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Abstract In order to apply polymer semiconductors to stretchable electronics, they need to be easily deformed under strain without being damaged. A small number of conjugated polymers, typically with semicrystalline packing structures, have been reported to exhibit mechanical stretchability. Herein, a method is reported to modify polymer semiconductor packing‐structure using a molecular additive, dioctyl phthalate (DOP), which is found to act as a molecular spacer, to be inserted between the amorphous chain networks and disrupt the crystalline packing. As a result, large‐crystal growth is suppressed while short‐range aggregations of conjugated polymers are promoted, which leads to an improved mechanical stretchability without affecting charge‐carrier transport. Due to the reduced conjugated polymer intermolecular interactions, strain‐induced chain alignment and crystallization are observed. By adding DOP to a well‐known conjugated polymer, poly[2,5‐bis(4‐decyltetradecyl)pyrrolo[3,4‐c]pyrrole‐1,4‐(2H,5H)‐dione‐(E)‐1,2‐di(2,2′‐bithiophen‐5‐yl)ethene] (DPPTVT), stretchable transistors are obtained with anisotropic charge‐carrier mobilities under strain, and stable current output under strain up to 100%. 

Abstract For wearable and implantable electronics applications, developing intrinsically stretchable polymer semiconductor is advantageous, especially in the manufacturing of large‐area and high‐density devices. A major challenge is to simultaneously achieve good electrical and mechanical properties for these semiconductor devices. While crystalline domains are generally needed to achieve high mobility, amorphous domains are necessary to impart stretchability. Recent progresses in the design of high‐performance donor–acceptor polymers that exhibit low degrees of energetic disorder, while having a high fraction of amorphous domains, appear promising for polymer semiconductors. Here, a low crystalline, i.e., near‐amorphous, indacenodithiophene‐co‐benzothiadiazole (IDTBT) polymer and a semicrystalline thieno[3,2‐b]thiophene‐diketopyrrolopyrrole (DPPTT) are compared, for mechanical properties and electrical performance under strain. It is observed that IDTBT is able to achieve both a high modulus and high fracture strain, and to preserve electrical functionality under high strain. Next, fully stretchable transistors are fabricated using the IDTBT polymer and observed mobility ≈0.6 cm²V⁻¹s⁻¹at 100% strain along stretching direction. In addition, the morphological evolution of the stretched IDTBT films is investigated by polarized UV–vis and grazing‐incidence X‐ray diffraction to elucidate the molecular origins of high ductility. In summary, the near‐amorphous IDTBT polymer signifies a promising direction regarding molecular design principles toward intrinsically stretchable high‐performance polymer semiconductor.