Well-defined structure-featuring giant-molecule acceptors (GMAs) can exhibit unique properties of small-molecule acceptors and polymers simultaneously, and the consecutive innovations in materials design have enabled GMA-based organic solar cells (OSCs) to exhibit outstanding device power conversion efficiency (PCE) over 19% and extended long-term stability. Here, through systematically selecting the numbers and positions of the selenium atom, π-spacer linking units and the outermost conjugate ring of the central core of monomers, four novel GMAs are successfully synthesized, GMA-SSS, GMA-SSeS, GMA-SeSSe and GMA-SeSeSe. Surprisingly, the PM6:GMA-SSeS-based OSC yields the highest PCE of 19.37% with a remarkable open current voltage of 0.917 V with reduced voltage loss (ΔE₃ = 0.246 eV) and excellent fill factor of 77.12%. Furthermore, when devices were annealed at 100 °C, the PM6:GMA-SSeS and PM6:GMA-SSS-based OSCs exhibited remarkably extended t_80% lifetimes of 5600 and 5250 h, respectively. Our work indicates that the selenium substituted regulation of linking units and monomers of GMA structures is a valuable approach to obtain devices with high-performance and long-term stability at the same time, shedding light on the further development of GMA-based OSCs.

中文翻译：

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具有大分子受体的良好调节结构可实现长期稳定性和高性能二元有机太阳能电池


具有大分子受体 （GMA） 的明确结构可以同时表现出小分子受体和聚合物的独特特性，材料设计的连续创新使基于 GMA 的有机太阳能电池 （OSC） 表现出超过 19% 的出色器件功率转换效率 （PCE） 和延长的长期稳定性。在这里，通过系统选择硒原子、π-间隔连接单元和单体中心核心最外层共轭环的数量和位置，成功合成了四种新型 GMA，GMA-SSS、GMA-SSeS、GMA-SeSSe 和 GMA-SeSeSeSe。令人惊讶的是，基于 PM6：GMA-SSeS 的 OSC 产生了最高的 19.37% 的 PCE，具有 0.917 V 的显着开路电流电压，电压损耗降低 （ΔE₃ = 0.246 eV） 和 77.12% 的出色填充因子。此外，当器件在 100 °C 下退火时，基于 PM6：GMA-SSeS 和 PM6：GMA-SSS 的 OSC 分别表现出 _80% 的显著延长寿命，分别为 5600 和 5250 小时。我们的工作表明，GMA 结构的连接单元和单体的硒取代调节是同时获得高性能和长期稳定性的器件的有价值的方法，为基于 GMA 的 OSC 的进一步发展提供了启示。