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A novel class of thienyltriazine triamides (TTTAs) was facile synthesized and firstly used as cathode interlayers (CILs) for organic solar cells (OSCs). By utilizing different aromatic arms and pendant polar groups, their optoelectronic properties and aggregation behaviors were effectively modulated. The combination of thienyltriazine (TT) core, naphthylamide arm and imidazole pendant group endows TT−N−M with suitable energy levels, intensified work function tunability, higher conductivity, and well‐balanced crystallinity and film‐forming ability, boosting both the performance and stability of OSCs significantly. Remarkably, the solar cell efficiency remains stable at around 90 % of the optimal efficiency even as the interlayer thickness varied from 5 to 95 nm, demonstrating its insensitivity to thickness. Moreover, TT−N−M exhibits compatibility with various active layer systems, achieving a maximum efficiency of 19.60 % for single‐junction solar cell. Its exceptional tolerance to thickness fluctuations and performance establishes a new benchmark for multi‐armed CIL‐based OSCs, also positioning them among the most high‐performing CIL materials documented thus far. This work not only broadens the scope of CIL materials for OSCs but also offers deep insights into design strategies and structure‐properties relationships, being beneficial for the future development of more efficient CIL materials for organic optoelectronic applications. [ABSTRACT FROM AUTHOR]

Comprehensive Summary: Tin oxide (SnO2) has been widely used as an electron transport layer (ETL) in optoelectronic devices. However, there are numerous surface or bulk defects in SnO2, working as charge recombination centers to degrade device. Here, an electroactive and self‐healing polyurethane (PHNN) was designed by integrating conjugated unit – naphthalene diimide (NDI) into a typical polyurethane backbone. Numerous hydrogen bonds and π interactions in PHNN work as non‐covalent interactions to endow this polymer with superior self‐healing properties. PHNN contains lots of aliphatic amine and carbonyl groups, which effectively passivate the defects in SnO2. The π stacking of NDI units will facilitate electron delocalization, endowing PHNN with electrical activity compared with traditional polyurethane. Doping SnO2 with PHNN can improve the conductivity and reduce the work function of SnO2 layer, which is conducive to efficient charge extraction and transport. Using PHNN doped SnO2 as ETL for PM6: Y6 and PM6: BTP‐eC9 based inverted organic solar cells can achieve a high efficiency of 17.16% and 17.51%, respectively. Devices containing doped SnO2 ETL show significantly improved efficiency and stability. Thus, the electroactive polyurethane doped SnO2 interlayers show high performance interfacial modification to align energy‐levels in solar cell devices, which have promising applications in organic electronics. [ABSTRACT FROM AUTHOR]

Comprehensive Summary: Tin oxide (SnO2) has been widely used as an electron transport layer (ETL) in optoelectronic devices. However, there are numerous surface or bulk defects in SnO2, working as charge recombination centers to degrade device. Here, an electroactive and self‐healing polyurethane (PHNN) was designed by integrating conjugated unit – naphthalene diimide (NDI) into a typical polyurethane backbone. Numerous hydrogen bonds and π interactions in PHNN work as non‐covalent interactions to endow this polymer with superior self‐healing properties. PHNN contains lots of aliphatic amine and carbonyl groups, which effectively passivate the defects in SnO2. The π stacking of NDI units will facilitate electron delocalization, endowing PHNN with electrical activity compared with traditional polyurethane. Doping SnO2 with PHNN can improve the conductivity and reduce the work function of SnO2 layer, which is conducive to efficient charge extraction and transport. Using PHNN doped SnO2 as ETL for PM6: Y6 and PM6: BTP‐eC9 based inverted organic solar cells can achieve a high efficiency of 17.16% and 17.51%, respectively. Devices containing doped SnO2 ETL show significantly improved efficiency and stability. Thus, the electroactive polyurethane doped SnO2 interlayers show high performance interfacial modification to align energy‐levels in solar cell devices, which have promising applications in organic electronics. [ABSTRACT FROM AUTHOR]