In silico design of photoresponsive peptide-based hydrogel with controllable structural and rheological properties

Abstract

Self-assembly of peptide-based molecules has emerged as an appealing strategy for developing intelligent nanomaterials with favorable biocompatibility and biodegradability. However, how to design the self-assembly systems with controllable and reversible rheological property is still challenging. In this study, coarse-grained molecular dynamics simulation is employed to develop peptides-based hydrogel with photo-stimuli-responsive capability. Our simulations demonstrate that the bisazoFA molecule, generated by grafting azobenzene (azo) moiety to the phenylalanyl-alanine (FA), can self-assemble into twisted networks. With the introduction of diphenylalanine (FF), the micelles undergo morphological transitions from networks to lamellar structures. By manipulating the UV–vis light irradiation, the wormlike structure with orderly-arranged hydrophobic interior is achieved. The distinct self-assembled structures can induce varied viscosity. Furthermore, the mechanisms underlying the self-assembly/stimuli-response processes are examined in the perspective from energy and structure. Specifically, the varied structural/rheological property of systems are driven by the stacking modes between bisazoFA and spatial arrangement of FF molecules. This bottom-up in silico design not only offers a feasible strategy to develop hydrogel with controllable and reversible rheological property, but also enrich our understanding of the self-assembly of peptide-based molecules.