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Supramolecular self-assembly at the solid-solid interface enables thedeposition and monolayer formation of insoluble organic semiconductors underambient conditions. The underlying process, termed as the Organic Solid-SolidWetting Deposition (OSWD), generates two-dimensional adsorbates directly fromdispersed three-dimensional organic crystals. This straightforward process hasimportant implications in various fields of research and technology, such as inthe domains of low-dimensional crystal engineering, the chemical doping andband-gap engineering of graphene, and in the area of field-effect transistorfabrication. However, till date, lack of an in-depth understanding of thephysico-chemical basis of the OSWD prevented the identification of importantparameters, essential to achieve a better control of the growth of monolayersand supramolecular assemblies with defined structures, sizes, and coverageareas. Here we propose a detailed model for the OSWD, derived from experimentaland theoretical results that have been acquired by using the organicsemiconductor quinacridone as an example system. The model reveals the vitalrole of the zeta potential and includes Casimir-like fluctuation-induced forcesand the effect of dewetting in hydrophobic nano-confinements. Based on ourresults, the OSWD of insoluble organic molecules can hence be applied toenvironmental friendly and low-cost dispersing agents, such as water. Inaddition, the model substantially enhances the ability to control the OSWD interms of adsorbate structure and substrate coverage.

journal of the american chemical society

Revealing the Physico-Chemical Basis of Organic Solid-Solid Wetting  Deposition: Casimir-Like Forces, Hydrophobic Collapse, and the Role of the  Zeta Potential