Architeturally encoding adhesion in brush polymer networks

The diverse viscoelastic behavior of pressure sensitive adhesives (PSAs) enables their ubiquitous use in devices from office supplies to biomedical devices. Current approaches to meet these wide-ranging viscoelastic properties rely on exploratory mixing of polymers and loose additives, such as tackifiers and plasticizers. This approach results in adhesives prone to property variation over time and imprecision due to chemical migration. We have developed an alternative, additive-free PSA design platform empowering topological control over adhesive performance without altering chemical composition. By leveraging brush polymer architecture, we can concurrently regulate elastic (softness and firmness) and viscoelastic (characteristic relaxation times) properties, which allows encoding work of adhesion within five orders of magnitude. This platform bridges the gap between nanoscale molecular structure and macroscale adhesion through relaxation dynamics as a pivotal step toward universal design of both UV-cured and hot-melt PSAs.