Flow-induced alignment of (100) fcc thin film colloidal crystals

The realization of structural diversity in colloidal crystals obtained by self-assembly techniques remains constrained by thermodynamic considerations and current limits on our ability to alter structure over large scales using imposed fields and confinement. In this work, a convective-based procedure to fabricate multi-layer colloidal crystal films with extensive square-like symmetry is enabled by periodic substrate motion imposed during the continuous assembly. The formation of film-spanning domains of (100) fcc symmetry as a result of added vibration is robust across a range of micron-scale monosized spherical colloidal suspensions (e.g., polystyrene, silica) as well as substrate surface chemistries (e.g., hydrophobic, hydrophilic). The generation of extensive single crystalline (100) fcc domains as large as 15 mm(2) and covering nearly 40% of the colloidal crystalline film is possible by simply tuning coating conditions and multi-layer film thickness. Preferential orientation of the square-packed domains with respect to the direction of deposition is attributed to domain generation based upon a shear-related mechanism. Visualization during assembly gives clues toward the mechanism of this flow-driven self-assembly method.