Understanding the forces acting in self-assembly and the implications for constructing three-dimensional (3D) supercrystals

The assembly of nanocrystals into ordered structures called supercrystals or superstructures has become a pivotal frontier owing to numerous useful applications such as correlating the arrangements of atoms in macroscopic crystals and tuning the collective properties to meet the demands of various applications. In this article, recent progress in the preparation of three-dimensional superlattices of nanocrystals is outlined, with a particular emphasis on the driving forces and evolutionary routes beyond orderly assembly. First, the leading or repulsive forces that internally and externally govern the formation of three-dimensional supercrystals are systematically identified and discussed with respect to their origins and functions in three-dimensional self-organization. Then a synoptic introduction of commonly applied means of nanocrystal self-assembly based on growth scenarios such as droplet evaporation and a liquid/liquid interface is presented with specific cases and detailed analyses. Finally, the existing challenges and prospects for this field are briefly highlighted.