Effect of Slip-Spring Parameters on the Dynamics and Rheology of Soft, Coarse-Grained Polymer Models.

ABSTRACT

Highly coarse-grained (hCG) linear polymer models allow for accessing long time and length scales by dissipative particle dynamics (DPD). This top-down strategy exploits the universal equilibrium behavior of long, flexible macromolecules by accounting only for the relevant interactions, such as molecular connectivity, and by parametrizing their strength via coarse-grained invariants, such as the mean-squared end-to-end distance. The description of the dynamics of long, entangled polymers, however, poses a challenge because (i) the noncrossability of the molecular backbones is not enforced by the soft interactions of an hCG model and (ii) the rheology involves multiple time and length scales, such as the Rouse-like dynamics on short scales and the reptation dynamics on long scales. One popular technique to effectively mimic the effect of entanglements in linear polymer melts via hCG models is slip-springs, and quantitative agreement with simulations that explicitly account for the noncrossability of molecular contours, experiments, and theoretical predictions has been achieved by identifying the time, length, and energy scales of the hCG model and adjusting the number of slip-springs per macromolecule. In the present work, we study how the spatial extent and the mobility of slip-springs affect the dynamics and discuss their implications in the choice of the degree of coarse-graining in computationally efficient hCG models.