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Self-assembly has proven to be a powerful tool for functional, smart materials such as hydrogels derived from low molecular weight compounds. However, the targeted design of functional gelators remains difficult. Here, we present a set of four Y-shaped aromatic amide tetramers with varying functionalities able to undergo different non-covalent interactions. These compounds were explored towards their self-assembly behavior and hydrogel formation by experimental methods such as UV-vis spectroscopy, rheology, small angle X-ray scattering (SAXS), scanning/transmission electron, and atomic force microscopy. Additionally, we investigated the main mechanisms behind oligomer aggregation and the structure of the resulting supramolecular chains through full atomistic molecular dynamics simulations.

The influence of substituents on gelation and stacking order of oligoaramid – based supramolecular networks