Robustness, Entrainment, and Hybridization in Dissipative Molecular Networks, and the Origin of Life

How simple chemical reactions self-assembled into complex, robust networks at the origin of life is unknown. This general problem—self-assembly of dissipative molecular networks—is also important in understanding the growth of complexity from simplicity in molecular and biomolecular systems. Here, we describe how heterogeneity in the composition of a small network of oscillatory organic reactions can sustain (rather than stop) these oscillations, when homogeneity in their composition does not. Specifically, multiple reactants in an amide-forming network sustain oscillation when the environment (here, the space velocity) changes, while homogeneous networks—those with fewer reactants—do not. Remarkably, a mixture of two reactants of different structure—neither of which produces oscillations individually—oscillates when combined. These results demonstrate that molecular heterogeneity present in mixtures of reactants can promote rather than suppress complex behaviors.