Viscoelasticity of reversibly crosslinked networks of semiflexible polymers

TL;DR

This paper develops a theoretical model for the viscoelastic behavior of reversible semiflexible polymer networks, emphasizing local network distortions and bending modes, with applications to linear and nonlinear rheology.

Contribution

It introduces a non-affine model that links network strain to local distortions and bending modes, advancing understanding of viscoelasticity in such networks.

Findings

Frequency-dependent linear rheology characterized.

Nonlinear response during creep and strain ramps modeled.

Insights into the role of crosslink dynamics in viscoelasticity.

Abstract

We present a theoretical framework for the linear and nonlinear visco-elastic properties of reversibly crosslinked networks of semiflexible polymers. In contrast to affine models where network strain couples to the polymer end-to-end distance, in our model strain rather serves to locally distort the network structure. This induces bending modes in the polymer filaments, the properties of wich are slaved to the surrounding network structure. Specifically, we investigate the frequency-dependent linear rheology, in particular in combination with crosslink binding/unbinding processes. We also develop schematic extensions to describe the nonlinear response during creep measurements as well as during constant-strainrate ramps.