“Aging” of the structure of crystals of hard colloidal spheres

We study the development of the structure of crystals of colloidal hard spheres in time when gravity effects are minimal and polydispersity is small (<3%). The initial stacking of the close-packed hexagonal layers that make up the crystals is varied by applying various types of shear stress during nucleation of the crystals. The experimental powder diffraction patterns are consistent with a fraction of a faulted-twinned face-centered cubic (fcc) structure that grows at the expense of randomly stacked crystallites. If a faulted-twinned fcc structure is generated initially, no change is found over a considerable time. The present observations rule out the possibility that a randomly stacked structure is the equilibrium structure of colloidal crystals of (nearly) hard spheres, and point to the thermodynamic or kinetic stability of faulted-twinned fcc crystals in these systems.