The self-assembly of materials driven by the inherent directionality of the constituent particles is of both practical and fundamental interest because it enables the fabrication of complex and hierarchical structures with tailored functionalities. By employing evaporation assisted self-assembly, we form opal-like structures with micro-sized magnetic superball particles. We study the structure formation of different superball shapes during evaporation of a dispersion droplet with in-situ small angle x-ray scattering with microradian resolution in the absence and presence of an external magnetic field. In the absence of a magnetic field, strong shape-dependent structures form as the water evaporates from the system. Applying a magnetic field to the droplet has a unique effect on the system; strong magnetic fields inhibit the growth of well-ordered assemblies due to the formation of out-of-equilibrium dipolar structures while lower magnetic fields allow particles to rearrange and orient without inhibition. In this work, we show how the superball assembly inside a droplet can be controlled by the magnetic field strength and the superball shape. The tunability of these parameters not only enables the controllable formation of macroscopic colloidal assemblies but also opens up possibilities for the development of functional materials with tailored properties on a macro-scale.@en

Understanding the relationship between colloidal building block shape and self-assembled material structure is important for the development of novel materials by self-assembly. In this regard, colloidal superballs are unique building blocks because their shape can smoothly transition between spherical and cubic. Assembly of colloidal superballs under spherical confinement results in macroscopic clusters with ordered internal structure. By utilizing Small Angle X-Ray Scattering (SAXS), we probe the internal structure of colloidal superball dispersion droplets during confinement. We observe and identify four distinct drying regimes that arise during compression via evaporating droplets, and we track the development of the assembled macrostructure. As the superballs assemble, we found that they arrange into the predicted paracrystalline, rhombohedral C₁-lattice that varies by the constituent superballs’ shape. This provides insights in the behavior between confinement and particle shape that can be applied in the development of new functional materials.

@en

Oriented attachment of PbSe nanocubes can result in the formation of two-dimensional (2D) superstructures with long-range nanoscale and atomic order. This questions the applicability of classic models in which the superlattice grows by first forming a nucleus, followed by sequential irreversible attachment of nanocrystals, as one misaligned attachment would disrupt the 2D order beyond repair. Here, we demonstrate the formation mechanism of 2D PbSe superstructures with square geometry by using in situ grazing-incidence X-ray scattering (small angle and wide angle), ex situ electron microscopy, and Monte Carlo simulations. We observed nanocrystal adsorption at the liquid/gas interface, followed by the formation of a hexagonal nanocrystal monolayer. The hexagonal geometry transforms gradually through a pseudo-hexagonal phase into a phase with square order, driven by attractive interactions between the {100} planes perpendicular to the liquid substrate, which maximize facet-to-facet overlap. The nanocrystals then attach atomically via a necking process, resulting in 2D square superlattices.

@en

Anodic aluminum oxide has unique and highly attractive properties, including self-ordering of porous structure during anodization. Although anodization regimes leading to formation of highly ordered porous structures had been found experimentally, many aspects of the self-organization mechanism remain unsolved. Here, the detailed in situ small-angle X-ray diffraction study of the self-ordering in porous alumina films is reported. Structure evolution kinetics was deduced by a quantitative analysis of diffraction patterns combined with electron microscopy. The rate of pore ordering is shown to have maximal value at the initial anodization stage and rapidly decreases inversely proportional to t^0.2. Self-organization is shown to occur via growth of domains possessing preferential in-plane orientation and "death" of other domains, similar to Ostwald ripening governed by difference in pore growth rates for domains of different orientations. The process is accompanied by pore death and splitting making a significant impact on anodic oxides utilization in any mass-transport issues. This finding opens a novel approach for growth of highly ordered porous anodic oxide films.

@en