Light-Fuelled Dissipative Replication and Selection in Adaptive Biomimetic Chemical Networks

Abstract

<p>Evolvability of the chemical replicator systems requires non-equilibrium energy dissipation, effective death pathways and transfer of structural information in the autocatalytic cycles. We engineered a chemical network with peptidic foldamer components, where UV light fuelled dissipative sequence-dependent exponential replication and replicator decomposition. The light-harvesting formation-recombination cycle of the thiyl radicals was coupled with the molecular recognition steps in the replication cycles. Thiyl radical-mediated chain reaction was responsible for the replicator death. The competing and kinetically asymmetric replication and decomposition processes led to light intensity-dependent selection and competitive exclusion. Dynamic adaptation to the energy input and the selection factor maximised the dissipation rate in the regime of exponential growth. The results contribute to the development of chemically evolvable replicator systems.</p>