Hierarchical organization is a key determinant of functional properties in bulk and thin film materials. For example, the organization of electron–donor and –acceptor groups is critical to electronic material performance. Strategies to rationally design hierarchical structures in bulk and thin film materials are limited, which hinders our understanding of how to improve material properties and device characteristics by manipulating hierarchical organization. Self-assembly of peptides into nanostructures and organization of these assemblies into networks has yielded excellent control over structure and function in some hierarchically organized materials. In order to endow self-assembling peptides with physical properties that are desirable for processing in bulk or into thin films, we employ dendrons to augment the physical properties of peptides. Dendrons are monodisperse and sequence-defined synthetic polymers, which makes them complementary to peptides. A versatile, graft-to strategy has been employed to create structurally perfect peptide-dendron hybrids in which the peptide adopt an α-helical conformation. The solvent compatibility of the hybrids is conveniently tailored through changes in the dendron structure. Assembly of the helical peptide-dendron hybrids into bundles that mimic helix bundle motifs in proteins is programmed through amino acid sequence of the peptide based on existing peptide design rules. Remarkably, the peptide design rules are robust enough that protein-like structures persist in bulk, nanostructured materials. The presentation will discuss the evolution toward rationally designed protein-like structures in abiological environments as a platform for rationally controlling hierarchical organization in bulk, nanostructured materials.

Programmed assembly of helix bundle-forming peptide-dendron hybrids

253rd National Meeting (2017)

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