Molecular Modeling and Simulation of Polymer Nanocomposites at Multiple Length Scales

Abstract

The complexity of intermolecular interactions and confinement in polymer—nanoparticle systems leads to spatial variations in structure and dynamics at both the meso and nanoscale. Molecular simulation holds great promise as a means of predicting these effects and understanding their microscopic origin. In order to shed some light onto local structure and segmental dynamics of atactic polystyrene/silica (PS/SiO2) and atactic polystyrene/fullerene (PS/C60) melt systems, molecular simulations have been conducted using two interconnected levels of representation: 1) A coarse-grained representation. Equilibration of coarse-grained polymer-nanoparticle systems at all length scales is achieved via connectivity-altering Monte Carlo simulations. 2) An atomistic representation. Initial configurations for atomistic molecular dynamics (MD) simulations are obtained by reverse mapping well-equilibrated coarse-grained configurations. The local structure around a silica nanoparticle immersed in the PS matrix, PS segmental, and local dynamics in both composites and mechanical properties and entanglements in PS/SiO2 are studied.