Autonomous Self-Recognition and Healing in Multilayer Soft Electronics Using Orthogonal Dynamic Polymers

Can we design multilayer electronics that can spontaneously heal themselves after damage? Having this functionality would protect electronic devices from traditional “wear and tear” damages, improving product lifetime, as well as from intense mechanical damage that would otherwise cause product failure. Compared to the self-healing of a single polymer composite, the self-healing of complex, multilayered devices requires simultaneous healing between multiple layers with distinct functions. Currently, this is achieved by manual alignment of the layers after damage. In this work, we demonstrate a multilayer electronic device that can autonomously re-align and heal after damage using orthogonal dynamic polymers. We show that dynamic polymers with controlled orthogonality exhibit significant and predictable variations in interfacial healing dynamics, allowing for autonomous self-recognition. When misaligned after damage, these multilayer structures possess surface tension gradients that drive directional chain diffusion to enable realignment. We experimentally characterize the interface between different orthogonal dynamic polymers and compare our results to coarse-grained molecular dynamics simulations and self-consistent field theory. Using these polymers, we prepare conductive and high dielectric composites to create thin film capacitors that can autonomously heal with thicknesses below 100 microns. We also demonstrate macroscopic self-assembly of these polymers after damage using magnetic composites. This work provides the first proof-of-concept demonstration of autonomously self-healing multilayered devices and opens a pathway for future autonomous self-assembly in multi-component dynamic materials via pattern recognition.