Strong Electron Acceptor of a Fluorine-Containing Group Leads to High Performance of Perovskite Solar Cells

Organic–inorganic hybrid perovskites have become one of the most promising thin-film solar cell materials owing to their remarkable photovoltaic properties. However, nonradiative recombination of carriers usually leads to inferior performance of perovskite (PVK) devices. Interface modification is one of the effective ways to improve separation of charges for perovskite solar cells (PSCs). Here, a small organic molecule of tetrafluorophthalonitrile (TFPN) is used to enhance the extraction and transportation of carriers at the PVK/hole transport layer (HTL) interface. The electron-rich C–F group effectively reduces the trap state density in the perovskite through chemical combination with the empty orbital of Pb2+ or other electron traps on the PVK surface, resulting in enhanced interface contact between the PVK and HTL. Meanwhile, the CN group in TFPN also inactivates the defects caused by Pb2+. The Fermi level of the perovskite shifts by 0.15 eV to its valence band due to the strong electron acceptor nature of the F atom, indicating that positive dipoles and p-type doping emerge, which validly suppress the recombination of carriers for the PVK film. Therefore, the optimized PSC shows the highest power conversion efficiency (PCE) of 22.82% compared to 19.40% for the control one. The champion FF reaches up to 81.2% (PCE 21.44%) due to the effectively enhanced carrier separation. In addition, the unencapsulated device shows enhanced stability under air conditions.