 Award ID(s):
 1628974
 NSFPAR ID:
 10323008
 Date Published:
 Journal Name:
 Journal of Rheology
 Volume:
 66
 Issue:
 3
 ISSN:
 01486055
 Format(s):
 Medium: X
 Sponsoring Org:
 National Science Foundation
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Polymer synthesis routes result in macromolecules with molecular weight dispersity ĐM that depends on the polymerization mechanism. The lowest dispersity polymers are those made by anionic and atomtransfer radical polymerization, which exhibit narrow distributions ĐM = Mw/Mn ∼ 1.02–1.04. Even for small dispersity, the chain length can vary by a factor of two from the average. The impact of chain length dispersity on the viscoelastic response remains an open question. Here, the effects of dispersity on stress relaxation and shear viscosity of entangled polyethylene melts are studied using molecular dynamics simulations. Melts with chain length dispersity, which follow a Schulz–Zimm (SZ) distribution with ĐM = 1.0–1.16, are studied for times up to 800 μs, longer than the terminal time. These systems are compared to those with binary and ternary distributions. The stress relaxation functions are extracted from the Green–Kubo relation and from stress relaxation following a uniaxial extension. At short and intermediate time scales, both the mean squared displacement and the stress relaxation function G(t) are independent of ĐM. At longer times, the terminal relaxation time decreases with increasing ĐM. In this time range, the faster motion of the shorter chains results in constraint release for the longer chains.more » « less

Poole, Robert J (Ed.)The FENEP (FinitelyExtensible Nonlinear Elastic) dumbbell constitutive equation is widely used in simulations and stability analyses of free and wallbounded viscoelastic shear flows due to its relative simplicity and accuracy in predicting macroscopic properties of dilute polymer solutions. The model contains three independent material parameters, which expressed in dimensionless form correspond to a Weissenberg number (Wi), i.e., the ratio of the dumbbell relaxation time scale to a characteristic flow time scale, a finite extensibility parameter (L), corresponding to the ratio of the fully extended dumbbell length to the root mean square endtoend separation of the polymer chain under equilibrium conditions, and a solvent viscosity ratio. An exact solution for the rheological predictions of the FENEP model in steady simple shear flow is available [Sureshkumar et al., Phys Fluids (1997)], but the resulting nonlinear and nested set of equations do not readily reveal the key shearthinning physics that dominates at high Wi as a result of the finite extensibility of the polymer chain. In this note we review a simple way of evaluating the steady material functions characterizing the nonlinear evolution of the polymeric contributions to the shear stress and first normal stress difference as the shear rate increases, provide asymptotic expansions as a function of Wi , and show that it is in fact possible to construct universal master curves for these two material functions as well as the corresponding stress ratio. Steady shear flow experiments on three highly elastic dilute polymer solutions of different finite extensibilities also follow the identified master curves. The governing dimensionless parameter for these master curves is Wi/L and it is only in strong shear flows exceeding Wi/L > 1 that the effects of finite extensibility of the polymer chains dominate the evolution of polymeric stresses in the flow field. We suggest that reporting the magnitude of Wi/L when performing stability analyses or simulating sheardominated flows with the FENEP model will help clarify finite extensibility effects.more » « less

Mud is a suspension of finegrained particles (sand, silt, and clay) in water. The interaction of clay minerals in mud gives rise to complex rheological behaviors, such as yield stress, thixotropy, and viscoelasticity. Here, we experimentally examine the flow behaviors of kaolinite clay suspensions, a model mud, using steady shear rheometry. The flow curves exhibit both yield stress and rheological hysteresis behaviors for various kaolinite volume fractions (ϕk). Further understanding of these behaviors requires fitting to existing constitutive models, which is challenging due to numerous fitting parameters. To this end, we employ a Bayesian inference method, Markov chain Monte Carlo, to fit the experimental flow curves to a microstructural viscoelastic model. The method allows us to estimate the rheological properties of the clay suspensions, such as viscosity, yield stress, and relaxation time scales. The comparison of the inherent relaxation time scales suggests that kaolinite clay suspensions are strongly viscoelastic and weakly thixotropic at relatively low ϕk, while being almost inelastic and purely thixotropic at high ϕk. Overall, our results provide a framework for predictive model fitting to elucidate the rheological behaviors of natural materials and other structured fluids.

The transition from laminar to turbulent flow is of great interest since it is one of the most difficult and unsolved problems in fluids engineering. The transition processes are significantly important because the transition has a huge impact on almost all systems that come in contact with a fluid flow by altering the mixing, transport, and drag properties of fluids even in simple pipe and channel flows. Generally, in most transportation systems, the transition to turbulence causes a significant increase in drag force, energy consumption, and, therefore, operating cost. Thus, understanding the underlying mechanisms of the laminartoturbulent transition can be a major benefit in many ways, especially economically. There have been substantial previous studies that focused on testing the stability of laminar flow and finding the critical amplitudes of disturbances necessary to trigger the transition in various wallbounded systems, including circular pipes and square ducts. However, there is still no fundamental theory of transition to predict the onset of turbulence. In this study, we perform direct numerical simulations (DNS) of the transition flows from laminar to turbulence in a channel flow. Specifically, the effects of different magnitudes of perturbations on the onset of turbulence are investigated. The perturbation magnitudes vary from 0.001 (0.1%) to 0.05 (5%) of a typical turbulent velocity field, and the Reynolds number is from 5,000 to 40,000. Most importantly, the transition behavior in this study was found to be in good agreement with other reported studies performed for fluid flow in pipes and ducts. With the DNS results, a finite amplitude stability curve was obtained. The critical magnitude of perturbation required to cause transition was observed to be inversely proportional to the Reynolds number for the magnitude from 0.01 to 0.05. We also investigated the temporal behavior of the transition process, and it was found that the transition time or the time required to begin the transition process is inversely correlated with the Reynolds number only for the magnitude from 0.02 to 0.05, while different temporal behavior occurs for smaller perturbation magnitudes. In addition to the transition time, the transition dynamics were investigated by observing the time series of wall shear stress. At the onset of transition, the shear stress experiences an overshoot, then decreases toward sustained turbulence. As expected, the average values of the wall shear stress in turbulent flow increase with the Reynolds number. The change in the wall shear stress from laminar to overshoot was, of course, found to increase with the Reynolds number. More interestingly was the observed change in wall shear stress from the overshoot to turbulence. The change in magnitude appears to be almost insensitive to the Reynolds number and the perturbation magnitude. Because the change in wall shear stress is directly proportional to the pumping power, these observations could be extremely useful when determining the required pumping power in certain flow conditions. Furthermore, the stability curve and wall shear stress changes can be considered robust features for future applications, and ultimately interpreted as evidence of progress toward solving the unresolved fluids engineering problem.more » « less

Dissipative particle dynamics (DPD) simulations are performed on coarsegrained replicas of linear, monodisperse entangled polyethylene melts [Formula: see text] and [Formula: see text] undergoing both steadystate and transient planar elongational flow (PEF). The fidelity of the DPD simulations is verified by direct comparison of flow topological and rheological properties of a 334particle chain liquid against the unitedatom [Formula: see text] liquid, simulated using nonequilibrium molecular dynamics (NEMD). These DPD simulations demonstrate that a flowinduced coilstretch transition (CST) and its associated hysteresis caused by configurational microphase separation, as observed in previous NEMD simulations of PEF, can be replicated using a more computationally efficient coarsegrained system. Results indicate that the breadth of the CST hysteresis loop is enlarged for the longer molecule liquid relative to the shorter one. Furthermore, relaxation simulations reveal that reducing the applied flow Deborah number ([Formula: see text]) from a high value corresponding to a homogeneous phase of highly stretched molecules to a [Formula: see text] within the biphasic region results in a twostage relaxation process. There is a fast initial stratification of the kinetically trapped highly stretched chains into regions of highly extended and less extended chains, which displays similar behavior to a system undergoing a spinodal decomposition caused by spatial configurational free energy fluctuations. After a short induction period of apparently random duration, the less extended chain regions experience a stochastic nucleation event that induces configurational relaxation to domains composed of coiled molecules over a much longer time scale, leaving the more highly extended chains in surrounding sheetlike domains. The time scales of these two relaxation processes are of the same order of magnitude as the Rouse and disengagement times of the equilibrium liquids.