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Nonlinear signatures of entangled polymer solutions in active microbead rheology

机译:在活性微珠流变的缠结聚合物溶液的非线性特征

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摘要

We present experimental data and numerical modeling of a nonlinear phenomenon in active magnetic microbead rheology that appears to be common to entangled polymer solutions (EPS). Dynamic experiments in a modest range of magnetic forces show: 1. a short-lived high viscosity plateau, followed by 2. a bead acceleration phase with a sharp drop in apparent viscosity, and 3. a terminal steady state that we show resides on the shear-thinning slope of the steady-state flow curve from cone and plate data. This latter feature implies a new protocol to access the nonlinear steady-state flow curve for many biological EPS only available in microliter-scale volumes. We solve the moment-closure form of the Rolie-Poly kinetic model for EPS hydrodynamics, together with a decoupling approximation that obviates the need for a full 3D flow solver, and show that the model qualitatively reproduces the dynamic experimental sequence above. In this way, we explain the phenomenon in terms of entangled polymer physics, and show how the nonlinear event (acceleration and termination on the shear-thinning response curve) is tunable by the interplay between molecular-scale mechanisms (relaxation via reptation and chain retraction) and magnetic force controls. The experimental conditions mimic movement of cilia tips, bacteria, and sperm in mucus barriers, implying a physiological relevance of the phenomenon, and compelling further development of the fully coupled, 3D flow-microstructure model to achieve quantitative accuracy.
机译:我们提供了主动磁微珠流变中的非线性现象的实验数据和数值模型,该现象似乎对于纠缠的聚合物溶液(EPS)很常见。在适度的磁力范围内进行的动态实验表明:1.寿命短暂的高粘度平稳期,其次; 2.磁珠加速阶段,表观粘度急剧下降;以及3.我们显示的最终稳态存在于圆锥和平板数据得出的稳态流动曲线的剪切稀化斜率。后一个特征暗示了一种新的协议,可以访问仅以微升为单位的许多生物EPS的非线性稳态流量曲线。我们解决了用于EPS流体动力学的Rolie-Poly动力学模型的矩闭合形式,以及消除了对完整3D流动求解器的需要的解耦近似,并表明该模型定性地再现了上面的动态实验序列。通过这种方式,我们从纠缠的聚合物物理学角度解释了这种现象,并展示了非线性事件(剪切稀化响应曲线上的加速和终止)如何通过分子尺度机制(通过复制和链缩回而松弛)之间的相互作用来调节。 )和磁力控制。实验条件模拟纤毛尖端,细菌和精子在粘液屏障中的运动,这暗示了该现象的生理相关性,并促使进一步开发完全耦合的3D流动微结构模型以实现定量精度。

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