Polymer fluctuation lubrication in hydrogel gemini interfaces.

Interfacial sliding speed and contact pressure between the sub-units of particulate soft matter assemblies can vary dramatically across systems and with dynamic conditions. By extension, frictional interactions between particles may play a key role in their assembly, global configuration, collective motion, and bulk material properties. For example, in tightly packed assemblies of microgels - colloidal microspheres made of hydrogel - particle stiffness controls the fragility of the glassy state formed by the particles. The interplay between particle stiffness and shear stress is likely mediated by particle-particle normal forces, highlighting the potential role of hydrogel-hydrogel friction. Here we study friction at a twinned "Gemini" interface between hydrogels. We construct a lubrication curve that spans four orders of magnitude in sliding speed, and find qualitatively different behaviour from traditional lubrication of engineering material surfaces; fundamentally different types of lubrication occur at the hydrogel Gemini interface. We also explore the role played by polymer solubility and hydrogel-hydrogel adhesion in hydrogel friction. We find that polymer network elasticity, mesh size, and single-chain relaxation times can describe friction at the gel-gel interface, including a transition between lubrication regimes with varying sliding speed.

Elastic contact mechanics: percolation of the contact area and fluid squeeze-out.

The dynamics of fluid flow at the interface between elastic solids with rough surfaces depends sensitively on the area of real contact, in particular close to the percolation threshold, where an irregular network of narrow flow channels prevails. In this paper, numerical simulation and experimental results for the contact between elastic solids with isotropic and anisotropic surface roughness are compared with the predictions of a theory based on the Persson contact mechanics theory and the Bruggeman effective medium theory. The theory predictions are in good agreement with the experimental and numerical simulation results and the (small) deviation can be understood as a finite-size effect. The fluid squeeze-out at the interface between elastic solids with randomly rough surfaces is studied. We present results for such high contact pressures that the area of real contact percolates, giving rise to sealed-off domains with pressurized fluid at the interface. The theoretical predictions are compared to experimental data for a simple model system (a rubber block squeezed against a flat glass plate), and for prefilled syringes, where the rubber plunger stopper is lubricated by a high-viscosity silicon oil to ensure functionality of the delivery device. For the latter system we compare the breakloose (or static) friction, as a function of the time of stationary contact, to the theory prediction.

Static or breakloose friction for lubricated contacts: the role of surface roughness and dewetting.

We present experimental data for the static or breakloose friction for lubricated elastomer contacts, as a function of the time of stationary contact. Due to fluid squeeze-out from the asperity contact regions, the breakloose friction force increases continuously with the time of stationary contact. We consider three different cases: (a) PDMS rubber balls against flat smooth glass surfaces, (b) PDMS cylinder ribs against different substrates (glass, smooth and rough PMMA and an inert polymer) and (c) application to syringes. Due to differences in the surface roughness and contact pressures the three systems exhibit very different time dependences of the breakloose friction. In case (a) for rough surfaces the dry contact area A is a small fraction of the nominal contact area A0, and the fluid squeeze-out is fast. In case (b) the dry contact area is close to the nominal contact area, A/A0 ≈ 1, and fluid squeeze-out is very slow due to percolation of the contact area. In this case, remarkably, different fluids with very different viscosities, ranging from 0.005 Pa s (water­glycerol mixture) to 1.48 Pa s (glycerol), give very similar breakloose friction forces as a function of the time of stationary contact. In case (c) the contact pressure and the surface roughness are larger than in case (b), and the squeeze-out is very slow so that even after a very long time the area of real contact is below the percolation threshold. For all cases (a)­(c), the increase in the breakloose friction is mainly due to the increase in the area of real contact with increasing time, because of the fluid squeeze-out and dewetting.

Adhesion: role of bulk viscoelasticity and surface roughness.

We study the adhesion between smooth polydimethylsiloxane (PDMS) rubber balls and smooth and rough poly(methyl methacrylate) (PMMA) surfaces, and between smooth silicon nitride balls and smooth PDMS surfaces. From the measured viscoelastic modulus of the PDMS rubber we calculate the viscoelastic contribution to the crack-opening propagation energy γeff(v,T) for a wide range of crack tip velocities v and for several temperatures T. The Johnson-Kendall-Roberts (JKR) contact mechanics theory is used to analyze the ball pull-off force data, and γeff(v,T) is obtained for smooth and rough surfaces. We conclude that γeff(v,T) has contributions of similar magnitude from both the bulk viscoelastic energy dissipation close to the crack tip, and from the bond-breaking process at the crack tip. The pull-off force on the rough surfaces is strongly reduced compared to that of the flat surface, which we attribute mainly to the decrease in the area of contact on the rough surfaces.