Photo-responsive tubular assemblies, also made from synthetic amphiphiles in aqueous media, can encapsulate short nucleotides and control their duplex binding upon external light sources 22. 1D conductive supramolecular polymers, composed of artificial amino acids, can be prepared in situ in aqueous media by coupling a biocatalytic reaction with monomer nucleation and elongation processes 21.

For example, the rheological properties of the cellular matrix have been recently mimicked, even with spatial resolution 17, 18, by hydrogelation of amphiphilic peptide nanotubes inside aqueous microdroplets 19, 20. In addition, new bottom–up strategies are being developed for the artificial reconstruction of different biomimetic tubular and fibrillar materials 14, 15, 16. Recent examples of such synthetic fibrillar biomaterials have demonstrated how these multivalent interactions can be used to transduce the hierarchical self-assembly of molecular entities into the macroscopic forces required to transform the size, shape and functional behaviour of soft matter 4, 13, 14. This hierarchical assembly strongly amplifies the intramolecular and intermolecular non-covalent contacts along the resulting longitudinal assemblies 9, 10, 11, 12. Some of these synthetic materials imitate the hierarchical self-assembly of biological building blocks across orders of magnitude in length, spanning from short nanotubes to microfibrillar networks 7, 8. In particular, synthetic one-dimensional (1D) supramolecular biomaterials have shown great potential for their application in biomedicine and soft nanofabrication 6. To understand and apply the different supramolecular designs found in biomolecular scaffolds, new strategies capitalise on synthetic surrogates that replicate their structure and function 1, 2, 3, 4, 5. These results demonstrate the potential of minimalistic 1D supramolecular polymerisation to modulate the behaviour of individual aqueous entities with their environment and within communities.

The confined connection of suitable dormant precursors triggered a physically autocatalysed chemical reaction that resulted in functional environmental responses such as molecular uptake, fusion and chemical exchange.

Here, we describe the different phenomena that resulted from the chemically triggered supramolecular fibrillation of synthetic peptide amphiphiles inside water microdroplets. Despite amphiphilic self-assembly being significantly studied in the context of aqueous encapsulation and autopoiesis, very little is currently known about the physico-chemical consequences and functional role of 1D supramolecular polymerisation confined in aqueous compartments. One-dimensional (1D) supramolecular polymers are commonly found in natural and synthetic systems to prompt functional responses that capitalise on hierarchical molecular ordering.

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