Anisotropic Nanocrystal Shape and Ligand Design for Co-Assembly*

In recent years, there has been increasing emphasis on using anisotropic building blocks to create metamaterials with emergent properties. However, unlike single shaped particle or co-assembly of binary spheres, there have been few reports of co-assembly of two anisotropic NCs that do not rely on explicit usage of shape complementarity. Here, we present a theory-driven approach for designing the co-assembly of cubes and triangular prisms. Specifically, we employ theory to select for a combination of design parameters that exhibit a broad co-assembly regime. Key to this process is the idea of removing geometrical incompatibilities between building blocks via tuning the shape of the ligand shell coating individual NCs. Direct applications of our design parameters are then shown to produce the predicted co-assembly behavior in experiments. This work sheds light on the cooperative role of both shape and ligand shell in directing the organization of multi-shaped objects.