Intrinsically Stretchable Polymer Semiconductor with Regional Conjugation for Stretchable Electronics

The development of intrinsically stretchable polymer semiconductor holds substantial promise in the field of wearable electronics. However, charge transport mobility is typically compromised in existing stretchable semiconductors to achieve the desired stretchability. Herein, a novel “regional conjugation” strategy is proposed to design an intrinsically stretchable polymer semiconductor oligo‐diketopyrrolopyrrole‐thieno[3,2‐b]thiophene (DPPTT)–urethane, in which oligo‐DPPTT conjugated units and alkyl urethane nonconjugated units are introduced. The regional conjugation of oligo‐DPPTT in the polymer backbone endows DPPTT–urethane with good molecular packing, leading to a high mobility of up to 1.7 cm2 V−1 s−1. Additionally, incorporating alkyl urethane nonconjugated units in the backbone can reduce film crystallinity and chain aggregation, which contribute to the stretchability of the polymer thin film. Consequently, fully stretchable transistors retain carrier mobility even at 100% biaxial tensile strain. Furthermore, the fully stretchable organic field‐effect transistor arrays show remarkable charge transport reversibility and durability after 1000 stretch–release cycles at 25% strain. Additionally, the device exhibits extraordinary electrical stability in air atmosphere. Overall, these results indicate that the “regional conjugation” strategy provides an effective and promising methodology to design intrinsically stretchable and high‐performance polymer semiconductor that can advance the development of soft and wearable electronics. “Regional conjugation” strategy is developed to design intrinsically stretchable and high‐performance polymer semiconductor diketopyrrolopyrrole‐thieno[3,2‐b]thiophene (DPPTT)−urethane with oligo‐DPPTT conjugated units and alkyl urethane nonconjugated units, enabling maintaining the good charge‐transporting property under stretching. Fully stretchable transistors exhibit almost constant mobility under 100% strain, and their arrays show remarkable charge transport reversibility and durability, enduring 1000 stretch–release cycles at 25% strain.