Light-Controlled Nucleation and Shaping of Self-Assembling Nanocomposites

Abstract

Controlling self-assembly of nanocomposites is a fundamental challenge with exciting implications for next-generation advanced functional materials. Precursors for composites can be generated photochemically, but limited insight in the underlying processes has hindered precise hands-on guidance. In this study, light-controlled nucleation and growth is demonstrated for self-assembling composites according to precise user-defined designs. Carbonate is generated photochemically with UV light to steer the precipitation of nanocomposites of barium carbonate nanocrystals and amorphous silica (BaCO₃ /SiO₂ ). Using a custom-built optical setup, the self-assembly process is controlled by optimizing the photogeneration, diffusion, reaction, and precipitation of the carbonate species, using the radius and intensity of the UV-light irradiated area and reaction temperature. Exploiting this control, nucleation is induced and the contours and individual features of the growing composite are sculpted according to micrometer-defined light patterns. Moreover, moving light patterns are exploited to create a constant carbonate concentration at the growth front to draw lines of nanocomposites with constant width over millimeters with micrometer precision. Light-directed generation of local gradients opens previously unimaginable opportunities for guiding self-assembly into functional materials.

Keywords: crystallization; nanocomposites; nucleation; patterning; photodecarboxylation; self-assembly.