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We studied crystal structures in mixtures of large and small oppositely charged spherical colloids with size ratio 0.31 using Monte Carlo simulations and confocal microscopy. We developed an interactive method based on simulated annealing to predict new binary crystal structures with stoichiometries from 1 to 8. Employing these structures in Madelung energy calculations using a screened Coulomb potential, we constructed a ground-state phase diagram, which shows a remarkably rich variety of crystals. Our phase diagram displays colloidal analogs of simple-salt structures and of the doped fullerene C60 structures, but also novel structures that do not have an atomic or molecular analog. We found three of the predicted structures experimentally, which provides confidence that our method yields reliable results.

Prediction and Observation of Crystal Structures of Oppositely Charged Colloids