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

31 August 2021, Version 2
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

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.

Keywords

dissipative adaptation
replication
chemical evolution
foldamer
disulphide
systems chemistry
dissipative assembly
non-equilibrium thermodynamics

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