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非线性微观流变学:体积应力与直接相互作用

Nonlinear microrheology: bulk stresses versus direct interactions.

作者信息

Squires Todd M

机构信息

Department of Chemical Engineering, University of California-Santa Barbara, CA 93106, USA.

出版信息

Langmuir. 2008 Feb 19;24(4):1147-59. doi: 10.1021/la7023692. Epub 2007 Dec 22.

Abstract

In passive microrheology, the linear viscoelastic properties of complex fluids are inferred from the Brownian motion of colloidal tracer particles. Active (but gentle) forcing may also be used to obtain such linear-response information. More significant forcing may drive the material significantly out of equilibrium, thus potentially providing a window into the nonlinear response properties of the material. In leaving the linear-response regime, however, the theoretical underpinning for passive microrheology is lost, and a variety of issues arise. Most generally, what exactly can be measured, and how can such measurements be interpreted? Here we motivate and discuss a variety of theoretical issues facing the interpretation of active microrheology. First, in the continuum limit, the inhomogeneous velocity field around the probe gives rise to rheological inhomogeneities, whereupon an assumed generalized Stokes drag yields a weighted average of the viscosities around the probe rather than the (homogeneous) viscosity measured macroscopically. We then explicitly treat the material microstructure using a model system (a large colloidal probe pulled through a dilute suspension of small bath particles). We examine the different sources of stress upon the probe particle (e.g., direct probe-bath collisions as well as microstructural deformations within the bulk suspension) and discuss their analog (or lack thereof) in the corresponding macrorheological system. We discuss several crucial issues for the interpretation of nonlinear microrheology: (1) how to interpret the inhomogeneous and nonviscometric nature of the deformation field around the probe, (2) the distinction between direct and bulk stresses and their deconvolution, and (3) the (Lagrangian) time-dependent nature of the stress histories experienced by material elements as they advect past the probe. Having identified these issues, we briefly discuss adaptations of the basic technique to recover bulk rheology more faithfully. Whereas we specifically discuss a model colloidal suspension, we ultimately envision a technique capable of measuring the nonlinear rheology of general materials.

摘要

在被动微流变学中,复杂流体的线性粘弹性特性是通过胶体示踪颗粒的布朗运动推断出来的。也可以使用主动(但温和)驱动来获取此类线性响应信息。更强的驱动可能会使材料显著偏离平衡状态,从而有可能为了解材料的非线性响应特性提供一个窗口。然而,在离开线性响应区域时,被动微流变学的理论基础就不再适用,会出现各种问题。最普遍的是,究竟能测量什么,以及如何解释这些测量结果?在这里,我们提出并讨论主动微流变学解释中面临的各种理论问题。首先,在连续介质极限下,探针周围的非均匀速度场会导致流变学上的不均匀性,于是假定的广义斯托克斯阻力会产生探针周围粘度的加权平均值,而不是宏观测量的(均匀)粘度。然后,我们使用一个模型系统(一个大的胶体探针在小浴颗粒的稀悬浮液中拉动)明确地处理材料微观结构。我们研究了作用在探针颗粒上的不同应力源(例如,探针与浴颗粒的直接碰撞以及整体悬浮液中的微观结构变形),并讨论了它们在相应宏观流变学系统中的类似物(或不存在类似物的情况)。我们讨论了非线性微流变学解释中的几个关键问题:(1)如何解释探针周围变形场的非均匀和非粘性本质,(2)直接应力和整体应力之间的区别及其反褶积,以及(3)材料元素在平流经过探针时所经历的应力历史的(拉格朗日)时间依赖性。在确定了这些问题之后,我们简要讨论了对基本技术的改进,以便更忠实地恢复整体流变学。虽然我们具体讨论的是一个模型胶体悬浮液,但我们最终设想的是一种能够测量一般材料非线性流变学的技术。

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