Revealing the Mechanism of π Aromatic Molecule as an Effective Passivator and Stabilizer in Highly Efficient Wide‐Bandgap Perovskite Solar Cells

Trap‐induced nonradiative recombination and decomposition are the major limiting factors that hinder the development of mixed‐halide wide‐bandgap perovskite solar cells. Specifically, the incorporation of formamidinium (FA + ) and bromide in wide‐bandgap (WBG) perovskite materials leads to shallow‐energy‐level traps and inferior light stability. Herein, the electron‐withdrawing molecule 2,3,5,6 tetrafluoro‐7,7,8,8‐tetracyanoquinodimethane (F4‐TCNQ) is used as an effective passivator and stabilizer, which has molecular interaction with the FA + cation for reducing trap densities and enhancing the stability of WBG perovskite solar cells. It is found that the extended π aromatic system in F4‐TCNQ can enhance the binding energy and stabilize the FA + cation in perovskite films. Furthermore, the 1.67 eV bandgap inverted perovskite solar cells with a small amount of F4‐TCNQ have shallower defect levels, reduced trap density, and decreased nonradiative recombination, therefore giving a remarkably improved power conversion efficiency (PCE) of 20.0%. Most importantly, the unencapsulated devices with F4‐TCNQ additive have greatly enhanced stability, maintaining 88% of their peak PCEs under continuous illumination after 840 h, whereas the control devices only retain 48% of their PCEs after 500 h.