Supramolecular Self‐Assembly Initiated by Solid–Solid Wetting

We present a preparation method for self‐assembled supra‐molecular monolayers of unsubstituted organic semiconductors and pigments on a solid substrate, applicable under ambient conditions. The deposition is based on a solid–solid wetting phenomenon, whereas the subsequent layer growth proceeds according to standard models. Molecular adsorption results from direct contact of the compound in a nanocrystalline state with the solid surface. Based on complementary force field calculations, we propose that molecules disintegrate from the crystalline state and adsorb on the surface because of a gain in binding energy. The preparation method is exemplified by means of a linear hydrogen‐bonded system, namely quinacridone (QAC) on graphite. In addition, the chosen system allows us to actively guide the self‐assembly after deliberate removal of molecules from a predefined area.