Light-Fueled Primitive Replication and Selection in Biomimetic Chemical Systems

The concept of chemically evolvable replicators is centralto abiogenesis.Chemical evolvability requires three essential components: energy-harvestingmechanisms for nonequilibrium dissipation, kinetically asymmetricreplication and decomposition pathways, and structure-dependent selectivetemplating in the autocatalytic cycles. We observed a UVA light-fueledchemical system displaying sequence-dependent replication and replicatordecomposition. The system was constructed with primitive peptidicfoldamer components. The photocatalytic formation-recombinationcycle of thiyl radicals was coupled with the molecular recognitionsteps in the replication cycles. Thiyl radical-mediated chain reactionwas responsible for the replicator death mechanism. The competingand kinetically asymmetric replication and decomposition processesled to light intensity-dependent selection far from equilibrium. Here,we show that this system can dynamically adapt to energy influx andseeding. The results highlight that mimicking chemical evolution isfeasible with primitive building blocks and simple chemical reactions

Light-fuelled primitive replication and selection in evolvable biomimetic chemical networks

The concept of chemically evolvable replicators is central to abiogenesis. Evolvability requires three essential components: energy harvesting mechanisms for non-equilibrium dissipation, kinetically asymmetric decomposition pathways, and transfer of structural information in the autocatalytic cycles. We observed a UVA light-fuelled chemical network displaying sequence-dependent replication and replicator decomposition. The system was constructed with primitive peptidic foldamer components. The photocatalytic 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 death mechanism. The competing and kinetically asymmetric replication and decomposition processes led to light intensity-dependent selection far from equilibrium. Here we show that this system can dynamically adapt to the level of energy influx and seeding. The results highlight the feasibility of the complex phenomenon of chemical evolvability with primitive building blocks and simple chemical reactions