Phase Separation in Binary Colloids with Charge Asymmetry

We report that binary dispersions of like-charged colloidal particles with large charge asymmetry but similar size exhibit phase separation into crystal and fluid phases under very low salt conditions. This is unexpected because the effective colloid-colloid pair interactions are accurately described by a Yukawa model which is stable to demixing. We show that colloid-ion interactions provide an energetic driving force for phase separation, which is initiated by crystallization of one species.