We show that simulations of polymer rheology at a fluctuating mesoscopic scale and at the macroscopic scale where flow instabilities occur can be achieved at the same time with dissipative particle dynamics (DPD) technique.} We model the visco-elasticity of polymer liquids by introducing a finite fraction of dumbbells in the standard DPD fluid. The stretching and tumbling statistics of these dumbbells is in agreement with what is known for isolated polymers in shear flows. At the same time, the model exhibits behaviour reminiscent of drag reduction in the turbulent state: as the polymer fraction increases, the onset of turbulence in plane Couette flow is pushed to higher Reynolds numbers. The method opens up the possibility to model nontrivial rheological conditions with ensuing coarse grained polymer statistics.
As a stiff polymer tumbles in shear flow, it experiences compressive viscous forces that can cause it to buckle and undergo a sequence of morphological transitions with increasing flow strength. We use numerical simulations to uncover the effects of these transitions on the steady shear rheology of a dilute suspension of stiff polymers. Our results agree with classic scalings for Brownian rods in relatively weak flows but depart from them above the buckling threshold. Signatures of elastoviscous buckling include enhanced shear thinning and an increase in the magnitude of normal stress differen…
Orientational origin of nonlinear shear rheology in unentangled polymer melts
Department of Chemical Science and Engineering, Kyoto University（京都大学化学工程系）；Advanced Manufacturing Technology Institute, Kanazawa University（金泽大学先进制造技术研究所）
We use non-equilibrium atomistic molecular dynamics simulations of unentangled melts of linear and star polymers ($\mathrm{C_{25}H_{52}}$) to study the steady-state viscoelastic response under confinement within nanoscale hematite $\left ( \mathrm{α-Fe_2O_3} \right )$ channels. We report (i) the negative (positive) first (second) normal stress difference and (ii) the presence of viscoelastic tension at low shear rates. We link these effects to bond alignment such that chains near the surface can carry the elastic force exerted on the walls, which decays as the chains become more aligned in the…
We use Brownian dynamics (BD) simulations and single molecule experiments to investigate the influence of topological constraints and hydrodynamic interactions on the dynamics and rheology of solutions of ring-linear polymer blends at the overlap concentration. We find agreement between simulation and experiment in that rings in solution blends exhibit large conformational fluctuations, including extension overshoots in the startup of flow and tumbling and tank-treading at steady state. Ring polymer fluctuations increase with blend fraction of linear polymers and are peaked at a ring Weissenbe…
We investigate the steady-state extensional rheology of a dilute suspension of spherical particles in a dilute polymer solution. For a particle-free polymeric fluid, in addition to the solvent viscosity, the extensional viscosity due to the polymers, $μ^\text{poly}$, contributes to the total non-dimensionalized extensional viscosity $1+μ^\text{poly}$. When a small volume fraction, $ϕ$, of spheres is added to a polymeric fluid, the stress is altered by the Einstein viscosity of 2.5$ϕ$ and two additional stress contributions: the interaction stresslet and the particle-induced polymer stress (PIP…
The dynamic rheology of a polymer melt composed of short chains with ten beads between rapidly oscillating plates is investigated for various oscillation frequencies by using the hybrid simulation of the molecular dynamics and computational fluid dynamics. In the rapidly oscillating plates, non-uniform boundary layer flows are generated over the plate due to inertia of the fluid, and the local rheological properties of the melt are spatially varied according to the local flow fields. Far from the plate, the local strain decreases as the oscillation frequency increases such that the dynamic rhe…
Encapsulation of chemicals using polymer membranes enables to control their transport and delivery for applications such as agrochemistry or detergency. To rationalize the design of polymer capsules, it is necessary to understand how the membranes' mechanical properties control the transport and release of the cargo. In this article, we use microfluidics to produce model polymer capsules and study in situ their behavior in controlled elongational flows. Our model capsules are obtained by assembling polymer mono and hydrogen-bonded bilayers at the surface of an oil droplet in water. We also use…
Extensional rheometry of mobile fluids. Part II: Comparison between the uniaxial, planar and biaxial extensional rheology of dilute polymer solutions using numerically-optimized stagnation point microfluidic devices
As the first endeavour, we have analyzed the pulsatile flow of Oldroyd-B viscoelastic fluid where the combined effects of fluid elasticity and pulsation parameters on the flow characteristics are numerically studied at a low Reynolds number. Computations are performed using a finite-volume based open-source solver OpenFOAM by appending the log-conformation tensor approach to stabilize the numerical solution at high Deborah number. Significant flow velocity enhancement is achieved by increasing the viscoelastic behaviour of the fluid. High-velocity gradient zones and high polymeric stress regio…
We investigate the shear thinning of red blood cell - dextran suspensions. Microscopic images show that at low polymer concentration, aggregation increases with increasing concentration until it reaches a maximum and then decreases again to non-aggregation. This bell shape dependency is also deduced from the rheological measurements, if the data are correctly normalized by the viscosity of the suspending phase since a significant amount of polymers adsorb to the cell surfaces. We find that the position of the maximum of this shear rate dependent bell shape increases with increasing viscosity o…
X-ray particle tracking velocimetry for steady-state rheological characterization: Case study of a complex polymer melt flow in material extrusion additive manufacturing
University of Stuttgart（斯图加特大学）；University of Milan（米兰大学）；CNR – Consiglio Nazionale delle Ricerche, Istituto di Chimica della Materia Condensata e di Tecnologie per l’Energia（意大利国家研究委员会凝聚态材料与能源技术研究所）
In this study, we report the use of digital holography microscopy (DHM) for 3D-resolved flow kinematics and shear rheometry of viscoelastic polymeric fluids. We computationally reconstruct the recorded holograms to visualize the tracer imbued flow volume in microchannels, followed by implementation of particle tracking velocimetry (PTV) to quantitate spatially-resolved velocity fields in 3D. In order to select optimal parameters for DHM-PTV characterization of complex fluids, we studied the effect of hologram recording distance, seeding density and particle size. Using the optimal parameters, …
We briefly review the recent advances in the rheology of entangled polymers and identify emerging research trends and outstanding challenges, especially with respect to branched polymers. Emphasis is placed on the role of well-characterized model systems, as well as the synergy of synthesis-characterization, rheometry and modeling/simulations. The theoretical framework for understanding the observed linear and nonlinear rheological phenomena is the tube model which is critically assessed in view of its successes and shortcomings, whereas alternative approaches are briefly discussed. Finally, i…
We investigate previously unclarified effects of fluid elasticity on shear-thickening in dilute suspensions in an Oldroyd-B viscoelastic fluid using a novel direct numerical simulation based on the smoothed profile method. Fluid elasticity is determined by the Weissenberg number Wi and by viscosity ratio $1-β=η_p/(η_s+η_p)$ which measures the coupling between the polymer stress and flow: $η_p$ and $η_s$ are the polymer and solvent viscosity, respectively.As $1-β$ increases, while the stresslet does not change significantly compared to that in the $β\to 1$ limit, the growth rate of the normaliz…
We simulate complex fluids by means of an on-the-fly coupling of the bulk rheology to the underlying microstructure dynamics. In particular, a macroscopic continuum model of polymeric fluids is constructed without a pre-specified constitutive relation, but instead it is actively learned from mesoscopic simulations where the dynamics of polymer chains is explicitly computed. To couple the macroscopic rheology of polymeric fluids and the microscale dynamics of polymer chains, the continuum approach (based on the finite volume method) provides the transient flow field as inputs for the (mesoscopi…
Surface tension-driven flow techniques have recently emerged as an efficient means of shedding light into the rheology of thin polymer films. Motivated by experimental and theoretical approaches in films bearing a varying surface topography, we present results on the capillary relaxation of a square pattern at the free surface of a viscoelastic polymer film, using molecular dynamics simulations of a coarse-grained polymer model. Height profiles are monitored as a function of time after heating the system above its glass-transition temperature and their time dependence is fitted to the theory o…
Thin polymer films have striking dynamical properties that differ from their bulk counterparts. With the simple geometry of a stepped polymer film on a substrate, we probe mobility above and below the glass transition temperature $T_{\textrm{g}}$. Above $T_{\textrm{g}}$ the entire film flows, while below $T_{\textrm{g}}$ only the near surface region responds to the excess interfacial energy. An analytical thin film model for flow limited to the free surface region shows excellent agreement with sub-$T_{\textrm{g}}$ data. The system transitions from whole film flow to surface localized flow ove…
