Nature-Inspired Semiconducting Polymers with Peptide Conjugation Breakers for Intrinsically Stretchable and Self-Healable Transistors

Intrinsically stretchable and self-healable polymer semiconductors have recently been extensively studied for flexible and wearable electronics. However, challenges lie in the scarcity of molecular designs, laborious synthesis, and an incomplete understanding of energy dissipation mechanisms. Nature-inspired peptide conjugation breakers (PCBs) can provide a robust system for expanding the molecular scope systematically due to the structural diversity of peptides concerning steric bulkiness and polarity. In this study, novel intrinsically stretchable and self-healable semiconducting polymers are developed by integrating PCBs into a diketopyrrolopyrrole moiety, and the distinct roles of intermolecular and intramolecular hydrogen bonds in stretchability are investigated. The former mainly disrupts chain packing and results in reduced crystallinity, while the latter restricts the conformational flexibility of the chain. Remarkably, the polymer containing a glycine-based PCB demonstrates a high mobility of 0.12 cm 2 V –1 s –1 with good cyclic durability and a crack-onset strain exceeding 100%. Mobility remains stable even at 100% strain in both rigid and fully stretchable transistors with self-healing characteristics. These results, for the first time, underscore the usefulness of nature-inspired moieties in stretchable and self-healable electronics and provide a molecular design strategy that balances intermolecular and intramolecular hydrogen bonds, thereby yielding desirable electrical and mechanical properties.