To achieve efficient non-fullerene polymer solar cells (NF-PSCs), an in-depth understanding of the key properties that govern the power output is necessary. Herein, three trialkylsilyl substituted benzodithiophene-based polymer donors (PJ1, PJ2, and PJ3) were synthesized with fine-tuning of the highest occupied molecular orbital (HOMO)/lowest unoccupied molecular orbital (LUMO) and optical absorption. Using the polymer series paired with absorption-complementary small molecular acceptors (SMAs), namely, m-ITIC, IDIC, and AIDIC, we systematically studied the performance of a 3 × 3 matrix of NF-PSCs. An increasing open-circuit voltage with deepening HOMOs of the polymer donors, and the enhanced short-circuit current (J_SC) and fill factor (FF) were ascribed to the well-intermixed blend morphology containing enhanced SMA order ranges with mixed face-on and edge-on orientations, the so-called 3-D texture. Such an optimal microstructure is best exemplified in the PJ2:IDIC combination, affording a highest efficiency of 12.01% with a simultaneously high J_SC of 17.0 mA cm⁻² and FF of 75.3%. The devices with an active layer thickness of 300 nm still maintain an impressive efficiency approaching 10% with a decent FF of 60.0%. Moreover, the Channel II process, i.e., photoinduced hole transfer through acceptor excitation, was demonstrated to be crucially important for photocurrent generation. This study highlights the importance of optimizing the trade-off between charge separation/transport and domain size to achieve high-performance NF-PSCs.

中文翻译：

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由3-D织构诱导的超快通道II工艺，具有增强的受体序数范围，适用于高性能非富勒烯聚合物太阳能电池†

为了获得有效的非富勒烯聚合物太阳能电池（NF-PSC），必须深入了解控制功率输出的关键特性。本文中，合成了三个三烷基甲硅烷基取代的苯并二噻吩基聚合物供体（PJ1，PJ2和PJ3），对微区的最高占据分子轨道（HOMO）/最低未占据分子轨道（LUMO）和光吸收进行了微调。使用与吸收互补小分子受体（SMA），即m -ITIC，IDIC和AIDIC配对的聚合物系列，我们系统地研究了3×3 NF-PSC基质的性能。开路电压增加，聚合物供体的HOMO变深，短路电流增加（J _SC填充因子（FF）和填充因子（FF）归因于充分混合的混合形态，该形态包含增强的SMA有序范围，具有面向上和面向上的混合方向，即所谓的3D纹理。这种最佳的微观结构在PJ2：IDIC组合中得到了最好的体现，它具有12.01％的最高效率，同时具有17.0 mA cm ^-2的高J _SC和75.3％的FF。有源层厚度为300 nm的器件在FF达到60.0％的情况下仍能保持接近10％的出色效率。此外，第二频道的过程，即通过受体激发而引起的光致空穴转移对光电流的产生至关重要。这项研究强调了优化电荷分离/传输与域大小之间的权衡以实现高性能NF-PSC的重要性。