Intrinsically stretchable semiconducting polymers are promising candidates for developing wearable electronics, but remain underdeveloped because the correlation between the microstructural evolution during stretching and the resultant charge transport is not clearly understood. In this study, we clarify the impact of molecular orientation on the dynamic performance of stretched semiconducting polymers, controlling molecular orientations via solvent-dependent spin-coating. We found that strain-enhanced electrical performance is feasible by quelling disorders within the face-on-packed aggregates. Strain facilitates 3D ordering in face-on-packed films, but increase the π-π orientation disorders and lamellar dislocation in the edge-on analogue, which contribute inversely to the charge transport. Consequently, the face-on samples maintain strain-resistant energetic disorder and a 1.5× increase in on-current, achieving a 10-times-higher retention than the edge-on analogue upon 100% strain. Furthermore, we developed a reliable way for measuring the photoelectrical stretchability of semiconducting polymer. This study contributes to developing high-performance stretchable semiconducting polymers.

本质上可拉伸的半导体聚合物是开发可穿戴电子产品的有希望的候选者，但由于拉伸过程中的微观结构演变与由此产生的电荷传输之间的相关性尚不清楚，因此仍然不发达。在这项研究中，我们阐明了分子取向对拉伸半导体聚合物动态性能的影响，通过溶剂依赖性旋涂控制分子取向。我们发现，通过抑制正面堆积的聚集体内的紊乱，应变增强的电性能是可行的。应变有利于正面堆积薄膜中的 3D 有序性，但会增加边缘类似物中的 π-π 取向紊乱和层状位错，这对电荷传输有相反的贡献。最后，正面样品保持了抗应变的能量紊乱，并且导通电流增加了 1.5 倍，在 100% 应变下实现了比侧面样品高 10 倍的保留。此外，我们开发了一种可靠的方法来测量半导体聚合物的光电拉伸性。这项研究有助于开发高性能可拉伸半导体聚合物。