Interfacial Engineering of PTAA/Perovskites for Improved Crystallinity and Hole Extraction in Inverted Perovskite Solar Cells

Inverted perovskite solar cells (PSCs) have gained rapid progress and increasing research interest in recent years. The poly (triarylamine) (PTAA) is the most frequently used semiconductor in the hole-transporting layer (HTL) in inverted PSCs for its favorable highest occupied molecular orbital energy level (−5.2 eV), excellent carrier mobility, and low-temperature solution processability. However, its intrinsic hydrophobic property hinders the growth of high-quality perovskite on the PTAA film, which is one of the main obstacles that limits the further development of inverted PSCs. Herein, a donor–acceptor–donor type organic molecule, 4,4′,4″-(1-hexyl-1H-dithieno [3′,2′:3,4; 2″,3″:5,6] benzo[1,2-d] imidazole-2,5,8-triyl) tris (N,N-bis(4-methoxyphenyl) aniline) (denoted as M2), is employed to modify the surface of PTAA. The PTAA/M2 composite hole transport layer facilitates the growth of perovskite films due to ameliorated hydrophobic property of PTAA. PTAA/M2 also exhibits enhanced hole mobility and conductivity than pristine PTAA. With enhanced crystallinity and hole extraction ability, using PTAA/M2 instead of pure PTAA as HTL, the power-conversion efficiency of inverted PSC increases from 18.67% to 20.23%. Furthermore, its operational stability is also enhanced. Our methodology carves out a novel path for addressing the hydrophobic issue of PTAA and improving the efficiency and photostability of inverted PSCs.