Local Self-Assembly of Dissipative Structures Sustained by Substrate Diffusion.
Haridas KarLorenzo GoldinDiego FrezzatoLeonard J PrinsPublished in: Angewandte Chemie (International ed. in English) (2024)
The coupling between energy-consuming molecular processes and the macroscopic dimension plays an important role in nature and in the development of active matter. Here, we study the temporal evolution of a macroscopic system upon the local activation of a dissipative self-assembly process. Injection of surfactant molecules in a substrate-containing hydrogel results in the local substrate-templated formation of assemblies, which are catalysts for the conversion of substrate into waste. We show that the system develops into a macroscopic (pseudo-)non-equilibrium steady state (NESS) characterized by the local presence of energy-dissipating assemblies and persistent substrate and waste concentration gradients. For elevated substrate concentrations, this state can be maintained for more than 4 days. The studies reveal an interdependence between the dissipative assemblies and the concentration gradients: catalytic activity by the assemblies results in sustained concentration gradients and, vice versa, continuous diffusion of substrate to the assemblies stabilizes their size. The possibility to activate dissipative processes with spatial control and create long lasting non-equilibrium steady states enables dissipative structures to be studied in the space-time domain, which is of relevance for understanding biological systems and for the development of active matter.