Systematic time-scale-bridging molecular dynamics applied to flowing polymer melts

Abstract

We present a thermodynamically guided, low-noise, time-scale-bridging, and pertinently efficient strategy for the dynamic simulation of microscopic models for complex fluids. The systematic coarse-graining method is exemplified for low-molecular polymeric systems subjected to homogeneous flow fields. We use established concepts of nonequilibrium thermodynamics and an alternating Monte Carlo-molecular-dynamics iteration scheme in order to obtain the model equations for the slow variables. For chosen flow situations of interest, the established model predicts structural as well as material functions beyond the regime of linear response. As a by-product, we present steady-state simulation results for polymers in general flow situations, including simple, planar, and yet unexplored equibiaxial elongation. The method is simple to implement and allows for the calculation of time-dependent behavior through quantities readily available from nonequilibrium steady states.