Scacchi Alberto, Krüger Matthias, Brader Joseph M
Department of Physics, University of Fribourg, CH-1700 Fribourg, Switzerland.
J Phys Condens Matter. 2016 Jun 22;28(24):244023. doi: 10.1088/0953-8984/28/24/244023. Epub 2016 Apr 26.
The classical dynamical density functional theory (DDFT) provides an approximate extension of equilibrium DFT to treat nonequilibrium systems subject to Brownian dynamics. However, the method fails when applied to driven systems, such as sheared colloidal dispersions. The breakdown of DDFT can be traced back to an inadequate treatment of the flow-induced distortion of the pair correlation functions. By considering the distortion of the pair correlations to second order in the flow-rate we show how to systematically correct the DDFT for driven systems. As an application of our approach we consider Poiseuille flow. The theory predicts that the particles will accumulate in spatial regions where the local shear rate is small, an effect known as shear-induced migration. We compare these predictions to Brownian dynamics simulations with generally good agreement.
经典动力学密度泛函理论(DDFT)提供了平衡密度泛函理论的一种近似扩展,用于处理受布朗动力学影响的非平衡系统。然而,该方法应用于驱动系统(如剪切胶体分散体)时会失效。DDFT的失效可追溯到对流量诱导的对关联函数畸变处理不当。通过考虑对关联在流速二阶项上的畸变,我们展示了如何系统地修正驱动系统的DDFT。作为我们方法的一个应用,我们考虑泊肃叶流。该理论预测粒子将在局部剪切率较小的空间区域积累,这一效应称为剪切诱导迁移。我们将这些预测与布朗动力学模拟结果进行比较,总体上吻合良好。