Wagner, JakubChavan, Rohit D.Kruszynska, JoannaAns, MuhammadMahapatra, ApurbaEbiç, Murat2025-01-122025-01-122024Wagner, J., Chavan, R. D., Kruszyńska, J., Ans, M., Mahapatra, A., Mrkyvkova, N., Siffalovic, P., Yadav, P., Ebic, M., Akin, S., Kubas, A., Lindner, M., & Prochowicz, D. (2024). T-shaped-n-doped polycyclic aromatic hydrocarbons: a new concept of dopant-free organic hole-transporting materials for perovskite solar cells. ACS Applied Materials & Interfaces, 16(47), 64940–64950. https://doi.org/10.1021/acsami.4c186361944-82441944-8252https://doi.org/10.1021/acsami.4c18636https://hdl.handle.net/11492/10211Although 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 pi-pi 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.enPerovskite solar cellsHalide perovskiteHole-transporting materialPolycyclic aromatic hydrocarbonsStabilityArticle16476494064950info:eu-repo/semantics/closedAccess2-s2.0-85209625380WOS:0013590075000013955757810.1021/acsami.4c18636Q1N/A