Molecularly Engineered DBC-Pyrene Hole Transport Material Achieves Dual Passivation-Transport Functionality for...

Persistent interfacial defects and instability remain key limitations for high-performance perovskite solar cells (PSCs), motivating the development of multifunctional materials that can simultaneously enable efficient charge transport and defect passivation. Here, we report a molecularly engineered dibenzo[g,p]chrysene (DBC)-based core molecule winged by N-(4-methoxyphenyl)pyren-1-amine units, SP-07, designed to operate in two distinct yet complementary roles: as a dopant-free hole-transport material (HTM) and as an interfacial passivation layer. Owing to its planar conjugated core and electron-rich functional groups, SP-07 exhibits high intrinsic hole mobility (∼28.7 × 10^-4 cm²/V·s), uniform film formation, and efficient charge extraction. When employed as a standalone HTM, SP-07-based PSCs achieve a stabilized power conversion efficiency (PCE) of 21.7% and demonstrate exceptional operational stability under continuous illumination at 85°C, outperforming spiro-OMeTAD-based reference devices. On the other hand, acting as a passivation layer, SP-07 constructively mitigates under-coordinated Pb²⁺/halide defects, reduces trap-assisted recombination, improves surface hydrophobicity, and maintains perovskite crystallinity, resulting in devices with a champion PCE exceeding 23%. Outstandingly, passivated devices retain ∼95% of their initial PCE after 1000 h of continuous operation under thermal and illumination stress and maintain structural integrity under ambient conditions for 30 days. These findings demonstrate that the dual functionality of SP-07 enables synergistic improvements in both efficiency and long-term stability, providing a promising strategy for advancing PSCs.