Transferring molecular level changes to bulk properties via tunable self-assembly and hierarchical ordering

Hierarchical self-assembly is an effective means of preparing useful materials. However, control over assembly across length scales is a difficult challenge, often confounded by the perceived need to re-design the molecular building blocks when new material properties are needed. Here, we show that we can treat a simple dipeptide building block as a polyelectrolyte and use polymer physics approaches to explain the self-assembly over a wide concentration range. This allows us to prepare interesting analogues to threads and webs, as well as films that lose order on heating and “noodles” which change dimensions on heating, showing that we can transfer molecular-level changes to bulk properties all from a single building block.