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Interface-Engineered Composite Self-Assembled Monolayers Driving Efficient and Stable Wide-Bandgap Perovskite and
Qingquan He1, Xinquan Wang1, Gang Xu1
1Science and Education Integration, College of Energy and Carbon Neutralization, College of Materials Science and Engineering, Zhejiang Provincial Key Laboratory of Clean Energy Conversion and Utilization, State Key Laboratory of Green Chemical Synthesis and Conversion, Zhejiang University of Technology, Hangzhou 310014, P. R. China.
Abstract:
Wide-bandgap (WBG) perovskite solar cells (PSCs) based on self-assembled monolayers (SAMs) have demonstrated impressive efficiencies, though their performance and longevity remain substantially compromised by poor wettability during film formation, defects, and energy-level misalignment at the interfaces. Herein, we develop an interface regulation strategy employing a tris(4-carboxyphenyl)phosphine oxide (TC) modified [4-(7H-benzimidazol-7-yl)butyl]phosphonic acid (4PADCB) to construct a multifunctional composite SAM (Co-SAM). The incorporation of TC molecules significantly enhances the interfacial wetting characteristics and crystallization quality of WBG perovskites, effectively passivating defects, optimizing energy-level alignment, and facilitating selective charge transport. This Co-SAM strategy yields impressive device performance: 1.68 eV WBG PSCs achieve a champion power conversion efficiency (PCE) of 22.40% while maintaining >90% of initial efficiency after 1440 h of ambient storage. Furthermore, perovskite/silicon tandem solar cells fabricated using this approach reach a PCE of 30.74%. Our work establishes a new paradigm in interfacial molecular engineering for highly efficient and operationally stable tandem photovoltaics.
