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Register a new userNon-monotonic density dependence of the diffusion of DNA fragments in low-salt suspensions
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The high linear charge density of 20-base-pair oligomers of DNA is shown to lead to a striking non-monotonic dependence of the long-time self-diffusion on the concentration of the DNA in low-salt conditions. This generic non-monotonic behavior results from both the strong coupling between the electrostatic and solvent-mediated hydrodynamic interactions, and from the renormalization of these electrostatic interactions at large separations, and specifically from the dominance of the far-field hydrodynamic interactions caused by the strong repulsion between the DNA fragments.
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Using super-heterodyne Doppler velocimetry with multiple scattering correction, we extend the opti-cally accessible range of concentrations in experiments on colloidal electro-kinetics. We here meas-ured the electro-phoretic mobility and the DC conductivity of aqueous charged sphere suspensions covering about three orders of magnitude in particle concentrations and transmissions as low as 40%. The extended concentration range for the first time allows the demonstration of a non-monotonic con-centration dependence of the mobility for a single particle species. Our observations reconcile previ-ous experimental observations made on other species over restricted concentration ranges. We com-pare our results to state of the art theoretical calculations using a constant particle charge and the carefully determined experimental boundary conditions as input. In particular, we consider so-called realistic salt free conditions, i.e. we respect the release of counter-ions by the particles, the solvent hydrolysis and the formation of carbonic acid from dissolved neutral CO2. We also compare to previ-ous results obtained under similarly well-defined conditions. This allows identification of three dis-tinct regions of differing density dependence. An ascent during the built up of double layer overlap which is not expected by theory, an extended plateau region in quantitative agreement with theoretical expectation based on a constant effective charge and a sudden decrease which occurs way before the expected gradual decrease. Our observations suggest a relation of the non-monotonic behavior to a decrease of particle charge, and we tentatively discuss possibly underlying mechanisms.
The discontinuous shear thickening (DST) of dense suspensions is a remarkable phenomenon in which the viscosity can increase by several orders of magnitude at a critical shear rate. It has the appearance of a first order phase transition between two hypothetical states that we have recently identified as Stokes flows with lubricated or frictional contacts, respectively. Here we extend the analogy further by means of novel stress-controlled simulations and show the existence of a non-monotonic steady-state flow curve analogous to a non-monotonic equation of state. While we associate DST with an S-shaped flow curve, at volume fractions above the shear jamming transition the frictional state loses flowability and the flow curve reduces to an arch, permitting the system to flow only at small stresses. Whereas a thermodynamic transition leads to phase separation in the coexistence region, we observe a uniform shear flow all along the thickening transition. A stability analysis suggests that uniform shear may be mechanically stable for the small Reynolds numbers and system sizes in a rheometer.
The behaviour in simple shear of two concentrated and strongly cohesive mineral suspensions showing highly non-monotonic flow curves is described. Two rheometric test modes were employed, controlled stress and controlled shear-rate. In controlled stress mode the materials showed runaway flow above a yield stress, which, for one of the suspensions, varied substantially in value and seemingly at random from one run to the next, such that the up flow-curve appeared to be quite irreproducible. The down-curve was not though, as neither was the curve obtained in controlled rate mode, which turned out to be triple-valued in the region where runaway flow was seen in controlled rising stress. For this first suspension, the total stress could be decomposed into three parts to a good approximation: a viscous component proportional to a plastic viscosity, a constant isostatic contribution, and a third shear-rate dependent contribution associated with the particulate network which decreased with increasing shear-rate raised to the -7/10th power. In the case of the second suspension, the stress could be decomposed along similar lines, although the strain-rate softening of the solid-phase stress was found to be logarithmic and the irreducible isostatic stress was small. The flow curves are discussed in the light of recent simulations and they conform to a very simple but general rule for non-monotonic behaviour in cohesive suspensions and emulsions, namely that it is caused by strain-rate softening of the solid phase stress.
We point out unconventional mechanical properties of confined active fluids, such as bacterial suspensions, under shear. Using a minimal model of an active liquid crystal with no free parameters, we predict the existence of a window of bacteria concentration for which a suspension of textit{E.~Coli} effectively behaves, at steady-state, as a negative viscosity fluid and reach quantitative agreement with experimental measurements. Our theoretical analysis further shows that a negative apparent viscosity is due to a non-monotonic local velocity profile, and is associated with a non-monotonic stress vs. strain rate flow curve. This implies that fixed stress and fixed strain rate ensembles are not equivalent for active fluids.
A study of a model rod-like polyelectrolyte molecule immersed into a monovalent or divalent electrolyte is presented. Results from the hypernetted-chain/mean spherical approximation (HNC/MSA) theory, for inhomogeneous charged fluids, {ch are} compared with molecular dynamics (MD) simulations. As a particular case, the parameters of the polyelectrolyte molecule are mapped to those of a DNA molecule. An excellent qualitative, and in some cases quantitative, agreement between HNC/MSA and MD is found. Both, HNC/MSA and MD, predict the occurrence of overcharging, which is not present in the Poisson-Boltzmann theory. Mean electrostatic potential and local concentration profiles, $zeta$-potential and charge distribution functions are obtained and discussed in terms of the observed overcharging effect. Particularly interesting results are a very non-monotonic behavior of the $zeta$-potential, as a function of the rod charge density, and the overcharging by {em monovalent} counterions.
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