We review continuum elastic models for the transmission of both external forces and internal active cellular forces in biopolymer gels, and relate them to recent experiments. Rather than being exhaustive, we focus on continuum elastic models for small affine deformations and intend to provide a systematic continuum method and some analytical perspectives to the study of force transmissions in biopolymer gels. We start from a very brief review of the nonlinear mechanics of individual biopolymers and a summary of constitutive models for the nonlinear elasticity of biopolymer gels. We next show that the simple 3-chain model can give predictions that well fit the shear experiments of some biopolymer gels, including the effects of strain-stiffening and negative normal stress. We then review continuum models for the transmission of internal active forces that are induced by a spherically contracting cell embedded in a three-dimensional biopolymer gel. Various scaling regimes for the decay of cell-induced displacements are identified for linear isotropic and anisotropic materials, and for biopolymer gels with nonlinear compressive-softening and strain-stiffening elasticity, respectively. After that, we present (using an energetic approach) the generic and unified continuum theory proposed in [Ben-Yaakov, Soft Matter, 2015, 11, 1412] about how the transmission of forces in the biogel matrix can mediate long-range interactions between cells with mechanical homeostasis. We show the predictions of the theory in a special hexagonal multicellular array, and relate them to recent experiments. Finally, we conclude this paper with comments on the limitations and outlook of continuum modeling, and highlight the needs of complementary theoretical approaches such as discrete network simulations to force transmissions in biopolymer gels and phenomenological active gel theories for multicellular systems.
Recent experimental investigations have revealed a non-Maxwellian absorption pattern in the rheological spectra of actin gels, which was interpreted in terms of transient bonds. Here we examine the consequences of reversible crosslinking on the apparent linear spectra of biopolymer solutions theoretically. For a schematic model consisting of a reversibly crosslinked power-law fluid we obtain a simple analytical prediction for the position of the absorption peak, which is backed up by a numerical evaluation of the inelastic glassy wormlike chain model. This establishes bond breaking as a nonlin…
The variational principle of minimum free energy (MFEVP) has been widely used in the study of soft matter statics. MFEVP can be used not only to derive equilibrium equations (including both bulk equations and boundary conditions), but also to develop direct variational methods (such as Ritz method) to find approximate solutions to these equilibrium equations. In this work, we applied these variational methods to study long-range force transmission in nonlinear elastic biopolymer gels. We showed that the slow decay of cell-induced displacements measured experimentally for fibroblast spheroids i…
We investigate the delayed rupture of biopolymer gels under a constant shear load by simultaneous dynamic light scattering and rheology measurements. We unveil the crucial role of normal stresses built up during gelation: all samples that eventually fracture self-weaken during the gelation process, as revealed by a partial relaxation of the normal stress concomitant to a burst of microscopic plastic rearrangements. Upon applying a shear stress, weakened gels exhibit in the creep regime distinctive signatures in their microscopic dynamics, which anticipate macroscopic fracture by up to thousand…
When sheared, most elastic solids such as metals, rubbers and polymer hydrogels dilate in the direction perpendicular to the shear plane. This well-known behaviour known as the Poynting effect is characterized by a positive normal stress. Surprisingly, biopolymer gels made of fibrous proteins such as fibrin and collagen, as well as many biological tissues exhibit the opposite effect, contracting under shear and displaying a negative normal stress. Here we show that this anomalous behaviour originates from the open network structure of biopolymer gels, which facilitates interstitial fluid flow …
We present an extensive experimental study of mode-I, steady, slow crack dynamics in gelatin gels. Taking advantage of the sensitivity of the elastic stiffness to gel composition and history we confirm and extend the model for fracture of physical hydrogels which we proposed in a previous paper (Nature Materials, doi:10.1038/nmat1666 (2006)), which attributes decohesion to the viscoplastic pull-out of the network-constituting chains. So, we propose that, in contrast with chemically cross-linked ones, reversible gels fracture without chain scission.
Following recent X-ray diffraction experiments by Wong, Li, and Safinya on biopolymer gels, we apply Onsager excluded volume theory to a nematic mixture of rigid rods and strong ``$π/2$'' cross-linkers obtaining a long-ranged, highly anisotropic depletion attraction between the linkers. This attraction leads to breakdown of the percolation theory for this class of gels, to breakdown of Onsager's second-order virial method, and to formation of heterogeneities in the form of raft-like ribbons.
We present a Landau type theory for the non-linear elasticity of biopolymer gels with a part of the order parameter describing induced nematic order of fibers in the gel. We attribute the non-linear elastic behavior of these materials to fiber alignment induced by strain. We suggest an application to contact guidance of cell motility in tissue. We compare our theory to simulation of a disordered lattice model for biopolymers. We treat homogeneous deformations such as simple shear, hydrostatic expansion, and simple extension, and obtain good agreement between theory and simulation. We also cons…
When calcium salts are added to an aqueous solution of polysaccharide pectin, ionic cross-links form between pectin chains, giving rise to a gel network in dilute solution. In this work, dynamic light scattering (DLS) is employed to study the microscopic dynamics of the fractal aggregates (flocs) that constitute the gels, while rheological measurements are performed to study the process of gel rupture. As calcium salt concentration is increased, DLS experiments reveal that the polydispersities of the flocs increase simultaneously with the characteristic relaxation times of the gel network. Abo…
Biopolymer gels such as fibrin and collagen networks are known to develop tensile axial stress when subject to torsion. This negative normal stress is opposite to the classical Poynting effect observed for most elastic solids including synthetic polymer gels, where torsion provokes a positive normal stress. As recently shown, this anomalous behavior in fibrin gels depends on the open, porous network structure of biopolymer gels, which facilitates interstitial fluid flow during shear and can be described by a phenomenological two-fluid model with viscous coupling between network and solvent. He…
Motivated by recent experiments showing nonlinear elasticity of in vitro networks of the biopolymer actin cross-linked with filamin, we present an effective medium theory of flexibly cross-linked stiff polymer networks. We model such networks by randomly oriented elastic rods connected by flexible connectors to a surrounding elastic continuum, which self-consistently represents the behavior of the rest of the network. This model yields a crossover from a linear elastic regime to a highly nonlinear elastic regime that stiffens in a way quantitatively consistent with experiment.
Animal cells form contractile structures to promote various functions, from cell motility to cell division. Force generation in these structures is often due to molecular motors such as myosin that require polar substrates for their function. Here, we propose a motor-free mechanism that can generate contraction in biopolymer networks without the need for polarity. This mechanism is based on active binding/unbinding of crosslinkers that breaks the principle of detailed balance, together with the asymmetric force-extension response of semiflexible biopolymers. We find that these two ingredients …
Hydrogels are widespread soft materials, which can serve a wide range of applications. The control over the viscoelastic properties of the gel is of paramount importance. Ongoing environmental issues have raised the consumer's concern towards the use of more sustainable materials, including hydrogels. However, are greener materials compatible with high functionality? In a safe-by-design approach, this work demonstrates that functional hydrogels with in situ responsivity of their elastic properties by external stimuli can be developed from entirely ``sustainable'' components, a biobased amphiph…
We propose a model for the elastic properties of RNA gels. The model predicts anomalous elastic properties in the form of a negative Poisson ratio and shape instabilities. The anomalous elasticity is generated by the non-Gaussian force-deformation relation of single-stranded RNA. The effect is greatly magnified by broken rotational symmetry produced by double-stranded sequences and the concomitant soft modes of uniaxial elastomers.
We present a statistical mechanical study of stiff polymers, motivated by experiments on actin filaments and the considerable current interest in polymer networks. We obtain simple, approximate analytical forms for the force-extension relations and compare these with numerical treatments. We note the important role of boundary conditions in determining force-extension relations. The theoretical predictions presented here can be tested against single molecule experiments on neurofilaments and cytoskeletal filaments like actin and microtubules. Our work is motivated by the buckling of the cytosk…
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 …
Elastic waves propagating at the interface of soft solids can be altered by the presence of external forces such as capillarity or gravity. We measure the dispersion relation of waves at the free surface of agarose gels with great accuracy, revealing the existence of multiple modes as well as an apparent dispersion. We disentangle the role of capillarity and elasticity by considering the 3D nature of mechanical waves, achieving quantitative agreement between theoretical predictions and experiments. Notably, our results show that capillarity plays an important role for wavenumbers much smaller …
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…
Unlike most synthetic materials, biological materials often stiffen as they are deformed. This nonlinear elastic response, critical for the physiological function of some tissues, has been documented since at least the 19th century, but the molecular structure and the design principles responsible for it are unknown. Current models for this response require geometrically complex ordered structures unique to each material. In this Article we show that a much simpler molecular theory accounts for strain stiffening in a wide range of molecularly distinct biopolymer gels formed from purified cytos…
We study a model of an active gel of cross-linked semiflexible filaments with additional active linkers such as myosin II clusters. We show that the coupling of the elasticity of the semiflexible filaments to the mechanical properties of the motors leads to contractile behavior of the gel, in qualitative agreement with experimental observations. The motors, however, soften the zero frequency elastic constant of the gel. When the collective motor dynamics is incorporated in the model, a stiffening of the network at high frequencies is obtained. The frequency controlling the crossover between lo…
The elastic response in polymeric gels is studied by means of a percolation dynamic model. By numerical simulations the fluctuations in the gyration radius and in the center of mass motion of the percolating cluster are determined. Their scaling behaviour at the gelation threshold gives a critical exponent for the elastic modulus $f \sim 2.5 \pm 0.1$ in agreement with the prediction $f = d ν$.
Suspensions of calcite in water are employed in many industrial fields such as paper filling, pharmaceutics, heritage conservation or building construction, where the rheological properties of the paste need to be controlled. We measure the impact of simple ions such as calcium, sodium or hydroxide on the elasticity of a nanocalcite paste, which behaves as a colloidal gel. We confront our macroscopic measurements to DLVO interaction potentials, based on chemical speciations and measurements of the zeta potential. By changing the ion type and concentration, we go beyond the small repulsion regi…
Colloidal gels, where nanoscale particles aggregate into an elastic yet fragile network, are at the heart of materials that combine specific optical, electrical and mechanical properties. Tailoring the viscoelastic features of colloidal gels in real-time thanks to an external stimulus currently appears as a major challenge in the design of "smart" soft materials. Here we introduce "rheo-acoustic" gels, a class of materials that are sensitive to ultrasonic vibrations. By using a combination of rheological and structural characterization, we evidence and quantify a strong softening in three wide…
The elastic properties of a soft matter material can be greatly altered by the presence of solid inclusions whose microscopic properties, such as their size and interactions, can have a dramatic effect. In order to shed light on these effects we use extensive rheology computer simulations to investigate colloidal gels with solid inclusions of different size. We show that the elastic properties vary in a highly non trivial way as consequence of the interactions between the gel backbone and the inclusions. In particular, we show that the key aspects are the presence of the gel backbone and its m…
We present a generic formulation of the continuum elasticity of an isotropic crosslinked active gel. The gel is described by a two-component model consisting of an elastic network coupled frictionally to a permeating fluid. Activity is induced by active crosslinkers that undergo an ATP-activated cycle and transmit forces to the network. The on/off dynamics of the active crosslinkers is described via rate equations for unbound and bound motors. For large activity motors yield a contractile instability of the network. At smaller values of activity, the on/off motor dynamics provides an effective…
A network of semiflexible biopolymers, known as the cytoskeleton, and molecular motors play fundamental mechanical roles in cellular activities. The cytoskeletal response to forces generated by molecular motors is profoundly linked to physiological processes. However, owing to the highly nonlinear mechanical properties, the cytoskeletal response on the microscopic level is largely elusive. The aim of this study is to investigate the microscopic mechanical response of semiflexible biopolymer networks by conducting microrheology (MR) experiments. Micrometer-sized colloidal particles, embedded in…
We provide a unified theory for the high force elasticity of biopolymers solely in terms of the persistence length, $ξ_p$, and the monomer spacing, $a$. When the force $f>\fh \sim k_BTξ_p/a^2$ the biopolymers behave as Freely Jointed Chains (FJCs) while in the range $\fl \sim k_BT/ξ_p < f < \fh$ the Worm-like Chain (WLC) is a better model. We show that $ξ_p$ can be estimated from the force extension curve (FEC) at the extension $x\approx 1/2$ (normalized by the contour length of the biopolymer). After validating the theory using simulations, we provide a quantitative analysis of the FECs for a…
A hydrostatically stressed soft elastic film circumvents the imposed constraint by undergoing a morphological instability, the wavelength of which is dictated by the minimization of the surface and the elastic strain energies of the film. While for a single film, the wavelength is entirely dependent on its thickness, a co-operative energy minimization dictates that the wavelength depends on both the elastic moduli and thicknesses of two contacting films. The wavelength can also depend on the material properties of a film if its surface tension has a pronounced effect in comparison to its elast…
In the perspective of developing smart hybrid materials with customized features, ferrogels and magnetorheological elastomers allow a synergy of elasticity and magnetism. The interplay between elastic and magnetic properties gives rise to a unique reversible control of the material behavior by applying an external magnetic field. Albeit few works have been performed on the time-dependent properties so far, understanding the dynamic behavior is the key to model many practical situations, e.g. applications as vibration absorbers. Here we present a way to calculate the frequency-dependent elastic…
A nematic liquid-crystal gel is a macroscopically homogeneous elastic medium with the rotational symmetry of a nematic liquid crystal. In this paper, we develop a general approach to the study of these gels that incorporates all underlying symmetries. After reviewing traditional elasticity and clarifying the role of broken rotational symmetries in both the reference space of points in the undistorted medium and the target space into which these points are mapped, we explore the unusual properties of nematic gels from a number of perspectives. We show how symmetries of nematic gels formed via s…
A simple and popular constitutive model used to describe the compressional strength of a consolidating strongly cohesive particulate gel is tested further with new experimental data. Strong cohesive particulate gels have variously been described as being ratchet (poro) elastic, on the one hand, and as having a yield stress in compression, on the other, to the point where same groups of workers have used both descriptions at one time or another. The dichotomy is real though as such gels do show a hitherto somewhat puzzling elastic-plastic duality. This can be explained in part by the strong con…
Motivated by recent experiments showing that stiff biopolymer gels exhibit highly unusual negative normal elastic stresses, we develop a computational model for stiff polymer networks subject to large strains. In all cases, we find that such networks develop normal stresses that are both negative and of magnitude comparable to the corresponding shear stress. We find that these normal stresses coincide with other nonlinearities in our networks, and specifically with compressive bucking of the individual filaments. Our results suggest that negative normal stresses are a characteristic feature of…
The physical gelation of colloids produces elastic structures that are commonly used to stabilize complex fluids in multiple industries. However, the ability to control the level of elastic modulus of these materials is limited by the universality of the arrested spinodal decomposition mechanism that governs their formation. We demonstrate that manipulating particle shape can yield very large shifts in gel elasticity relative to this universal behavior, and that these changes are generated by a set of independent mechanisms that act multiplicatively. Modeling demonstrates that this efficient g…
Aiming at the mechanical properties of cross-linked biopolymers, we set up and analyze a model of two weakly bending wormlike chains subjected to a tensile force, with regularly spaced inter-chain bonds (cross-links) represented by harmonic springs. Within this model, we compute the force-extension curve and the differential stiffness exactly and discuss several limiting cases. Cross-links effectively stiffen the chain pair by reducing thermal fluctuations transverse to the force and alignment direction. The extra alignment due to cross-links increases both with growing number and with growing…
We image semi-flexible polymer networks under shear at the micrometer scale. By tracking embedded probe particles, we determine the local strain field, and directly measure its uniformity, or degree of affineness, on scales of 2-100 micron. The degree of nonaffine strain depends on polymer length and crosslink density, consistent with theoretical predictions. We also find a direct correspondence between the uniformity of the microscale strain and the nonlinear elasticity of the networks in the bulk.
Structuring wheat gluten proteins into gels with tunable mechanical properties would provide more versatility for the production of plant protein-rich food products. Gluten, a strongly elastic protein material insoluble in water, is hardly processable. We use a novel fractionation procedure allowing the isolation from gluten of a water/ethanol soluble protein blend, enriched in glutenin polymers at an unprecedented high ratio (50%). We investigate here the viscoelasticity of suspensions of the protein blend in a water/ethanol (50/50 v/v) solvent, and show that, over a wide range of concentrati…
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…
The mechanics of cells is strongly affected by molecular motors that generate forces in the cellular cytoskeleton. We develop a model for cytoskeletal networks driven out of equilibrium by molecular motors exerting transient contractile stresses. Using this model we show how motor activity can dramatically increase the network's bulk elastic moduli. We also show how motor binding kinetics naturally leads to enhanced low-frequency stress fluctuations that result in non-equilibrium diffusive motion within an elastic network, as seen in recent \emph{in vitro} and \emph{in vivo} experiments.
We investigate the stretching response of a thick polymer model by means of extensive stochastic simulations. The computational results are synthesized in an analytic expression that characterizes how the force versus elongation curve depends on the polymer structural parameters: its thickness and granularity (spacing of the monomers). The expression is used to analyze experimental data for the stretching of various different types of biopolymers: polypeptides, polysaccharides and nucleic acids. Besides recovering elastic parameters (such as the persistence length) that are consistent with tho…
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…
We use continuum theory to show that chirality is a key thermodynamic control parameter for the aggregation of biopolymers: chirality produces a stable disperse phase of hexagonal bundles under moderately poor solvent conditions, as has been observed in {\it in-vitro} studies of F-actin [O. Pelletier {\it et al.}, Phys. Rev. Lett. {\bf 91}, 148102 (2003)]. The large characteristic radius of these chiral bundles is not determined by a mysterious long-range molecular interaction but by in-plane shear elastic stresses generated by the interplay between a chiral torque and an unusual, but universa…
We construct a three-dimensional lattice model for biological gels in which straight lines of bonds correspond to filamentous semi-flexible polymers and lattice sites, which are exactly four-fold coordinated, to crosslinks. With only stretching central forces between nearest neighbors, this lattice is sub-isostatic with an extensive number of zero modes; but all of its elastic constants are nonzero, and its elastic response is affine. Removal of bonds with probability $1-p$ leads to a lattice with average coordination number less than four and a distribution of polymer lengths. When bending fo…
We show that gels formed by arrested spinodal decomposition of protein solutions exhibit elastic properties in two distinct frequency domains, both elastic moduli exhibiting a remarkably strong dependence on volume fraction. Considering the large difference between the protein size and the characteristic length of the network we model the gels as porous media and show that the high and low frequency elastic moduli can be respectively attributed to stretching and bending modes. The unexpected decoupling of the two modes in the frequency domain is attributed to the length scale involved: while s…
We report analytical and numerical modelling of active elastic networks, motivated by experiments on crosslinked actin networks contracted by myosin motors. Within a broad range of parameters, the motor-driven collapse of active elastic networks leads to a critical state. We show that this state is qualitatively different from that of the random percolation model. Intriguingly, it possesses both euclidean and scale-free structure with Fisher exponent smaller than $2$. Remarkably, an indistinguishable Fisher exponent and the same euclidean structure is obtained at the critical point of the rand…
We study the effects of intrinsic sequence-dependent curvature for a two dimensional semiflexible biopolymer with short-range correlation in intrinsic curvatures. We show exactly that when not subjected to any external force, such a system is equivalent to a system with a well-defined intrinsic curvature and a proper renormalized persistence length. We find the exact expression for the distribution function of the equivalent system. However, we show that such an equivalent system does not always exist for the polymer subjected to an external force. We find that under an external force, the eff…
Readily synthesizable nano-graphene and poly ethylene glycol based stable gels have been synthesized employing an easy refluxing method and exhaustive rheological and viscoelastic characterizations have been performed to understand the nature of such complex gel systems. The gels exhibit shear thinning response with pronounced yield stress values which is indicative of a microstructure where the graphene nanoflakes intercalate with the polymer chains and form a pseudo spring damper network. Experimentations on the thixotropic behavior of the gels indicate that the presence of the G nanoflakes …
We report detailed theoretical investigations of the micro-mechanics and bulk elastic properties of composites consisting of randomly distributed stiff fibers embedded in an elastic matrix in two and three dimensions. Recent experiments published in Physical Review Letters [102, 188303 (2009)] have suggested that the inclusion of stiff microtubules in a softer, nearly incompressible biopolymer matrix can lead to emergent compressibility. This can be understood in terms of the enhancement of the compressibility of the composite relative to its shear compliance as a result of the addition of sti…
Unlike hard materials such as metals and ceramics, rubbery materials can endure large deformations due to the large conformational degree of freedom of the crosslinked three-dimensional polymer network. However, the effect of the branching factor of the network on the ultimate mechanical properties of rubbery materials has not yet been clarified. This study shows that tri-branching, which entails the lowest branching factor, results in a large elastic deformation near the theoretical upper bound. This ideal elastic limit is realized by reversible strain-induced crystallization, providing on-de…
Precise measuring the deforming force and observation of the deformation dynamics along with difficulties of micro sample preparation are the main problems which make the micro-scale experiments difficult. Here we present a method for direct observation and measurements of mechanical parameters of elastic microfibrils in air using the pressure of optical light. For DNA microfibers, observation of the behavior dynamics of mechanical characteristics and the method sensitivity to changing the structure are demonstrated.
Many microorganisms swim through gels, materials with nonzero zero-frequency elastic shear modulus, such as mucus. Biological gels are typically heterogeneous, containing both a structural scaffold (network) and a fluid solvent. We analyze the swimming of an infinite sheet undergoing transverse traveling wave deformations in the "two-fluid" model of a gel, which treats the network and solvent as two coupled elastic and viscous continuum phases. We show that geometric nonlinearities must be incorporated to obtain physically meaningful results. We identify a transition between regimes where the …
Magnetic gels and elastomers are promising candidates to construct reversibly excitable soft actuators, triggered from outside by magnetic fields. These magnetic fields induce or alter the magnetic interactions between discrete rigid particles embedded in a soft elastic polymeric matrix, leading to overall deformations. It is a major challenge in theory to correctly predict from the discrete particle configuration the type of deformation resulting for a finite-sized system. Considering an elastic sphere, we here present such an approach. The method is in principle exact, at least within the fr…
