Polymer aggregation plays a critical role in the miscibility of materials and the performance of all‐polymer solar cells (APSCs). However, many aspects of how polymer texturing and aggregation affect photoactive blend film microstructure and photovoltaic performance are poorly understood. Here the effects of aggregation in donor–acceptor blends are studied, in which the number‐average molecular weights (M_ns) of both an amorphous donor polymer, poly[4,8‐bis(5‐(2‐ethylhexyl)thiophen‐2‐yl)benzo[1,2‐b;4,5‐b′]dithiophene‐2,6‐diyl‐alt‐(4‐(2‐ethylhexyl)‐3‐fluorothieno[3,4‐b]thiophene‐)‐2‐carboxylate‐2‐6‐diyl)] (PBDTT‐FTTE) and a semicrystalline acceptor polymer, poly{[N,N′‐bis(2‐octyldodecyl)naphthalene‐1,4,5,8‐bis(dicarboximide)‐2,6‐diyl]‐alt‐5,5′‐(2,2′‐bithiophene)} (P(NDI2OD‐T2)) are systematically varied. The photovoltaic performance is correlated with active layer microstructural and optoelectronic data acquired by in‐depth transmission electron microscopy, grazing incidence wide‐angle X‐ray scattering, thermal analysis, and optical spectroscopic measurements. Coarse‐grained modeling provides insight into the effects of polymer aggregation on the blend morphology. Notably, the computed average distance between the donor and the acceptor polymers correlates well with solar cell photovoltaic metrics such as short‐circuit current density (J_sc) and represents a useful index for understanding/predicting active layer blend material intermixing trends. Importantly, these results demonstrate that for polymers with different texturing tendencies (amorphous/semicrystalline), the key for optimal APSC performance, photovoltaic blend morphology can be controlled via both donor and acceptor polymer aggregation.

中文翻译：

---

通过系统地调节全聚合物太阳能电池中的聚集来进行光敏共混物形态工程

聚合物聚集在材料的混溶性和全聚合物太阳能电池（APSC）的性能中起着至关重要的作用。但是，关于聚合物纹理化和聚集如何影响光敏共混膜微结构和光伏性能的许多方面，人们对此知之甚少。在这里，在供体-受体混合物聚集的影响进行了研究，其中所述数均分子量（中号_Ñ两者的一个或多个）无定形供体聚合物，聚[4,8-双（5-（2-乙基己基）噻吩2-基）苯并[1,2- b ; 4,5 - b' ]二噻吩-2,6-二基-alt-（4-（2-乙基己基）-3-氟噻吩[3,4- b ]噻吩）-2-羧酸酯-2-6-二基）]（PBDTT-FTTE）和半结晶受体聚合物poly {[ N，N'-双（2-辛基十二烷基）萘-1,4,5,8-双（二​​甲酰亚胺）-2,6-二基] -alt-5,5'-（2,2'-联噻吩）}（P（ NDI2OD-T2））是系统地变化的。光伏性能与通过深入透射电子显微镜，掠入射入射的广角X射线散射，热分析和光谱测量获得的活性层微结构和光电数据相关。粗粒度建模可以深入了解聚合物聚集对共混物形态的影响。值得注意的是，计算得到的供体和受体聚合物之间的平均距离与太阳能电池光伏指标（例如短路电流密度（J _sc），它是了解/预测活性层共混材料相互混合趋势的有用指标。重要的是，这些结果表明，对于具有不同纹理化趋势（非晶/半结晶）的聚合物，APSC性能最佳的关键，可以通过施主和受主聚合物的聚集来控制光伏共混物的形态。