Minimal Catalytic Assemblies Can Oscillate Utilizing Feedback Loops

Abstract The light-dark cycles created from Earth’s rotation helped in the emergence of extant cellular life that integrates evolved oscillatory networks to control circadian rhythms, cell division, metabolism and so forth. Out of equilibrium networks of organic chemical reactions with dynamic self-assembled structures that emerged from Darwin’s nutrient-rich warm pond played crucial roles in spawning the protolife under a fluctuating environmental condition. Dynamic chemical networks with simple chemicals that can display emergent network dynamics can contribute to our understanding of complex behaviours from simple organic reactions. Here we have designed a single amino acid-based system that could self-assemble and oscillate under non-equilibrium conditions, importantly in the absence of evolved biocatalysts. The two-component based building block exploits pH driven non-covalent assembly and time-delayed accelerated catalysis from self-assembled state to install orthogonal feedback loops with a single batch of reactants. Modifications of these autonomous systems from purely synthetic molecules can enable the design of exceptional life-like materials and evolving systems with acute spatiotemporal control of properties.