Non-equilibrium Spatiotemporal Patterns of Charge-transfer Supramolecular Assembly

Spatiotemporal organization and patterns are a hallmark of life, exemplified by the spatiotemporal organization of microtubules during cell division. The emerging interest in lifelike materials has motivated a paradigm shift from equilibrium to non-equilibrium supramolecular assemblies. However, the next challenge is to program the self-assembly process to drive its spatiotemporal patterns, thereby controlling its structure and properties across both space and time. In this study, we integrate a redox-based dissipative self-assembly with a reaction-diffusion system to generate spatiotemporal patterns of supramolecular assemblies. Our findings reveal that the components of dissipative self-assemblies critically influence the emergent patterns, which can be precisely directed by external perturbations, such as the addition of oxidizing agent. This approach offers a versatile strategy for manipulating a broad range of monomers to generate diverse spatiotemporal patterns of supramolecular architectures of different shapes and material properties. This enables the investigation of their collective behaviour across various length scales. This strategy not only advances our understanding to build complex non-equilibrium supramolecular architectures but also paves the way for development of lifelike materials spatiotemporally tunable properties.