Diversification of self-replicating molecules

Abstract

How new species emerge in nature is still incompletely understood and difficult to study directly. Self-replicating molecules provide a simple model that allows us to capture the fundamental processes that occur in species formation. We have been able to monitor in real time and at a molecular level the diversification of self-replicating molecules into two distinct sets that compete for two different building blocks ('food') and so capture an important aspect of the process by which species may arise. The results show that the second replicator set is a descendant of the first and that both sets are kinetic products that oppose the thermodynamic preference of the system. The sets occupy related but complementary food niches. As diversification into sets takes place on the timescale of weeks and can be investigated at the molecular level, this work opens up new opportunities for experimentally investigating the process through which species arise both in real time and with enhanced detail.

Controlling supramolecular polymerization through multicomponent self‐assembly

“…This strategy is an elegant approach for kinetically controlled product formation in supramolecular materials, via the combination of reversible covalent bonds and noncovalent interactions. [420][421][422] The strategies that have been highlighted so far, demonstrate the impact of and potential for kinetic control in supramolecular polymeric assemblies of controlled length and architecture, driven by epitaxial crystallization of blocked copolymers, 31,350 or by the combination of reversible covalent bonds and noncovalent interactions in macrocyclic unimers. 10,[420][421][422] Alternatively, the manipulation of self-assembly pathways was very recently achieved via the rational design of selfassembling small molecular weight building blocks by three different groups.…”

“…[420][421][422] The strategies that have been highlighted so far, demonstrate the impact of and potential for kinetic control in supramolecular polymeric assemblies of controlled length and architecture, driven by epitaxial crystallization of blocked copolymers, 31,350 or by the combination of reversible covalent bonds and noncovalent interactions in macrocyclic unimers. 10,[420][421][422] Alternatively, the manipulation of self-assembly pathways was very recently achieved via the rational design of selfassembling small molecular weight building blocks by three different groups. [423][424][425] Sugiyasu, Takeuchi and coworkers have been able to show that seed-induced growth in combination with a competing off-pathway aggregation leads to a "living" supramolecular polymerization of a Zn(II)-porphyrin dye ZnP4 in apolar methylcyclohexan (MCH).…”

A Versatile Approach to Noncanonical, Dynamic Covalent Single- and Multi-Loop Peptide Macrocycles for Enhancing Antimicrobial Activity

“…25 Because these previously studied peptides were not specifically designed for use as antimicrobial agents, their assemblies displayed modest activities. Still, this discovery prompted us to test the effect of DC assembly on a naturally occurring CAMP sequence, buforin II.…”

“…DC functionalities have been incorporated into peptide oligomers leading to interesting applications, such as templated assembly of fluorophores, 21 α -helix formation, 22 macrocyclization, 23 peptide–peptide ligation, 24 self-replication, 25 formation of catenanes, 26 and formation of β -hairpin mimics. 26 Very recently, our group reported the facile incorporation of aldehyde and hydrazide functionalities using solid-phase copper-catalyzed azide–alkyne cycloaddition (SP-CuAAC) “click” reactions (Scheme 1).…”

Synergistic Assembly of Covalent and Supramolecular Polymers

“…[ 8 ] Otto and co-workers accurately analyzed the process of self-replicated molecules. [ 9 ] Overall, smart integration of covalent and noncovalent compartments is undoubtedly a novel breakthrough.…”