T-Shaped-N-Doped Polycyclic Aromatic Hydrocarbons: A New Concept of Dopant-Free Organic Hole-Transporting Materials for Perovskite Solar Cells
Jakub Wagner, Rohit D. Chavan, Joanna Kruszyńska, Muhammad Ans, Apurba Mahapatra, Nada Mrkyvkova, Peter Šiffalovič, Pankaj Yadav, Murat Ebiç, Seçkin Akın, Adam Kubas, Marcin Lindner, Daniel Prochowicz
Abstract
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.