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Contacts between particles in dense, sheared suspensions are believed to underpin much of their rheology. Roughness and adhesion are known to constrain the relative motion of particles, and thus globally affect the shear response, but an experimental description of how they microscopically influence the transmission of forces and relative displacements within contacts is lacking. Here we show that an innovative colloidal-probe atomic force microscopy technique allows the simultaneous measurement of normal and tangential forces exchanged between tailored surfaces and microparticles while tracking their relative sliding and rolling, unlocking the direct measurement of coefficients of rolling friction, as well as of sliding friction. We demonstrate that, in the presence of sufficient traction, particles spontaneously roll, reducing dissipation and promoting longer-lasting contacts. Conversely, when rolling is prevented, friction is greatly enhanced for rough and adhesive surfaces, while smooth particles coated by polymer brushes maintain well-lubricated contacts. We find that surface roughness induces rolling due to load-dependent asperity interlocking, leading to large off-axis particle rotations. In contrast, smooth, adhesive surfaces promote rolling along the principal axis of motion. Our results offer direct values of friction coefficients for numerical studies and an interpretation of the onset of discontinuous shear thickening based on them, opening up new ways to tailor rheology via contact engineering., Comment: 7 Figures

The underlying mechanisms and physics of catalytic Janus microswimmers is highly complex, requiring details of the associated phoretic fields and the physiochemical properties of catalyst, particle, boundaries, and the fuel used. Therefore, developing a minimal (and more general) model capable of capturing the overall dynamics of these autonomous particles is highly desirable. In the presented work, we demonstrate that a coarse-grained dissipative particle-hydrodynamics model is capable of describing the behaviour of various chemical microswimmer systems. Specifically, we show how a competing balance between hydrodynamic interactions experienced by a squirmer in the presence of a substrate, gravity, and mass and shape asymmetries can reproduce a range of dynamics seen in different experimental systems. We hope that our general model will inspire further synthetic work where various modes of swimmer motion can be encoded via shape and mass during fabrication, helping to realise the still outstanding goal of microswimmers capable of complex 3-D behaviour

Shear thickening denotes the reversible increase in viscosity of a suspension of rigid particles under external shear. This ubiquitous phenomenon has been documented in a broad variety of multiphase particulate systems, while its microscopic origin has been successively attributed to hydrodynamic interactions and frictional contact between particles. The relative contribution of these two phenomena to the magnitude of shear thickening is still highly debated and we report here a discriminating experimental study using a model shear-thickening suspension that allows us to tune independently both the surface chemistry and the surface roughness of the particles. We show here that both properties matter when it comes to continuous shear thickening (CST) and that the presence of hydrogen bonds between the particles is essential to achieve discontinuous shear thickening (DST) by enhancing solid friction between closely contacting particles. Moreover, a simple argument allows us to predict the onset of CST, which for these very rough particles occurs at a critical volume fraction much lower than that previously reported in the literature. Finally, we demonstrate how mixtures of particles with opposing surface chemistry make it possible to finely tune the shear-thickening response of the suspension at a fixed volume fraction, paving the way for a fine control of the shear-thickening transition in engineering applications., Comment: 16 pages, 16 figures