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Depletion effects and gelation in a binary hard-sphere fluid

A study of the binary hard-sphere fluid with size ratio [sgrave]B/[sgrave]A = 0.1 is reported. Molecular dynamics and Monte Carlo simulations have been carried out over the mole fraction (x A) range 0.002-0.1 and over the high density range where several recent authors have predicted a thermodynamic demising transition on the basis of integral equations. In this region, there is no evidence of such first-order thermodynamic phase separation, or two fluid phases. The effect of the depletion force, arising from the entropic exclusion of B spheres from between two A spheres, as x B is increased at constant packing fraction y A, is to cause a large increase in the partial pressure of A and the radial distribution function of A at contact, a reduction on the mobility of A, and eventually, at a sufficient x B, the gelation of component A to an open, low coordination, amorphous structure. This gelation transition of A shows discontinuities similar to a glass transition; it can be traced back to the hard sphere g...