Vitamin Natural Molecule Enabled Highly Efficient and Stable Planar n–p Homojunction Perovskite Solar Cells with Efficiency Exceeding 24.2%

Abstract The defect passivation and interface energetics‐modification between perovskite and transport layers are significant for the further improvement of efficiency and stability of perovskite solar cells (PSCs). Here, a double‐layer modification engineering strategy is employed by different functionalized natural vitamins into the electron transport layer and perovskite, respectively. Considering the different role of each functional layer in PSCs, the vitamin C (VC) with high conductivity is introduced into SnO 2 , showing electron mobility enhancement, an interface energy‐levels offsets reduction, and enhanced interfacial charge transfer. Meanwhile, antioxidant vitamin D2 (VD2) with multiple passivating functional groups is introduced into the perovskite bulk to moderately tailor its intrinsic characteristics. The surface energetics of perovskite are changed from n‐type to p‐type, the thickness of the p‐type perovskite is 80 nm, thus the spontaneous n–p homojunction is formed in perovskite caused by VD2, which increases the built‐in electric field and the efficiency of perovskite hole extraction. The synergistic effect of VC and VD2 better heightens the charge extraction efficiency and achieves charge‐carrier transport balance in PSCs. The optimum device achieves a power conversion efficiency of 24.20% and a fill factor of 81.01% with negligible hysteresis. This efficiency is among the best PSCs employing natural molecules reported so far.