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Three azahelicene derivatives with electron-rich bis(4-methoxyphenyl)amino or bis(p-methoxyphenyl)aminophenyl groups at the terminals were deliberately designed, synthesized, and characterized as hole-transporting materials (HTMs) for perovskite solar cells (PSCs). Optical and thermal properties, energy level alignments, film morphologies, hole extraction ability, and hole mobility were studied in detail. PSCs using the newly synthesized molecules as HTMs were fabricated. A maximum power conversion efficiency (PCE) of 17.34% was observed for the bis(p-methoxyphenyl)amino-substituted derivative (SY1) and 16.10% for the bis(p-methoxyphenyl)aminophenyl-substituted derivative (SY2). Longer-chain substituent such as hexyloxy group greatly diminishes the efficiency. In addition, the dopant-free devices fabricated with SY1 as the HTM shows an average PCE of 12.13%, which is significantly higher than that of spiro-OMeTAD (7.61%). The ambient long-term stability test revealed that after 500 h, the devices prepared from SY1 and SY2 retained more than 96% of its initial performance, which is much improved than the reference device with standard spiro-OMeTAD as the HTM under the same conditions. Detailed material cost analysis reveals that the material cost for SY1 is less than 8% of that for spiro-OMeTAD. These results provide a useful direction for designing a new class of HTMs to prepare highly efficient and more durable PSCs.

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Two hole-transporting materials (HTMs) based on carbohelicene cores, CH1 and CH2, are developed and used in fabricating efficient and stable perovskite solar cells (PSCs). Owing to the rigid conformation of the helicene core, both compounds possess unique CH−π interactions in the crystalline packing pattern and good phase stability, which are distinct from the π–π intermolecular interactions of conventional planar and spiro-type molecules. PSCs based on CH1 and CH2 as HTMs deliver excellent device efficiencies of 19.36 and 18.71%, respectively, outperforming the control device fabricated with spiro-OMeTAD (18.45%). Furthermore, both PSCs exhibit better ambient stability, with 90% of initial performance retained after aging with a 50–60% relative humidity at 25 °C for 500 h. Due to the low production cost of both compounds, these newly designed carbohelicene-type HTMs have the potential for the future commercialization of PSCs.