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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.
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Achieving High Performance Stretchable Conjugated Polymers via Donor Structure Engineering
Abstract A backbone engineering strategy is developed to tune the mechanical and electrical properties of conjugated polymer semiconductors. Four Donor–Acceptor (D–A) polymers, named PTDPPSe, PTDPPTT, PTDPPBT, and PTDPPTVT, are synthesized using selenophene (Se), thienothiophene (TT), bithiophene (BT), and thienylenevinylenethiophene (TVT) as the donors and siloxane side chain modified diketopyrrolopyrrole (DPP) as acceptor. The influences of the donor structure on the polymer energy level, film morphology, molecular stacking, carrier transport properties, and tensile properties are all examined. The films of PTDPPSe show the best stretchability with crack‐onset‐strain greater than 100%, but the worst electrical properties with a mobility of only 0.54 cm2 V−1 s−1. The replacement of the Se donor with larger conjugated donors, that is, TT, BT, and TVT, significantly improves the mobility of conjugated polymers but also leads to reduced stretchability. Remarkably, PTDPPBT exhibits moderate stretchability with crack‐onset‐strain ≈50% and excellent electrical properties. At 50% strain, it has a mobility of 2.37 cm2V−1 s−1parallel to the stretched direction, which is higher than the mobility of most stretchable conjugated polymers in this stretching state.
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- Award ID(s):
- 2047689
- PAR ID:
- 10419255
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Macromolecular Rapid Communications
- Volume:
- 44
- Issue:
- 17
- ISSN:
- 1022-1336
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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