Although metal halide perovskites are positioned as the most powerful light-harvesting materials for sustainable energy conversion, there is a need for a thorough understanding of molecular design principles that would guide better engineering of organic hole-transporting materials, which are vital for boosting the performance and stability of perovskite solar cells. To address this formidable challenge, here, we developed a new design strategy based on the curved N-doped polycyclic aromatic hydrocarbon merged with T-shaped phenazines being decorated with (phenyl)-di-p-methoxyphenylamine (OMeTAD)─N-PAH23/24 and -3,6-ditertbutyl carbazole (TBCz)─N-PAH25/26. As N-PAH23/24 exhibited satisfying thermal stability, the comparative studies performed with various experimental and simulation methods revealed a pronounced correlation between the depth of the central cyclazine core and the form of the T-shape units. This proved to be a crucial factor in controlling their π–π intermolecular interaction as well as self-assembly behavior with the perovskite layer, leading to enhanced humidity resistance, operational stability, and a maximum power conversion efficiency of 20.39% denoted for N-PAH23, which is superior to the benchmarked device with doped spiro-OMeTAD (19.23%). These studies not only resulted in optimized stability and device performance but also opened a conceptually new chemical space in the photovoltaic technology.

中文翻译：

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T 形 N 掺杂多环芳烃：钙钛矿太阳能电池用无掺杂有机空穴传输材料的新概念


尽管金属卤化物钙钛矿被定位为可持续能源转换最强大的光收集材料，但需要对分子设计原理有透彻的了解，以指导更好地设计有机空穴传输材料，这对于提高钙钛矿太阳能电池的性能和稳定性至关重要。为了应对这一艰巨的挑战，我们开发了一种新的设计策略，该策略基于弯曲的 N 掺杂多环芳烃与用（苯基）-二对-甲氧基苯胺 （OMeTAD）─N-PAH23/24 和 -3,6-二丁基咔唑 （TBCz）─N-PAH25/26 修饰的 T 形吩嗪融合。由于 N-PAH23/24 表现出令人满意的热稳定性，因此使用各种实验和模拟方法进行的比较研究揭示了中心环嗪核心的深度与 T 形单元的形式之间存在显着的相关性。事实证明，这是控制它们的π-π分子间相互作用以及与钙钛矿层的自组装行为的关键因素，从而增强了耐湿性、操作稳定性和 N-PAH23 的最大功率转换效率为 20.39%，优于掺杂螺-OMeTAD 的基准器件 （19.23%）。这些研究不仅优化了稳定性和器件性能，而且在光伏技术中开辟了概念上新的化学空间。