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To assess the role of particle roughness in the rheological phenomena of concentrated colloidal suspensions, we develop model colloids with varying surface roughness length scales up to 10% of the particle radius. Increasing surface roughness shifts the onset of both shear thickening and dilatancy towards lower volume fractions and critical stresses. Experimental data are supported by computer simulations of spherical colloids with adjustable friction coefficients, demonstrating that a reduction in the onset stress of thickening and a sign change in the first normal stresses occur when friction competes with lubrication. In the quasi-Newtonian flow regime, roughness increases the effective packing fraction of colloids. As the shear stress increases and suspensions of rough colloids approach jamming, the first normal stresses switch signs and the critical force required to generate contacts is drastically reduced. This is likely a signature of the lubrication films giving way to roughness-induced tangential interactions that bring about load-bearing contacts in the compression axis of flow., National Science Foundation (U.S.) (Award 1232937), National Science Foundation (U.S.) (Award 1602183), United States. Army Research Office (Grant W911NF10-1-0518)

We investigate experimentally??-phage and T2-coliphage DNA molecules near both non-adsorbing glass and adsorbing 3-aminopropyltriethoxysilane (APTES)-coated glass surfaces in a simple steady shearing flow generated by a torsional flow cell. The DNA molecular deformations near the surface are found to be considerably weaker than in bulk flow at the same shear rate. This affects the DNA molecule???s deposition and stretching on the adsorbing surface. Surprisingly, for a simple shearing flow in the torsional shearing device, the observed stretch, for molecules both near (<10????m) the surface and adsorbed to it, is much less than predicted by simulations.

The???hierarchical model??? proposed earlier [Larson in Macromolecules 34:4556???4571, 2001] is herein modified by inclusion of early time fluctuations and other refinements drawn from the theories of Milner and McLeish for more quantitative prediction. The hierarchical model predictions are then compared with experimental linear viscoelastic data of well-defined long chain branched 1,4-polybutadienes and 1,4-polyisoprenes using a single set of parameter values for each polymer, which are obtained from experimental data for monodisperse linear and star polymers. For a wide range of monodisperse branched polymer melts, the predictions of the hierarchical model for monodisperse melts are very similar to those of the Milner???McLeish theories, and agree well with experimental data for many, but not all, of the branched polymer samples. Since the modified hierarchical model accounts for arbitrary polydispersity in molecular weight and branching distributions, which is not accounted for in the Milner???McLeish theories, the hierarchical algorithm is a promising one for predicting the relaxation of general mixtures of branched polymers.

The???dual constraint??? model developed by Mead, Van Dyke et???al. is here extended by inclusion of???early-time??? contour-length fluctuations and constraint-release Rouse relaxation, and then evaluated by comparing its predictions with literature data for over 50 different linear and star polymers. By combining the reptation model of Doi and Edwards with contour-length fluctuations and constraint release, the model provides a systematic approach to prediction of the rheological properties of polymers. The parameters are taken from the literature and used consistently for linear polymers, star polymers, and their mixtures having the same chemical compositions. In most cases, the predictions of the model appears to agree well with data for monodisperse, bidisperse, and polydisperse linear and star polymers, except at low molecular weights.

???The results of an experimental study to measure the tumbling parameter,??, for various small-molecule liquid crystals and their mixtures are presented. The methods used include textural observations (twist walls), a direct method, a rheological method, and the oscillatory method developed by Mather, Pearson, and Burghardt in 1995. The single-component results are compared with a molecular theory derived in 1995 by Archer and Larson as well as Kr??ger and Sellers, which predicts the temperature dependence of??, while the results from the binary mixtures are compared to a continuum theory derived by Rey in 1996, giving the concentration dependence of??. The results from the four experimental methods agree with each other for single-component liquid crystals, but not for mixtures. This suggests a failure of the single director Leslie-Ericksen theory to describe the rheology of liquid crystal mixtures.