Templated self-organization of polymer-tethered gold nanoparticles into freestanding superlattices at the liquid–air interface

Programmable organization of uniform organic/inorganic functional building blocks into large-scale ordered superlattices has attracted considerable attention since the bottom-up self-organization strategy opens up a robust and universal route for designing novel and multifunctional materials with advanced applications in memory storage devices, catalysis, photonic crystals, and biotherapy. Despite making great efforts in the construction of superlattice materials, there still remains a challenge in the preparation of organic/inorganic hybrid superlattices with tunable dimensions and exotic configurations. Here, we report the spontaneous self-organization of polystyrene-tethered gold nanoparticles (AuNPs@PS) into freestanding organic/inorganic hybrid superlattices templated at the diethylene glycol-air interface. The resulting multilayer 3D superlattices exhibit hexagonally honeycomb and periodically tetrahedral lattices after the evaporation of AuNPs@PS building blocks at the liquid-air interface. Notably, a particular Moiré pattern originating from the twisted stacking of the adjacent layers is observed when the twist angle is 30°, leading to the exquisite quasi-crystalline packing with 12-fold rotational symmetry. In addition, the interparticle distance and gap within the 2D superlattice can be precisely regulated by adjusting the length of polymer segments, thereby generating distinctive 3D graphene-skeleton configurations in the freestanding superlattice. This finding presents a highly efficient and versatile way to artificially produce multifunctional organic/inorganic hybrid superlattice materials with adjustable dimensions and internal configurations.