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

Evolvability of chemical replicator systems requires non-equilibrium energy dissipation, effective decomposition pathways and transfer of structural information in the autocatalytic cycles. We engineered a chemical network with peptidic foldamer components, with UV light-fuelled dissipative sequence-dependent replication and replicator decomposition. The light-harvesting formation-recombination cycle of thiyl radicals was coupled with the molecular recognition steps in the replication cycles. Thiyl radical-mediated chain reaction was responsible for the replicator breakdown. The competing and kinetically asymmetric replication and decomposition processes led to light intensity-dependent selection, which differs from the equilibrium composition. The results contribute to the development of chemically evolvable dissipative replicator systems.