Mesoscale Polymer Ribbons as Hierarchical Building Blocks

Mesoscale polymer ribbons (MSPs) are unique high aspect ratio structures formed by controlled evaporative self-assembly. Due to their 3D helical conformation upon release in solution and their sensitivity to environmental changes, MSPs offer a novel system of building blocks to construct hierarchical assemblies. Control of synthetic materials from building blocks spanning hundreds of nanometers to tens of microns presents an opportunity to impart anisotropy and enhanced mechanical performance, though current methods of mesoscale control are limited. We harness interfacial forces to control the assembly of long, flexible MSPs in aqueous media.Our data quantifies the changes in inter-ribbon entanglement and aggregation as a function of ion concentration in aqueous environments and at the perfluorodecalin-water interface. Using light microscopy, we study the evolution of ribbon conformation and inter-ribbon interactions as a function of time. This work elucidates the interfacial interactions and assembly phenomena in multi-ribbon mesoscale structures, underpinning the MSP as an emerging platform in soft, bioinspired hierarchical assemblies.