Responsive Interfacial Assemblies Based on Charge‐Transfer Interactions

Charge transfer (CT) interactions have been widely used to construct supramolecular systems, such as functional nanostructures and gels. However, to date, there is no report on the generation of CT complexes at the liquid-liquid interface. Here, by using an electron-deficient acceptor dissolved in water and an electron-rich donor dissolved in oil, we present the in-situ formation and assembly of CT complex surfactants (CTCSs) at the oil-water interface. With time, CTCSs can assemble into higher ordered nanofilms with exceptional mechanical properties, allowing the stabilization of liquids and, offering the possibility to structure liquids into nonequilibrium shapes. Moreover, due to the redox-responsiveness of the electron-deficient acceptor, the association and dissociation of CTCSs can be reversibly manipulated in a redox process, leading to the switchable assembly and disassembly of the resultant constructs.