Relation between aggregation and phase separation: three-dimensional Monte Carlo simulations.

We study phase separation of particles in solution using Monte Carlo simulations of reversible aggregation on a cubic lattice. Two stages of the phase separation can be clearly distinguished: initial random aggregation and subsequent densification. Step one leads to a distribution of fractal aggregates close to the binodal and to a temporary gel for large attractive interaction. Step two leads to isolated spherical dense domains close to the binodal and branched wormlike strands for large attractive interactions. The transition between the two types of structure is gradual and there is no clear feature that shows the existence of a spinodal. The first stage of the phase separation is metastable very close to the binodal or at very large interaction energy. In the latter case, the second step can be viewed as an aging process of the gel formed in the first step.