A clear understanding of the structure-property relationship of intrinsically stretchable polymer semiconductors (ISPSs) is essential for developing high-performance polymer-based electronics. Herein, we investigate the effect of the fluorination position on the crystalline structure, charge-carrier mobility, and stretchability of polymer semiconductors based on a benzodithiophene--benzotriazole configuration. Although four different polymer semiconductors showed similar field-effect mobilities for holes (μ ≈ 0.1 cm V s), polymer semiconductors with nonfluorinated backbones exhibited improved thin-film stretchability confirmed with crack onset strain (ε ≈ 20%-50%) over those of fluorinated counterparts (ε ≤ 10%). The enhanced stretchability of polymer semiconductors with a nonfluorinated backbone is presumably due to the higher face-on crystallite ratio and π-π stacking distance in the out-of-plane direction than those of the other polymer semiconductors. These results provide new insights into how the thin-film stretchability of polymer semiconductors can be improved by using precise molecular tailoring without deteriorating electrical properties.
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