American Chemical Society
ja9b02554_si_001.pdf (1.67 MB)

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

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journal contribution
posted on 2019-04-30, 00:00 authored by Brian J. Cafferty, Albert S. Y. Wong, Sergey N. Semenov, Lee Belding, Samira Gmür, Wilhelm T. S. Huck, George M. Whitesides
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.