Organic Chemistry

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

Abstract

The concept of chemically evolvable replicators is central to abiogenesis. Evolvability requires three essential components: energy harvesting mechanisms for non-equilibrium dissipation, effective decomposition pathways and transfer of structural information in the autocatalytic cycles. We observed a UVA light-fuelled dissipative 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.

Version notes

1. Autocatalysis has been substantiated in the time-domain via seeding experiments. 2. Dynamic energy influx-dependent adaptivity has been proved. 3. The ability of the disulfide bond to absorb UVA light has been shown. UVA-dependent replicator synthesis and break down processes have been independently supported. 4. All figures have been updated, and new figures have been added.

Content

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