![]() ![]() They have shown intriguing mechanical, thermal, and biomedical properties associated with spherical packing. Polymer crystalsomes are a class of hollow crystalline polymer nanoparticles with shells formed by single crystals with broken translational symmetry. In this work, a new strategy to design molecular dyads by using a fused‐ring design has been established, which can enable the molecular dyads to have end‐on orientation, higher charge carrier mobilities, and better crystallinity, so that the fill factors approaching 0.60 and power conversion efficiencies of 4.89% can be achieved. ![]() As a consequence, vertical charge carrier mobilities in F‐MDPBI are one order of magnitude higher than those with preferential edge‐on orientation, so single‐component OSCs based on this molecular dyad as a single photoactive layer provided a power conversion efficiency of 4.89% compared to 1.70% based on L‐MDPBI with preferential edge‐on orientation. Surprisingly, a shifting trend of the molecular orientation from dominating edge‐on in L‐MDPBI to preferential end‐on in F‐MDPBI was observed. This was realized by introducing a fused‐ring structure to replace linear terthiophenes with conjugated backbones, yielding F‐MDPBI and L‐MDPBI respectively. In this work, we for the first time obtained the preferential end‐on orientation in a conjugated molecular dyad that contains a conjugated backbone as donor and perylene bisimide side units as acceptor. Since in organic solar cells (OSCs) charge transport is along the vertical direction, end‐on orientation with conjugated backbones perpendicular to the substrate is recognized as the ideal microstructure for OSCs. Edge‐on and face‐on orientations have been widely observed, while end‐on orientation has been rarely reported. The molecular orientations of conjugated materials on the substrate mainly include edge‐on, face‐on, and end‐on. ![]()
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March 2023
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