A Comprehensive Landscape for Fibril Association Behaviors Encoded Synergistically by Saccharides and Peptides

Nature provides us a panorama of fibrils with tremendous structural polymorphism from molecular building blocks to hierarchical association behaviors. Despite recent achievements in creating artificial systems with individual building blocks through self-assembly, molecularly encoding the relationship from model building blocks to fibril association, resulting in controlled macroscopic properties, has remained an elusive goal. In this paper, by employing a designed set of glycopeptide building blocks and combining experimental and computational tools, we report a library of controlled fibril polymorphism with elucidation from molecular packing to fibril association and the related macroscopic properties. The growth of the fibril either axially or radially with right- or left-handed twisting is determined by the subtle trade-off of oligosaccharide and oligopeptide components. Meanwhile, visible evidence for the association process of double-strand fibrils has been experimentally and theoretically proposed. Finally the fibril polymorphs demonstrated significant different macroscopic properties on hydrogel formation and cellular migration control.

Automated summary

This study reports a controlled fibril polymorphism library generated by designed glycopeptide building blocks and experimental and computational tools. The growth of fibrils, either axially or radially, is determined by a subtle balance of oligosaccharide and oligopeptide components, leading to right- or left-handed twisting structure. The study also provides visible evidence for the association process of double-strand fibrils, and demonstrates significant differences in macroscopic properties of fibril polymorphs on hydrogel formation and cellular migration control.