Liquids lack the spatial order required for advanced functionality. Interfacial assemblies of colloids, however, can be used to shape liquids into complex, 3D objects, simultaneously forming 2D layers with novel magnetic, plasmonic, or structural properties. Fully exploiting all-liquid systems that are structured by their interfaces would create a new class of biomimetic, reconfigurable, and responsive materials. Here, printed constructs of water in oil are presented. Both form and function are given to the system by the assembly and jamming of nanoparticle surfactants, formed from the interfacial interaction of nanoparticles and amphiphilic polymers that bear complementary functional groups. These yield dissipative constructs that exhibit a compartmentalized response to chemical cues. Potential applications include biphasic reaction vessels, liquid electronics, novel media for the encapsulation of cells and active matter, and dynamic constructs that both alter, and are altered by, their external environment.

Electrostatic interactions between nanoparticles (NPs) and functionalized ligands lead to the formation of NP surfactants (NPSs) that assemble at the water-oil interface and form jammed structures. To understand the interfacial behavior of NPSs, it is necessary to understand the mechanism by which the NPSs attach to the interface and how this attachment depends on the areal coverage of the interface. Through direct observation with high spatial and temporal resolution, using laser scanning confocal microscopy and in situ atomic force microscopy (AFM), we observe that early-stage attachment of NPs to the interface is diffusion limited and with increasing areal density of the NPSs, further attachment requires cooperative displacement of the previously assembled NPSs both laterally and vertically. The unprecedented detail provided by in situ AFM reveals the complex mechanism of attachment and the deeply nonequilibrium nature of the assembly.

We report on numerical simulations of a monolayer of charge-stabilized colloids driven over a substrate potential by an external dc force acting along a symmetry axis of the monolayer. Using overdamped Langevin dynamics, we studied the sliding transition for various inter-particle interaction strengths as a function of the driving force. For weak interactions, the diffusion of individual defects is responsible for the motion of the monolayer. As the interaction strength is increased, sliding is induced by distinct density compression and decompression zones. For very strong interactions, a type of stick-slip mechanism emerges, in which the sliding of the monolayer is mediated by the propagation of collective distortion waves. Our predictions can be tested experimentally with two-dimensional arrangements of colloidal particles exposed to periodic light fields and our work shows that the inter-particle interaction strength tunes the degree of correlation in the sliding mechanism adopted by a monolayer driven over a commensurate substrate.