Science China Materials, 2024 (SCI-Expanded)
Self-assembled molecules (SAMs), which consist of a π-conjugated unit and an anchoring group linked by a side chain, play a critical role in functioning as hole-selective contacts. They significantly influence the performance and stability of inverted perovskite solar cells (PSCs). Current research primarily focuses on optimizing the side chains to enhance device performance. However, the effects of π-conjugation structures on the power conversion efficiency (PCE) and stability of PSCs remain largely unexplored. In this study, we designed a series of SAMs featuring gradually extended π-conjugation structures while maintaining a fixed anchoring group, in order to elucidate the impact of extended π-conjugation on electronic properties. As the π-conjugation of the SAM core structure was extended, we observed an improvement in device performance due to enhanced hole extraction and transport. Furthermore, the operational stability of PSCs increased as intermolecular π-π interactions strengthened. The SAM with the optimal π-conjugation structure, referred to as Py2, resulted in an inverted PSC with enhanced operational stability and a PCE of up to 25.2%. (Figure presented.)