Brownian dynamics simulation of gelation in soft sphere systems with irreversible bond formation

Abstract

Brownian dynamics simulation is used to study the structure and small-deformation shear rheology of three-dimensional particle gels formed from a model of soft spherical particles incorporating a combination of flexible, irreversible bond formation and non-bonded interparticle interactions. An essential feature of the model is the restriction of angular reorganization of cross-linked aggregates during and after gelation. Numerical data relating to the fractal structure and porosity of the gels are compared with those from some related particle gel simulation models in two and three dimensions. Stress relaxation and frequency dependent rheological properties are determined as a function of the strength and nature of the interparticle interactions, and the results are discussed in relation to structural properties. A linear relationship is demonstrated between the high-frequency modulus and the number of bonds in the gel network.