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Although common in nature, the self-assembly of small molecules atsold-liquid interfaces is difficult to control in artificial systems. The highmobility of dissolved small molecules limits their residence at the interface,typically restricting the self-assembly to systems under confinement or withmobile tethers between the molecules and the surface. Small hydrogen-bondingmolecules can overcome these issues by exploiting group-effect stabilization toachieve non-tethered self-assembly at hydrophobic interfaces. Significantly,the weak molecular interactions with the solid makes it possible to influencethe interfacial hydrogen bond network, potentially creating a wide variety ofsupramolecular structures. Here we investigate the nanoscale details of waterand alcohols mixtures self-assembling at the interface with graphite throughgroup effect. We explore the interplay between inter-molecular and surfaceinteractions by adding small amounts of foreign molecules able to interferewith the hydrogen bond network and systematically varying the length of thealcohol hydrocarbon chain. The resulting supramolecular structures forming atroom temperature are then examined using atomic force microscopy with insightsfrom computer simulations. We show that the group-based self-assembly approachinvestigated here is general and can be reproduced on other substrates such asmolybdenum disulphide and graphene oxide, potentially making it relevant for awide variety of systems.

Self-assembly of small molecules at hydrophobic interfaces using group effect