Directionally Selective Polyhalide Molecular Glue for Stable Inverted Perovskite Solar Cells

Abstract

The fundamental instability of hybrid perovskite solar cells originates from the considerable halide vacancies. Furthermore, the local roles of halide vacancies between grain boundaries and grain bulk generally conflict, thus inhibiting complete passivation. To overcome this obstacle, a rational polyhalide ligand, di‐(2‐picolyl)amine triiodide, is designed as a molecular “glue” to achieve comprehensive passivation. Unlike a monohalide ligand, this ligand has multiple iodide ions and a quasiplanar tridentate chelation capability, contributing to directional passivation along the grain boundaries and overall passivation throughout the grain bulk. Using this molecular glue passivation, the best inverted solar cell yields an efficiency of 20.02%. Moreover, the relative stability of this cell in ambient air (≈40% humidity, 800 h aging) and under light‐soaking conditions (500 h aging) is profoundly enhanced by 33.33% and 22.26%, respectively. Herein, important insights into the design of passivating molecules to achieve low‐defect perovskites toward the development of multifunctional devices are provided.