Formation of double helical and filamentous structures in models of physical and chemical gels

Abstract

This Highlight discusses two recent models, one that captures physical network formation starting from the molecular architecture of its constituents and another that contains the basic features of phase separation in cross-linked polymer gels: A) the Janus chain (multibead bead-spring type) model exhibiting semiflexibility and induced curvature and B) a stretched elastic network of Lennard-Jones particles. The length scales and related structures predicted by the two generic models are different. Model B, a generic soft solid model, exhibits hysteresis and the formation of filamentous structures in two dimensions. The Janus chain model A is able to describe the process of the formation of double helical superstructures, will be operated in three dimensions, and its internal parameters are directly deduced from atomistic simulation. Both models rely on classical ingredients which have been separately studied extensively: i) the Lennard-Jones particle system, ii) the elastic solid, and iii) the FENE-B model for semiflexible, finitely extendable nonlinear elastic (FENE) polymer chains. While model A combines i) and iii), model B combines i) and ii). This aspect of technical simplicity, however, is contrasted by the rich phenomenology observed for these models. The Janus model even resolves structure formation on the molecular scale. Intriguingly, the coarse dynamical models capture a wide range of superstructures known for polymeric networks and therefore clearly serve to understand their underlying physical mechanisms.