Multi‐Responsive Peptide‐Based Ultrathin Nanosheets Prepared by a Horizontal Monolayer Assembly

Abstract

AbstractIn this study, peptide‐based self‐assembled nanosheets with a thickness of approximately 1 nm were prepared using a hierarchical covalent physical fabrication strategy. The covalent alternating polymerization of helical peptide E3 with an azobenzene (AZO) structure yielded copolymers CoP(E3‐AZO), which physically self‐assembled into ultrathin nanosheets in an unanticipated two‐dimensional horizontal monolayer arrangement. This special monolayer arrangement enabled the thickness of the nanosheets to be equal to the cross‐sectional diameter of a single linear copolymer, which is a rare phenomenon. Molecular dynamics simulations suggested that the synergistic effect of multiple molecular interactions drives the self‐assembly of CoP(E3‐AZO) into nanosheets and that various methods, including phototreatment, pH adjustment, the addition of additives, and introduction of cosolvents, can alter the molecular interactions and modulate the self‐assembly of CoP(E3‐AZO), yielding diverse nanostructures. Remarkably, the ultrathin nanosheets selectively inhibited cancer cells at certain concentrations.