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Comprehensive calculations were performed to predict the phase behaviour oflarge spherical colloids mixed with small spherical colloids that act asdepletant. To this end, the free volume theory (FVT) of Lekkerkerker et al.[Europhys. Lett. 20 (1992) 559] is used as a basis and is extended toexplicitly include the hard-sphere character of colloidal depletants into theexpression for the free volume fraction. Taking the excluded volume of thedepletants into account in both the system and the reservoir provides arelation between the depletant concentration in the reservoir and in the systemthat accurately matches with computer simulation results of Dijkstra et al.[Phys. Rev. E 59 (1999) 5744]. Moreover, the phase diagrams for highlyasymmetric mixtures with size ratios q . 0:2 obtained by using this newapproach corroborates simulation results significantly better than earlier FVTapplications to binary hard-sphere mixtures. The phase diagram of a binaryhard-sphere mixture with a size ratio of q = 0:4, where a binary interstitialsolid solution is formed at high densities, is investigated using a numericalfree volume approach. At this size ratio, the obtained phase diagram isqualitatively different from previous FVT approaches for hard-sphere andpenetrable depletants, but again compares well with simulation predictions.

Phase Behaviour of Binary Hard-Sphere Mixtures: Free Volume Theory Including Reservoir Hard-Core Interactions