Perovskite Nanocrystal Self-Assemblies in 3D Hollow Templates

Highly ordered nanocrystal (NC) assemblies, namely, superlattices (SLs), have been investigated as materials for optical and optoelectronic devices due to their unique properties based on interactions among neighboring NCs. In particular, lead halide perovskite NC SLs have attracted significant attention owing to their extraordinary optical characteristics of individual NCs and collective emission processes like superfluorescence (SF). So far, the primary method for preparing perovskite NC SLs has been the drying-mediated self-assembly method, in which the colloidal NCs spontaneously assemble into SLs during solvent evaporation. However, this method lacks controllability because NCs form random-sized SLs at random positions on the substrate, rendering NC assemblies in conjunction with device structures, such as photonic waveguides or microcavities, challenging. Here, we demonstrate template-assisted self-assembly to deterministically place perovskite NC SLs and control their geometrical properties. A solution of CsPbBr₃ NCs is drop-casted on a substrate with lithographically defined hollow structures. After solvent evaporation and removal of excess NCs from the substrate surface, NCs remain only in the templates, thereby defining the position and size of these NC assemblies. We performed photoluminescence (PL) measurements on these NC assemblies and observed signatures of SF, similar to those in spontaneously assembled SLs. Our findings are crucial for optical devices that harness embedded perovskite NC assemblies and enable fundamental studies on how these collective effects can be tailored through the SL geometry.