Regular H-Bonding-Containing Polymers with Stretchability up to 100% External Strain for Self-Healable Plastic Transistors

Intrinsically stretchable, electroactive materials featuring self-healing abilities will allow for a variety of next-generation stretchable electronics. Here, we synthesize diketopyrrolopyrrole-based alternating copolymers with urethane-containing side chains, that is, PDPPurethane copolymers, and use them as active layers in intrinsically stretchable and self-healable plastic transistors. The long-branched urethane side chains possessing moderate H-bonding strength enable sufficient solubility and excellent dynamic bonding, facilitating the stress dissipation under mechanical deformation. PDPPurethane thin films exhibit outstanding stretchability up to 100% external strain without degradation of electrical performance in the organic transistor platform. They also feature self-healing properties with the healing of cracks and the recovery of electrical properties after treatment. The structure-property relationships of PDPPurethane thin films under strain have been thoroughly investigated using a variety of characterization methods. Our results demonstrate a viable approach for the development of stretchable and self-healable plastic electronics using stretchable, semiconducting copolymers obtained via side chain engineering.