Stabilizing Buried Interface via Synergistic Effect of Fluorine and Sulfonyl Functional Groups Toward Efficient and Stable Perovskite Solar Cells

The interfacial defects and energy barrier are main reasons for interfacial nonradiative recombination. In addition, poor perovskite crystallization and incomplete conversion of PbI2 to perovskite restrict further enhancement of the photovoltaic performance of the devices using sequential deposition. Herein, a buried interface stabilization strategy that relies on the synergy of fluorine (F) and sulfonyl (S=O) functional groups is proposed. A series of potassium salts containing halide and non-halogen anions are employed to modify SnO2/perovskite buried interface. Multiple chemical bonds including hydrogen bond, coordination bond and ionic bond are realized, which strengthens interfacial contact and defect passivation effect. The chemical interaction between modification molecules and perovskite along with SnO2 heightens incessantly as the number of S=O and F augments. The chemical interaction strength between modifiers and perovskite as well as SnO2 gradually increases with the increase in the number of S=O and F. The defect passivation effect is positively correlated with the chemical interaction strength. The crystallization kinetics is regulated through the compromise between chemical interaction strength and wettability of substrates. Compared with Cl-, all non-halogen anions perform better in crystallization optimization, energy band regulation and defect passivation. The device with potassium bis (fluorosulfonyl) imide achieves a tempting efficiency of 24.17%.

Automated summary

The interfacial defects and energy barrier are the main reasons for interfacial nonradiative recombination. Additionally, poor perovskite crystallization and incomplete conversion of PbI2 to perovskite limit the enhancement of photovoltaic performance in devices using sequential deposition. A strategy of buried interface stabilization, involving the synergy of fluorine (F) and sulfonyl (S=O) functional groups, is proposed. Chemical bonds including hydrogen, coordination, and ionic bonds are formed to enhance interfacial contact and defect passivation. The chemical interaction between modifier molecules and perovskite, as well as SnO2, increases with the augmentation of S=O and F groups, leading to improved defect passivation and crystallization kinetics.