(127f) Evaporative Templating for Directing Hierarchical, Multi-Component Nanoparticle Assemblies

Hierarchical organization is becoming increasingly popular in colloidal and nano-scale assembly as a way to systematically control the formation of complex, multi-component materials. However, traditional approaches aimed at hierarchical organization often experience major bottlenecks in synthesis due either to the complexity required in pattern fabrication for directing particle organization or to surface modification techniques required to program directed interactions between building blocks. Here, we present a theoretical framework that aims to bypass such limitations by leveraging the evaporative dynamics of the solvent to drive the organization of multi-component, hierarchical ordering of nanoscale particles. We test our theory via direct comparison with Monte Carlo simulations as well as an experimental system of Au nanoparticles and CdSe/CdS/ZnS core/shell/shell quantum dots, showing excellent agreement across theory, simulations and experiments. These results suggest that evaporation-driven organization can be a powerful tool for the design and fabrication of hierarchical, multi-functional materials.