Using symmetry to elucidate the importance of stoichiometry in colloidal crystal assembly

We demonstrate a method based on symmetry to predict the structure of self-assembling, multicomponent colloidal mixtures. This method allows us to feasibly enumerate candidate structures from all symmetry groups and is many orders of magnitude more computationally efficient than combinatorial enumeration of these candidates. In turn, this permits us to compute ground-state phase diagrams for multicomponent systems. While tuning the interparticle potentials to produce potentially complex interactions represents the conventional route to designing exotic lattices, we use this scheme to demonstrate that simple potentials can also give rise to such structures which are thermodynamically stable at moderate to low temperatures. Furthermore, for a model two-dimensional colloidal system, we illustrate that lattices forming a complete set of 2-, 3-, 4-, and 6-fold rotational symmetries can be rationally designed from certain systems by tuning the mixture composition alone, demonstrating that stoichiometric control can be a tool as powerful as directly tuning the interparticle potentials themselves.