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Exponential replication is one of the requirements for molecular-level Darwinian evolution, but is difficult to achieve in synthetic systems. Here, the authors show a peptide-functionalized macrocycle that forms supramolecular fibres with exponential growth when subjected to mild agitation.

Self-replicating molecules provide a simple molecular level system to study the processes occurring in speciation. Now it is shown that in a pool of interconverting macrocycles, constructed from two building blocks, two distinct sets of self-replicating molecules emerge, and that one is a descendant of the other.

A molecular 'walker' can be made to move up and down a molecular 'track' by alternately locking and unlocking the two different types of covalent bonds that join the two components together. By changing the conditions under which one of the bond-forming/bond-breaking processes occurs, a directional bias for walking can be achieved.

It is unclear whether Darwinian principles extend to chemistry and if they can direct chemistry to produce specific products. Now it has been shown that competition between self-replicating molecules can result in the survival of the fittest product or coexistence of a small subset of products, depending on how resources are partitioned between the replicators.

The use of molecules as fuels to achieve function is largely unexplored. Now it has been shown that fuelled dissipative self-assembly can yield transient droplets that release a surfactant, driving the macroscopic transport of these droplets.

By using reversible enzyme reactions involving short peptides, molecular synthesis can be controlled by the self-assembly of the resulting products.

The onset of eco-evolutionary dynamics marks a stepping stone in the transition from chemistry to biology. Now a minimal replicator system showing such dynamics has been developed. The replicators adapt to changes in their environment that they themselves induced through photoredox catalysis.

High- and ultra-performance liquid chromatography are valuable tools for the identification of components in complex mixtures, but these instruments lack sample stirring capabilities. Here the authors design an automated device that enables continuous stirring of samples inside an ultra-performance liquid chromatography system, and can be reproduced and modified using 3D printing technology.

The integration of replication with metabolism represents a key step in the transition of chemistry into biology. Now, it has been shown that a self-replicator can recruit and activate two different photocatalytic cofactors, which then catalyse the synthesis of the precursors for the replicator.

The majority of discrete structures obtained by self-assembly possess high symmetry, and thus low complexity: all subunits relate to their neighbours in a similar manner. Now, the spontaneous formation of complex low-symmetry assemblies produced from a single building block has been demonstrated using a systems chemistry approach. The single building block oligomerizes to form specific homomeric cyclic macromolecules that adopt a folded conformation.

In the development of chemical complexity—and the transition into biology—developing catalytic functionality is essential. Here the authors report the emergence of catalytic activity for two separate reactions (including one demonstrating a positive feedback on replication) in a self-replicating system.

The merging of supramolecular chemistry and systems chemistry is beginning to unveil the richness of emerging physicochemical properties attainable by exploiting far-from-equilibrium systems, as this Review explains.

Biomolecular condensates show distinct physicochemical properties that may affect the rate of enzymatic activity and control cellular redox reactions, however, their influence on the other types of chemical reaction remains underexplored. Here, the authors use reactive Martini simulations to probe the non-enzymatic macrocyclization reaction of benzene-1,3-dithiol in the presence of peptide condensates.

Self-replicating systems play a central role in the emergence of life. This Review describes the features that self-replicating systems need to acquire to transition from chemistry to biology and surveys the progress made in theoretical and experimental approaches.