Mesoscale Ordering 3D Mosaic Self-Assembly of Dopant-Free Hole Transport Material for Perovskite Solar Cells
Xiao‐Yuan Liu, Keli Wang, Yuheng Li, Shuai You, Tuo Liu, Yifan Lv, Yuan Li, Yu Wang, Haoxiang He, Yinxin Li, Qian Chen, Pengfei Xie, Yonghua Chen, Xiong Li, Zong‐Xiang Xu
Abstract
To enhance n-i-p perovskite solar cell (PSC) performance, we optimized the hole transport material (HTM) by using a cost-effective N, N ′-bicarbazole-based molecule, BCzSPA, with a 3D conjugated extended “L”-type configuration, to fix the molecular packing model and charge hopping channel. By implementing mesoscale molecular tailoring strategies to order the molecular stacking of BCzSPA, we have significantly realized a dense 3D mosaic self-assembly with intermolecular coupling and multichannel charge hopping properties. The proper incorporation of heteroatom-promoted multidirectional molecular interactions and enhanced morphological stability has simultaneously optimized the perovskite/HTM interfacial contact, inhibited defect formation, and further suppressed charge recombination loss. As a result, the resulting PSCs have achieved a promising efficiency of 25.42% (certified PCE, 24.53%) for a small-area (0.1 cm 2 ) device as well as 24.01% for a large-area (1 cm 2 ) device, while demonstrating remarkable stabilities, with T 80 lifetimes exceeding 2400 h under operation or thermal aging at 85 °C.