Lawrence Berkeley National Laboratory

The self-assembly of nanocrystals enables new classes of materials whose properties are controlled by the periodicities of the assembly, as well as by the size, shape and composition of the nanocrystals. While self-assembly of spherical nanoparticles has advanced significantly in the last decade, assembly of rod-shaped nanocrystals has seen limited progress due to the requirement of orientational order. Here, the parameters critically relevant to self-assembly are systematically quantified using a combination of diffraction and theoretical modeling; these highlight the importance of kinetics on orientational order. Through drying-mediated self-assembly we achieve unprecedented control over orientational order (up to 96percent vertically oriented rods on 1cm2 areas) on a wide range of substrates (ITO, PEDOT:PSS, Si3N4). This opens new avenues for nanocrystal-based devices competitive with thin film devices, as problems of granularity can be tackled through crystallographic orientational control over macroscopic areas.