Department of Physics, University of Fribourg, CH-1700 Fribourg, Switzerland.
J Chem Phys. 2013 Sep 14;139(10):104108. doi: 10.1063/1.4820399.
We derive a dynamic Ornstein-Zernike equation for classical fluids undergoing overdamped Brownian motion and driven out of equilibrium. Inhomogeneous two-time correlation functions are obtained from functional differentiation of the one-body density and current with respect to an appropriately chosen external field. Functional calculus leads naturally to non-Markovian equations of motion for the two-time correlators. Memory functions are identified as functional derivatives of a space- and time-nonlocal power dissipation functional. We propose an excess (over ideal gas) dissipation functional that both generates mode-coupling theory for the two-body correlations and extends dynamical density functional theory for the one-body fields, thus unifying the two approaches.
我们推导出经典流体在过阻尼布朗运动和非平衡驱动下的动态奥恩斯坦-泽尔尼克方程。非均匀双时间相关函数是通过对适当选择的外场的单分子密度和电流进行功能微分得到的。泛函演算自然导致双时间相关函数的非马尔可夫运动方程。记忆函数被确定为空间和时间非局部功率耗散泛函的函数导数。我们提出了一个超额(超过理想气体)耗散泛函,它既能产生双体相关的模式耦合理论,又能扩展单分子场的动力学密度泛函理论,从而统一了这两种方法。