Tuning the Glass Transition: Enhanced Crystallization of the Laves Phases in Nearly Hard Spheres

Colloidal crystals with a diamond and pyrochlore structure display wide photonic band gaps at low refractive index contrasts. However, these low-coordinated and open structures are notoriously difficult to self-assemble from colloids interacting with simple pair interactions. To circumvent these problems, one can self-assemble both structures in a closely packed MgCu Laves phase from a binary mixture of colloidal spheres and then selectively remove one of the sublattices. Although Laves phases have been proven to be stable in a binary hard-sphere system, they have never been observed to spontaneously crystallize in such a fluid mixture in simulations nor in experiments of micron-sized hard spheres due to slow dynamics. Here we demonstrate, using computer simulations, that softness in the interparticle potential suppresses the degree of fivefold symmetry in the binary fluid phase and enhances crystallization of Laves phases in nearly hard spheres.