Evaporation-Driven, Template-Assisted Nanocrystal Assembly (ETNA): A Novel Approach to Fabrication of Functional Nanocrystal Solids

Synthesis of nanocrystals is one of the most rapidly advancing areas of nanoscience, and today nanocrystals can be produced with impressive control over their composition, size, shape, polydispersity, and surface chemistry. As such, they are ideal building blocks for fabricating hierarchical architectures with tailorable functionality on every level of the hierarchy. Here an evaporation-driven, template-assisted nanocrystal assembly (ETNA) technique is developed, providing a novel and general approach to fabricating freestanding, 3D, functional architectures using diverse combinations of colloidal nanocrystal species and porous templates of arbitrary geometry. Colloidal PbS (photoluminescent) and CoFe2O4 (superparamagnetic) nanocrystals are template-assembled to fabricate freestanding nanorods and inverse opals, which retain the size-dependent properties of their constituent building blocks while replicating the geometry and preserving the functionality of the templates. Further multifunctionality is demonstrated through mixed-nanocrystal architectures which exhibit the aggregate functionality of their building blocks. ii