Position‐ and Orientation‐Controlled Growth of Wulff‐Shaped Colloidal Crystals Engineered with DNA

Abstract Colloidal crystals have emerged as promising candidates for building optical microdevices. Techniques now exist for synthesizing them with control over their nanoscale features (e.g., particle compositions, sizes, shapes, and lattice parameters and symmetry); however, the ability to tune macroscale structural features, such as the relative positions of crystals to one another and lattice orientations, has yet to be realized. Here, inspiration is drawn from epitaxial growth strategies in atomic crystallization, and patterned substrates are prepared that, when used in conjunction with DNA‐mediated nanoparticle crystallization, allow for control over individual Wulff‐shaped crystal growth, location, and orientation. In addition, the approach allows exquisite control over the patterned substrate/crystal lattice mismatch, something not yet realized for any epitaxy process. This level of structural control is a significant step toward realizing complex, integrated devices with colloidal crystal components, and this approach provides a model system for further exploration in epitaxy systems.