Reconfigurable Chiral Self-Assembly of Peptides through Control of Terminal Charges

Self-assembly of chiral nanostructures is of considerable interest, since the ability to control the chirality of these structures has direct ramifications in biology and materials science. A new approach to design chiral nanostructures from self-assembly of N-(9-fluorenylmethoxycarbonyl)-protected phenylalanine-tryptophan-lysine tripeptides is reported. The terminal charges can induce helical twisting of the assembled β-sheets, enabling the formation of well-defined chiral nanostructures. The degree and direction of twisting in the β-sheets can be precisely tailored through in situ pH and temperature modulations. This enables the assembly of reconfigurable chiral nanomaterials with easily adjustable size and handedness. These results offer new insight into the mechanism of helical twist formation, which may enable the precise assembly of highly dynamical materials with potential applications in biomedicine, chiroptics, and chiral sensing.