Two-Stage Assembly of Nanoparticle Superlattices with Multiscale Organization

Self-assembly processes, while promising forenabling the fabrication of complexly organized nanomaterialsfrom nanoparticles, are often limited in creating structures withmultiscale order. These limitations are due to difficulties inpractically realizing the assembly processes required to achievesuch complex organizations. For a long time, a hierarchicalassembly attracted interest as a potentially powerful approach.However, due to the experimental limitations, intermediate-levelstructures are often heterogeneous in composition and structure,which significantly impacts the formation of large-scale organizations. Here, we introduce a two-stage assembly strategy: DNAorigami frames scaffold a coordination of nanoparticles into designed 3D nanoclusters, and then these clusters are assembled intoordered lattices whose types are determined by the clusters'valence. Through modulating the nanocluster architectures andintercluster bindings, we demonstrate the successful formation of complexly organized nanoparticle crystals. The presented two-stageassembly method provides a powerful fabrication strategy for creating nanoparticle superlattices with prescribed unit cells.