Ionic Liquid-Induced Multisite Synergistic Interactions for Highly Efficient Inverted Perovskite Solar Cells

The interfacial properties of p-i-n inverted perovskite solar cells (PSCs) play a key role in further improving the photovoltaic performance of PSCs. Herein, multisite synergistic interactions were constructed using ionic liquids (ILs) prepared by mixing urea and choline chloride (ChCl) to substantially improve the interfacial properties of inverted PSCs. Systematically theoretical calculations and experimental studies are comprehensively performed, which reveal that the C═O···Pb²⁺ coordination interaction, N-H···I hydrogen bond, and Cl-Pb bond could be simultaneously formed between the perovskites and IL, and Ch in IL could interact with the perovskite by occupying the formamidinium site. Meanwhile, -OH/π and -NH/π interactions could be formed between -OH and -NH in IL and the phenyl group in PTAA, respectively. These multisite synergistic interactions are beneficial to improve the perovskite film quality and interfacial properties of inverted PSCs, which could greatly suppress nonradiative recombination within the PSCs. Consequently, the inverted PSCs show an impressive efficiency of 22.4% and an excellent electroluminescence efficiency of 3.7%.