Friction experiments were conducted on hydrogel thin films sliding against a rigid sphere in a low velocity regime where molecular adsorption at the sliding interface sets the friction force, through a dissipative adsorption-stretching-desorption mechanism initially postulated by Schallamach. By carefully imaging the contact from the initial indentation step of the sphere into the hydrogel to steady state sliding, we evidence for the first time that this very same adsorption mechanism also results in a normal force pulling the sphere further into the hydrogel. Observations of this tangential-normal coupling is made on a variety of chemically modified silica spheres, over 3 decades in velocity and at varied normal load, thereby demonstrating its robustness. Quantitative measurements of the extra normal force and of the friction-velocity relationship versus normal load are well rationalized within a theoretical model based on the thermal actuation of molecular bonds. To do so, we account for the finite non-zero thickness of the sliding interface at which molecular adsorption and stretching events produce an out-of-plane force responsible for both friction and normal pull-in.
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…
\textbf{Background} Hydrogels are crosslinked polymer networks that can absorb and retain a large fraction of liquid. Near a critical sliding velocity, hydrogels pressed against smooth surfaces exhibit time-dependent frictional behavior occurring over multiple timescales, yet the origin of these dynamics is unresolved. \textbf{Objective} Here, we characterize this time-dependent regime and show that it is consistent with two distinct molecular processes: sliding-induced relaxation and quiescent recovery. \textbf{Methods} Our experiments use a custom pin-on-disk tribometer to examine poly(acryl…
We report on the frictional behaviour of thin poly(dimethylacrylamide) (PDMA) hydrogels films grafted on glass substrates in sliding contact with a glass spherical probe. Friction experiments are carried out at various velocities and applied normal loads with the contact fully immersed in water. In addition to friction force measurements, a novel optical set-up is designed to image the shape of the contact under steady-state sliding. The velocity-dependence of both friction force $F_t$ and contact shape is found to be controlled by a Péclet number Pe defined as the ratio of the time $τ$ needed…
Hydrogel consists of a crosslinked polymer matrix imbibed with a solvent such as water at volume fractions that can exceed 90\%. They are important in many scientific and engineering applications due to their tunable physiochemical properties, bio-compatibility, and ultra-low friction. Their multiphase structure leads to a complex interfacial rheology, yet a detailed, microscopic understanding of hydrogel friction is still emerging. Using a custom-built tribometer, here we identify three distinct regimes of frictional behavior for polyacrylic acid (PAA), polyacrylamide (PAAm), and agarose hydr…
We report on the transient frictional response of contacts between a rigid spherical glass probe and a micrometer-thick poly(dimethylacrylamide) hydrogel film grafted onto a glass substrate when a lateral relative motion is applied to the contact initially at rest. From dedicated experiments with \textit{in situ} contact visualization, both the friction force and the contact size are observed to vary well beyond the occurrence of a full sliding condition at the contact interface. Depending on the imposed velocity and on the static contact time before the motion is initiated, either an overshoo…
Subjected to compressive stresses, soft polymers with stiffness gradients can display various buckling patterns. These compressive stresses can have different origins, like mechanical forces, temperature changes, or, for hydrogel materials, osmotic swelling. Here, we focus on the influence of the transient nature of osmotic swelling on the initiation of buckling in confined layered hydrogel structures. A constitutive model for transient hydrogel swelling is outlined and implemented as a user-subroutine for the commercial finite element software Abaqus. The finite element procedure is benchmark…
The hyperstatic nature of granular packings of perfectly rigid disks is analyzed algebraically and through numerical simulation. The elementary loops of grains emerge as a fundamental element in addressing hyperstaticity. Loops consisting of an odd number of grains behave differently than those with an even number. For odd loops, the latent stresses are exterior and are characterized by the sum of frictional forces around each loop. For even loops, the latent stresses are interior and are characterized by the alternating sum of frictional forces around each loop. The statistics of these two ty…
We present molecular dynamics friction calculations for confined hydrocarbon solids with molecular lengths from 20 to 1400 carbon atoms. Two cases are considered: (a) polymer sliding against a hard substrate, and (b) polymer sliding on polymer. We discuss the velocity dependence of the frictional shear stress for both cases. In our simulations, the polymer films are very thin (approx. 3 nm), and the solid walls are connected to a thermostat at a short distance from the polymer slab. Under these circumstances we find that frictional heating effects are not important, and the effective temperatu…
The formalism proposed in Phys. Rev. Lett. 116, 078001 (2016) for determination of the normal and tangential inter-particle forces in frictional disks from visual data was criticized in a comment to that paper. However the theory developed in the original publication is aimed at finding the forces when provided with accurate measurements while the comment addresses a different problem, being the statistics of forces in a configuration with uncertainty of the relevant parameters. We address this difference in perspectives and point out that even with experimental errors one can improve the resu…
We report on the frictional properties of a single contact between a glassy polymer lens and a flat silica substrate covered either by a disordered or by a self-assembled alkylsilane monolayer. We find that, in contrast to common belief, the Amontons proportionality between frictional and normal stresses does not hold. Besides, we observe that the velocity dependence of the sliding stress is strongly sensitive to the structure of the silane layer. Analysis of the frictional rheology observed on both disordered and self-assembled monolayers suggests that dissipation is controlled by the plastic…
When a soft hydrogel sphere is placed on a rigid hydrophilic substrate, it undergoes arrested spreading by forming an axisymmetric foot near the contact line, while conserving its global spherical shape. In contrast, liquid water (that constitutes greater than 90% of the hydrogel's volume) spreads into a thin film on the same surface. We study systematically this elastowetting of gel spheres on substrates of different surface energies, and find that their contact angle increases as the work of adhesion between the gel and the substrate decreases, as one would observe for drops of pure water - …
We report the results of three-dimensional molecular dynamics simulations of sheared granular system in a Couette geometry.\cite{movies} The simulations use realistic boundary conditions that may be expected in physical experiments. For a range of boundary properties we report velocity and density profiles, as well as forces on the boundaries. In particular, we find that the results for the velocity profiles throughout the shearing cell depend strongly on the interaction of the system particles with the physical boundaries. Even frictional boundaries can allow for significant slippage of the p…
The granular jamming transition is experimentally investigated in a two-dimensional system of frictional, bi-dispersed disks subject to quasi-static, uniaxial compression at zero granular temperature. Currently accepted results show the jamming transition occurs at a critical packing fraction $ϕ_c$. In contrast, we observe the first compression cycle exhibits {\it fragility} - metastable configuration with simultaneous jammed and un-jammed clusters - over a small interval in packing fraction ($ϕ_1 < ϕ< ϕ_2$). The fragile state separates the two conditions that define $ϕ_c$ with an exponential …
A granular system composed of frictional glass beads is simulated using the Discrete Element Method. The inter-grain forces are based on the Hertz contact law in the normal direction with frictional tangential force. The damping due to collision is also accounted for. Systems are loaded at various stresses and their quasi-static elastic moduli are characterized. Each system is subjected to an extensive dynamic testing protocol by measuring the resonant response to a broad range of AC drive amplitudes and frequencies via a set of diagnostic strains. The system, linear at small AC drive amplitud…
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 …
The packing and flow of aspherical frictional particles are studied using discrete element simulations. Particles are superballs with shape $|x|^{s}+|y|^{s}+|z|^{s} = 1$ that varies from sphere ($s=2$) to cube ($s=\infty$), constructed with an overlapping-sphere model. Both packing fraction, $ϕ$, and coordination number, $z$, decrease monotonically with microscopic friction $μ$, for all shapes. However, this decrease is more dramatic for larger $s$ due to a reduction in the fraction of face-face contacts with increasing friction. For flowing grains, the dynamic friction $\tildeμ$ - the ratio o…
The understanding of sliding friction for wet, patterned surfaces from first principles is challenging. While emerging applications have sought design principles from biology, a general framework is lacking because soft interfaces experience a multiphysics coupling between solid deformation and fluid dissipation. We investigate the elastohydrodynamic sliding of >50 patterned sliding pairs comprising elastomers, thermosets, and hydrogels, and discover that texturing induces a critical transition in the macroscopic friction coefficient. This critical friction scales universally, without any fitt…
The determination of the normal and transverse (frictional) inter-particle forces within a granular medium is a long standing, taunting, and yet unresolved problem. We present a new formalism which employs the knowledge of the external forces and the orientations of contacts between particles (of any given sizes), to compute all the inter-particle forces. Having solved this problem we exemplify the efficacy of the formalism showing that the force chains in such systems are determined by an expansion in the eigenfunctions of a newly defined operator.
The dynamic initiation of sliding at planar interfaces between deformable and rigid solids is studied with particular focus on the speed of the slip front. Recent experimental results showed a close relation between this speed and the local ratio of shear to normal stress measured before slip occurs (static stress ratio). Using a two-dimensional finite element model, we demonstrate, however, that fronts propagating in different directions do not have the same dynamics under similar stress conditions. A lack of correlation is also observed between accelerating and decelerating slip fronts. Thes…
We review the present state of understanding of solid friction at low velocities and for systems with negligibly small wear effects. We first analyze in detail the behavior of friction at interfaces between wacroscopic hard rough solids, whose main dynamical features are well described by the Rice-Ruina rate and state dependent constitutive law. We show that it results from two combined effects : (i) the threshold rheology of nanometer-thick junctions jammed under confinement into a soft glassy structure (ii) geometric aging, i.e. slow growth of the real arrea of contact via asperity creep int…
Hydrogels of semiflexible biopolymers such as collagen have been shown to contract axially under shear strain, in contrast to the axial dilation observed for most elastic materials. Recent work has shown that this behavior can be understood in terms of the porous, two-component nature and consequent time-dependent compressibility of hydrogels. The apparent normal stress measured by a torsional rheometer reflects only the tensile contribution of the axial component $σ_{zz}$ on long (compressible) timescales, crossing over to the first normal stress difference, $N_1 = σ_{xx}-σ_{zz}$ at short (in…
The failure of the population of micro-junctions forming the frictional interface between two solids is central to fields ranging from biomechanics to seismology. This failure is mediated by the propagation along the interface of various types of rupture fronts, covering a wide range of velocities. Among them are so-called slow fronts, which are recently discovered fronts much slower than the materials' sound speeds. Despite intense modelling activity, the mechanisms underlying slow fronts remain elusive. Here, we introduce a multi-scale model capable of reproducing both the transition from fa…
Using Molecular Dynamics simulations of a polymer liquid flowing past flat and patterned surfaces, we investigate the influence of corrugation, wettability and pressure on slippage and friction at the solid-liquid interface. For one-dimensional, rectangular grooves, we observe a gradual crossover between the Wenzel state, where the liquid fills the grooves, and the Cassie state, where the corrugation supports the liquid and the grooves are filled with vapor. Using two independent flow set-ups, we characterize the near-surface flow by the slip length, $δ$, and the position, $z_\textrm{h}$, at w…
When adhesive elastomeric materials slide over hard rough surfaces at low velocities, there are two primary dissipative mechanisms that control how friction changes with sliding velocity: viscoelastic dissipation and adhesive dissipation. To distinguish the contribution of these dissipative mechanisms we have measured frictional shear stresses for crosslinked polydimethylsiloxane (PDMS) on three different rough surfaces of similar surface chemistry across nearly six decades of sliding velocity. The results show that the observed friction is dominated by adhesive dissipation, rather than viscoe…
We study the frictional behavior of both elastic and viscoelastic thin coatings bonded to a seemingly rigid substrate and sliding against a rough profile in the presence of Coulomb friction at the interface. The aim is to explore the effect of the coupling between the normal and tangential displacement fields arising from the finiteness of the material thickness and to quantify the contribution this can have on energy losses. We found that, due to normal-tangential coupling, asymmetric contacts and consequently additional friction are observed even for purely elastic layers, indeed associated …
We report on normal contact and friction measurements of model multicontact interfaces formed between smooth surfaces and substrates textured with a statistical distribution of spherical micro-asperities. Contacts are either formed between a rigid textured lens and a smooth rubber, or a flat textured rubber and a smooth rigid lens. Measurements of the real area of contact $A$ versus normal load $P$ are performed by imaging the light transmitted at the microcontacts. For both interfaces, $A(P)$ is found to be sub-linear with a power law behavior. Comparison to two multi-asperity contact models,…
