be stiffened by two orders of magnitude while stiffening achieved with incompliant linkers such as scruin is significantly smaller, typically a factor of two, in excellent agreement with recent experiments. We show that the differences arise from the fact that the motors are able to stretch the compliant crosslinks to the fullest possible extent, which…
Stress induced yielding/fluidization in disordered solids, characterized by irreversibility and enhanced dissipation, is important for a wide range of industrial and geological processes. Although, such phenomena in thermal systems have been extensively studied, they remain poorly understood for granular solids. Here, using oscillatory shear rheology and in-situ optical imaging, we study energy dissipation in a dense granular suspension of adhesive particles that forms yield stress solids far below the isotropic jamming point obtained in the limit of hard-sphere repulsion. We find interesting …
Bistability of cellular traction on strain-stiffening substrates
Universitat de Barcelona（巴塞罗那大学）；Institució Catalana de Recerca i Estudis Avançats (ICREA)（加泰罗尼亚研究与高等学院）；Max Planck Institute for the Physics of Complex Systems（马克斯·普朗克复杂系统物理研究所）；TU Dresden（德累斯顿工业大学）
We use optical tweezers microrheology and fluorescence microscopy to apply nonlinear microscale strains to entangled and crosslinked actin networks, and measure the resulting stress and actin filament deformations. We couple nonlinear stress response and subsequent relaxation to the velocity profiles of individual fluorescent-labeled actin segments at varying times throughout the strain and varying distances from the strain path to determine the underlying molecular dynamics that give rise to the debated nonlinear response and stress propagation of crosslinked and entangled actin networks at t…
Strain-stiffening critical exponents of fiber networks under uniaxial deformation
Universität Augsburg（奥格斯堡大学）；Rice University（莱斯大学）；Institut für Physik, Universität Augsburg（奥格斯堡大学物理研究所）；Department of Chemical and Biomolecular Engineering, Rice University（莱斯大学生物化学工程系）；Center for Theoretical Biological Physics, Rice University（莱斯大学理论生物物理中心）；Department of Chemistry, Rice University（莱斯大学化学系）；Department of Physics and Astronomy, Rice University（莱斯大学物理与天文系）；Bereich Theorie der Polymere, Leibniz-Institut für Polymerforschung（莱布尼茨高分子研究所聚合物理论部）
Granular chain packings exhibit a striking emergent strain-stiffening behavior despite the individual looseness of the constitutive chains. Using indentation experiments on such assemblies, we measure an exponential increase in the collective resistance force $F$ with the indentation depth $z$, and with the square root of the number $\mathcal{N}$ of beads per chain. These two observations are respectively reminiscent of the self-amplification of friction in a capstan or in interleaved books, as well as the physics of polymers. The experimental data are well captured by a novel model based on t…
This paper presents an electromechanical analysis of the nonlinear static response and the superimposed small-amplitude wave characteristics in an infinite periodic compressible dielectric elastomer (DE) laminate subjected to electrostatic excitations and prestress in the thickness direction. The enriched Gent material model is employed to account for the effects of strain stiffening and electrostriction of the DE laminate. The theory of nonlinear electroelasticity and related linearized incremental theory are exploited to derive the governing equations of nonlinear response and the dispersion…
Bundles of polymer filaments are responsible for the rich and unique mechanical behaviors of many biomaterials, including cells and extracellular matrices. In fibrin biopolymers, whose nonlinear elastic properties are crucial for normal blood clotting, protofibrils self-assemble and bundle to form networks of semiflexible fibers. Here we show that the extraordinary strain-stiffening response of fibrin networks is a direct reflection of the hierarchical architecture of the fibrin fibers. We measure the rheology of networks of unbundled protofibrils and find excellent agreement with an affine mo…
Compression stiffening, or an increase in shear modulus with increasing compressive strain, has been observed in recent rheometry experiments on brain, liver, and fat tissues. Here, we extend the known types of biomaterials exhibiting this phenomenon to include agarose gel and fruit flesh. Further, we show that two different results from classic elasticity theory can account for the phenomenon of linear compression stiffening. One result is due to Barron and Klein, extended here to the relevant geometry and pre-stresses; the other is due to Birch. For incompressible materials, there are no adj…
We present theoretical and experimental studies of the elastic response of fibrous networks subjected to uniaxial strain. Uniaxial compression or extension is applied to extracellular networks of fibrin and collagen using a shear rheometer with free water in/outflow. Both axial stress and the network shear modulus are measured. Prior work [van Oosten et al., Scientific Reports, 2015, 6, 19270] has shown softening/stiffening of these networks under compression/extension, together with a nonlinear response to shear, but the origin of such behaviour remains poorly understood. Here, we study how u…
We study the micromechanics of collagen-I gel with the goal of bridging the gap between theory and experiment in the study of biopolymer networks. Three-dimensional images of fluorescently labeled collagen are obtained by confocal microscopy and the network geometry is extracted using a 3d network skeletonization algorithm. Each fiber is modeled as a worm-like-chain that resists stretching and bending, and each cross-link is modeled as torsional spring. The stress-strain curves of networks at three different densities are compared to rheology measurements. The model shows good agreement with e…
Intermediate filaments are cytoskeletal proteins that are key regulators of cell mechanics, a role which is intrinsically tied to their hierarchical structure and their unique ability to accommodate large axial strains. However, how the single-filament response to applied strains translates to networks remains unclear, particularly with regards to the crosslinking role played by the filaments' disordered "tail" domains. Here we test the role of these noncovalent crosslinks in the nonlinear rheology of reconstituted networks of the intermediate filament protein vimentin, probing their stress- a…
When elastic solids are sheared, a nonlinear effect named after Poynting gives rise to normal stresses or changes in volume. We provide a novel relation between the Poynting effect and the microscopic Grüneisen parameter, which quantifies how stretching shifts vibrational modes. By applying this relation to random spring networks, a minimal model for, e.g., biopolymer gels and solid foams, we find that networks contract or develop tension because they vibrate faster when stretched. The amplitude of the Poynting effect is sensitive to the network's linear elastic moduli, which can be tuned via …
We investigate the system size dependent rheological response of branched type I collagen gels. When subjected to a shear strain, the highly interconnected mesh dynamically reorients, resulting in overall stiffening of the network. When a continuous shear strain is applied to a collagen network, we observe that the local apparent modulus, in the strain-stiffening regime, is strongly dependent on the gel thickness. In addition, we demonstrate that the overall network failure is determined by the ratio of the gel thickness to the mesh size. These findings have broad implications for cell-matrix …
Both animal and plant tissue exhibit a nonlinear rheological phenomenon known as compression stiffening, or an increase in moduli with increasing uniaxial compressive strain. Does such a phenomenon exist in single cells, which are the building blocks of tissues? One expects an individual cell to compression soften since the semiflexible biopolymer-based cytoskeletal network maintains the mechanical integrity of the cell and in vitro semiflexible biopolymer networks typically compression soften. To the contrary, we find that mouse embryonic fibroblasts (mEFs) compression stiffen under uniaxial …
We investigate the cyclic mechanical behavior in uniaxial tension of three different commercial thermoplastic polyurethane elastomers (TPU) often considered as a sustainable replacement for common filled elastomers. All TPU have similar hard segment contents and linear moduli but sensibly different large strain properties as shown by X-Ray analysis. Despite these differences, we found a stiffening effect after conditioning in step cyclic loading which greatly differs from the common softening (also referred as Mullins effect) observed in chemically crosslinked filled rubbers. We propose that t…
We use numerical simulations and an athermal quasi-static shear protocol to investigate the yielding of a model colloidal gel. Under increasing deformation, the elastic regime is followed by a significant stiffening before yielding takes place. A space-resolved analysis of deformations and stresses unravel how the complex load curve observed is the result of stress localization and that the yielding can take place by breaking a very small fraction of the network connections. The stiffening corresponds to the stretching of the network chains, unbent and aligned along the direction of maximum ex…
We present a revised theoretical study of the affine assumption applied to semiflexible networks. Drawing on simple models of semiflexible worm-like chains we derive an expression for the probability distribution of crosslink separations valid at all separations. This accounts for both entropic and mechanical filament stretching. From this we obtain the free energy density of such networks explicitly as a function of applied strain. We are therefore able to calculate the elastic moduli of such networks for any imposed strain or stress. We find that accounting for the distribution of cross-link…
We find the strain energy function for isotropic incompressible solids exhibiting a linear relationship between shear stress and amount of shear, and between torque and amount of twist, when subject to large simple shear or torsion deformations. It is inclusive of the well-known neo-Hookean and the Mooney-Rivlin models, but also can accommodate other terms, as certain arbitrary functions of the principal strain invariants. Effectively, the extra terms can be used to account for several non-linear effects observed experimentally but not captured by the neo-Hookean and Mooney-Rivlin models, such…
Histotripsy relies on cavitation to mechanically homogenize soft tissue. There is strong evidence that the high stresses, strains, and strain rates developed as bubbles grow and collapse contribute to this tissue homogenization. While such stresses and strains have been examined computationally in model systems with assumed constitutive models (e.g., finite-deformation Neo-Hookean model) and viscoelastic properties determined under quasi-static conditions, recent studies proposed that the Quadratic Law Kelvin-Voigt (QLKV) constitutive model, which additionally accounts for strain stiffening, m…
We introduce a strain-energy based nonlinear hyper-elastic formulation to model the material properties of ultrasoft dielectric elastomers over a wide range of elastic properties, prestretch, and thicknesses. We build on the uniaxial Gent formulation, and under the conditions of equi-biaxial strain, derive an expression for the bulge deformation versus pressure. A circular bulge test methodology is developed to experimentally measure the mechanical response of the silicone membranes. The Gent model captures both neo-Hookean and strain-stiffening behaviors, and gives predictions which are in ag…
Disordered soft materials, such as fibrous networks in biological contexts exhibit a nonlinear elastic response. We study such nonlinear behavior with a minimal model for networks on lattice geometries with simple Hookian elements with disordered spring constant. By developing a mean-field approach to calculate the differential elastic bulk modulus for the macroscopic network response of such networks under large isotropic deformations, we provide insight into the origins of the strain stiffening and softening behavior of these systems. We find that the nonlinear mechanics depends only weakly …
We study geometrical clues of a rigidity transition due to the emergence of a system-spanning state of self stress in under-constrained systems of individual polygons and spring networks constructed from such polygons. When a polygon with harmonic bond edges and an area spring constraint is subject to an expansive strain, we observe that convexity of the polygon is a necessary condition for such a self stress. We prove that the cyclic configuration of the polygon is a sufficient condition for the self stress. This correspondence of geometry and rigidity is akin to the straightening of a one di…
Collagen is the most abundant extracellular-matrix protein in mammals and the main structural and load-bearing element of connective tissues. Collagen networks show remarkable strain-stiffening properties which tune the mechanical functions of tissues and regulate cell behaviours. Linear and non-linear mechanical properties of in-vitro disordered collagen networks have been widely studied using rheology for a range of self-assembly conditions in recent years. However, a one to one correlation between the onset of macroscopic network failure and local deformations inside the sample is yet to be…
A widely-studied model for gels or biopolymeric fibrous materials are networks with central force interactions, such as Hookean springs. Less commonly studied are materials whose mechanics are dominated by non-central force interactions such as bond-bending potentials. Inspired by recent experimental advancements in designing colloidal gels with tunable interactions, we study the micro- and macroscopic elasticity of two-dimensional planar graphs with strong bond bending potentials, in addition to weak central forces. We introduce a theoretical framework that allows us to directly investigate t…
We construct and analyze a model for a disordered linear spring network with anisotropy. The modeling is motivated by, for example, granular systems, nematic elastomers, and ultimately cytoskeletal networks exhibiting some underlying anisotropy. The model consists of a triangular lattice with two different bond occupation probabilities, $p_x$ and $p_y$, for the linear springs. We develop an effective medium theory (EMT) to describe the network elasticity as a function of $p_x$ and $p_y$. We find that the onset of rigidity in the EMT agrees with Maxwell constraint counting. We also find beyond …
We study the dynamical rheology of spring networks with a percolation model constructed by bond dilution in a two-dimensional triangular lattice. Hydrodynamic interactions are implemented by a Stokesian viscous coupling between the network nodes and a uniformly deforming liquid. Our simulations show that in a critical connectivity regime, these systems display weak power law rheology in which the complex shear modulus scales with frequency as G^* ~ (i * omega)^Delta where Delta = 0.41, in discord with a mean field prediction of Delta = 1/2. The weak power law rheology in the critical regime ca…
Networks with only central force interactions are floppy when their average connectivity is below an isostatic threshold. Although such networks are mechanically unstable, they can become rigid when strained. It was recently shown that the transition from floppy to rigid states as a function of simple shear strain is continuous, with hallmark signatures of criticality (Nat. Phys. 12, 584 (2016)). The nonlinear mechanical response of collagen networks was shown to be quantitatively described within the framework of such mechanical critical phenomenon. Here, we provide a more quantitative charac…
Living tissues show an extraordinary adaptiveness to strain, which is crucial for their proper biological functioning. The physical origin of this mechanical behaviour has been widely investigated using reconstituted networks of collagen fibres, the principal load-bearing component of tissues. However, collagen fibres in tissues are embedded in a soft hydrated polysaccharide matrix which generates substantial internal stresses whose effect on tissue mechanics is unknown. Here, by combining mechanical measurements and computer simulations, we show that networks composed of collagen fibres and a…
Disordered spring networks can exhibit rigidity transitions, due to either the removal of materials in over-constrained networks or the application of strain in under-constrained ones. While an effective medium theory (EMT) exists for the former, there is none for the latter. We, therefore, formulate an EMT for random regular networks, under-constrained spring networks with purely geometrical disorder, to predict their stiffness via the distribution of tensions. We find a linear dependence of stiffness on strain in the rigid phase and a nontrivial dependence on both the mean and standard devia…
Repeated/cyclic shearing can drive amorphous solids to a steady-state encoding a memory of the applied strain amplitude. However, recent experiments find that the effect of such memory formation on the mechanical properties of the bulk material is rather weak. Here we study the memory effect in a yield stress solid formed by a dense suspension of cornstarch particles in paraffin oil. Under cyclic shear, the system evolves towards a steady-state showing training-induced strain stiffening and plasticity. A readout reveals that the system encodes a strong memory of the training amplitude as indic…
