Influence of Donor Skeleton on Intramolecular Electron Transfer Amount for Efficient Perovskite Solar Cells

The passivation of the defects derived from rapid-crystallization with electron-donating molecules is always a prerequisite to obtain desirable perovskite films for efficient and stable solar cells, thus, the in-depth understanding on the correlations between molecular structure and passivation capacity is of great importance for screening passivators. Here, we introduce the double-ended amide molecule into perovskite precursor solution to modulate crystallization process and passivate defects. By regulating the intermediate bridging skeletons with alkyl, alkenyl and benzene groups, the results show the passivation strength highly depends on the spin-state electronic structure that serves as an intrinsic descriptor to determine the intramolecular charge distribution by controlling orbital electron transfer from the donor segment to acceptor segment. Upon careful optimization, the benzene-bridged amide molecule demonstrates superior efficacy on improving perovskite film quality. As a physical proof-of-concept, the carbon-based, all-inorganic CsPbI2Br solar cell delivers a significantly increased efficiency of 15.51 % with a remarkably improved stability. Based on the same principle, a champion efficiency of 24.20 % is further obtained on the inverted (Cs0.05MA0.05FA0.9)Pb(I0.93Br0.07)3 solar cell. These findings provide new fundamental insights into the influence of spin-state modulation on effective perovskite solar cells. We multidimensionally reveal the relationship between passivation strength of organic passivator on perovskite film and the spin-state electronic structure of intermediate donor skeleton. Agreeing well with the calculated amounts of transferred electron between D-A pairs, the best benzene-amide pair delivers a champion efficiency of 15.51 % for carbon-based, all-inorganic CsPbI2Br solar cell and 24.20 % in an inverted (Cs0.05MA0.05FA0.9)Pb(I0.93Br0.07)3 cell. image