pH-modulated self-assembly of colloidal nanoparticles in a dual-droplet inkjet printing process

Interfacial self-assembly has been demonstrated as a powerful driving mechanism for creating various nanostructured assemblies. In this work, we employed a dual-droplet printing process and interfacial self-assembly mechanism to produce deposits with controlled assembly structures of colloidal nanoparticles. We hypothesize that pH modulation of the droplet will influence the interfacial self-assembly through the multibody interactions, e.g. particle-particle, particle-interface, and particle-substrate interactions, correspondingly affecting the deposition morphology of the colloidal nanoparticles.

During the dual-droplet printing, a wetting droplet, containing colloidal nanoparticles, was jetted over a supporting droplet that contains water only. pH modulation was carried out to the supporting droplet. The self-assembly of two kinds of functionalized polystyrene (PS) nanoparticles (carboxyl-PS and sulfate-PS) was systematically investigated under various pH conditions.

Depending on the pH level of the supporting droplet, deposits of carboxyl-PS particles ranging from clear ring-like patterns to nearly uniform monolayer depositions have been obtained. On the other hand, the sulfate-PS particles, even at extreme basic and acidic environments, successfully assemble into nearly monolayer depositions. The multibody interactions are discussed. Such findings can be harnessed in manufacturing high-performance optical and electronic devices.