Improving Buried Interface Contact by Bidentate Anchoring for Inverted Perovskite Solar Cells

Abstract Nickel oxide (NiO x ) is a promising hole transport layer (HTL) to fabricate efficient and large‐scale inverted perovskite solar cells (PSCs) due to its low cost and superior chemical stability. However, inverted PSCs based on NiO x are still lagging behind that of other HTL because of the poor quality of buried interface contact. Herein, a bidentate ligand, 4,6‐bis (diphenylphosphino) phenoxazine (2DPP), is used to regulate the NiO x surface and perovskite buried interface. The diphosphine Lewis base in the 2DPP molecule can coordinate both with NiO x and lead ions at NiO x /perovskite interface, leading to high‐quality perovskite films with minimized defects. It is found that the inverted PSCs with 2DPP‐modified buried interface exhibit double advantages of being both fast charge extraction and reduced nonradiative recombination, which is a combination of multiple factors including favorable energetic alignment, improved interface contact and strong binding between NiO x /2DPP and perovskite. The optimal PSC based on 2DPP modification yields a champion power conversion efficiency (PCE) of 21.9%. The unencapsulated PSC maintains above 75% of its initial PCE in the air with a relative humidity (RH) of 30–40% for 1000 h.