Combination of Metal Oxide and Polytriarylamine: A Design Principle to Improve the Stability of Perovskite Solar Cells

In the last decade, perovskite photovoltaics gained popularity as a potential rival for crystalline silicon solar cells, which provide comparable efficiency for lower fabrication costs. However, insufficient stability is still a bottleneck for technology commercialization. One of the key aspects for improving the stability of perovskite solar cells (PSCs) is encapsulating the photoactive material with the hole-transport layer (HTL) with low gas permeability. Recently, it was shown that the double HTL comprising organic and inorganic parts can perform the protective function. Herein, a systematic investigation and comparison of four double HTLs incorporating polytriarylamine and thermally evaporated transition metal oxides in the highest oxidation state are presented. In particular, it was shown that MoOx, WOx, and VOx-based double HTLs provided stable performance of PSCs for 1250 h, while devices with NbOx lost 30% of their initial efficiency after 1000 h. Additionally, the encapsulating properties of all four double HTLs were studied in trilayer stacks with HTL covering perovskite, and insignificant changes in the absorber composition were registered after 1000 h under illumination. Finally, it was demonstrated using ToF-SIMS that the double HTL prevented the migration of perovskite volatile components within the structure. Our findings pave the way towards improved PSC design that ensures their long-term operational stability.