Process Dependent Complexity in Multicomponent Gels

Mixing low molecular weight gelators (LMWGs) can be used to combine favorable properties of the individual components within a multifunctional gel. Such multicomponent systems are complex enough in themselves but the method of combining components is not commonly considered something to influence self‐assembly. Herein, two multicomponent systems comprising of a naphthalene‐based dipeptide hydrogelator and one of two modified naphthalene diimides (NDIs), one of which forms gels, and the other does not, are investigated. These systems are probed, examining the structures formed and their gel properties (when preparing a solution from either a mixed powder of both components or by mixing pre‐formed solutions of each component) using rheology, small angle neutron scattering (SANS), and absorbance spectroscopy. It is found that by altering the method of preparation, it is can either induce self‐sorting or co‐assembly within the fibers formed that underpin the gel network. Self‐sorting and co‐assembled gels can be controlled by the pre‐mixing of components and using the same gelation conditions. The co‐assembled vs. self‐sorted gels have different properties despite using the same molecules and the same gelation method.