Lithographically defined microwell templates are used to study DNA-guided colloidal crystal assembly parameters, including superlattice position, habit orientation, and size, in an effort to increase our understanding of the crystallization process. In addition to enabling the synthesis of arrays of individual superlattices in arbitrary predefined patterns, the technique allows one to study the growth pathways of the crystals via scanning electron microscopy. Importantly, a Volmer-Weber (VM) (island formation)-like growth mode is identified, which has been reproduced via simulations. Notably, both experiment and simulation reveal that the crystallites merge and reorient within the microwells that defined the crystal growth to form single-crystalline structures, an observation not common for VM pathways. The control afforded by this platform will facilitate efforts in constructing metamaterials from colloidal crystals as well as their integration into optical devices and applications.
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