Pattern-Induced Directional Shear Force Synergized With Regulation of Multicomponent Fragments Entropy Effect for...

The ordered arrangement of polymer chains in printable all-polymer solar cells (all-PSCs) is constrained by weak shear force during the blade-coating process, which hinders the construction of dual-fiber network morphology in the active layer. Herein, we have first proposed a synergistic strategy by patterned blade-coating with modulation of multicomponent fragmental entropy effect to construct pseudo-planar heterojunction (PPHJ) all-PSCs with an ideal vertical gradient distribution. The patterned blades allow polymer fluid to be extruded in a confined space, which can enhance the directional shear capability during the printing process, thus effectively guiding the stretching of polymer chains. Furthermore, the introduction of PTQ10 with favorable packing orientation can effectively bind with PM6 fragments to suppress the entropy-driven retraction effect and alleviate excessive aggregation of PM6 fragments, which is beneficial to form PPHJ structure with favorable phase separation. Therefore, the device based on PM6:PTQ10/PY-DT system exhibits a competitive power conversion efficiency (PCE) of 19.78%, with a fill factor of nearly 80%. Notably, the corresponding 16.94 cm² flexible module achieves PCE of 16.08%. These results indicate directional fluid force guidance and ordered polymer fragments stacking are key for dual-fiber morphology, providing a reliable approach for all-PSCs commercialization.