Interfacial Hybrid Engineering Strategy for Highly Efficient and Stable Large-Area Perovskite Solar Modules

Self-assembled molecules (SAMs) are considered promising materials for hole transport layers (HTL) in inverted perovskite solar cells (p-i-n PSCs). However, incomplete coverage, poor uniformity, and insufficient stability of SAM films still hinder the large-scale industrial application of SAM-based HTLs in PSCs. Here, an interfacial hybrid engineering (IHE) strategy is proposed that incorporates a molecular suppressor, 4,4,4-tris(phosphoryl) triphenylmethane (PA), to regulate SAM assembly and optimize interfacial properties. PA effectively mitigates molecular aggregation of 2-(9H-carbazol-9-yl) ethylphosphonic acid (2PACz) through steric hindrance and chemical interactions, which ensures the homogeneous distribution, well-ordered assembly, and scale-up preparation of SAM molecules. Thereby, the perovskite/HTL interface exhibits improved energy level alignment, charge extraction efficiency, and defect passivation. The champion PCE of the PA-based small-area devices is 26.55%. Large-area modules incorporating PA exhibit record-breaking efficiencies of 22.81% (22.8 cm²) and 20.16% (750.5 cm²), representing the highest performance reported for single SAM-HTL layers in scalable PSCs. Additionally, PA-modified devices demonstrate remarkable operational stability under ISOS-D and ISOS-L testing conditions. This IHE strategy provides an effective and scalable solution for achieving uniform SAM deposition in large-area PSCs while simultaneously enhancing device efficiency and long-term durability, paving the way for the commercialization of SAM-based perovskite photovoltaics.