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Peptide co-assembly is of interest for the development of functional supramolecular biomaterials. Herein, computational simulations were combined with experimental validation to aid the design and understanding of cooperative co-assembly of a structure-forming tripeptide (FFD) and a functional copper-binding tripeptide (GHK) leading to hydrogel formation in response to complexation with copper ions.

We demonstrate an in situ ultrasonic approach to influence self-assembly across the supramolecular to micron length scales, showing enhancement of supramolecular interactions, chirality and orientation, which depends on the peptide sequence and solvent environment. This is the first successful demonstration of using oscillating pressure waves to generate anisotropic organo- and hydrogels consisting of oriented tripeptides structures.

Supramolecular structures were produced by in situ enzymatic condensation of Fmoc-Phe-(4-X), where X denotes electron withdrawing or donating groups, with Phe-NH2. The relative contribution of π-stacking and H-bonding interactions can be regulated by the nature of X, resulting in tuneable nanoscale morphologies.