Structural and Photophysical Properties of Guanidinium-Iodide-Treated Perovskite Solar Cells

Use of the guanidinium iodide (GAI) cation is widely recognized as an interface engineering technique for perovskite solar cells that deliver stability improvements via defect passivation on surfaces and grain boundaries. However, a comprehensive understanding of the relationship between the structural and photophysical properties is lacking. Herein, GAI-induced perovskite structural modifications, including derivative phases and underlying transitions, are detected in GAI surface-treated Cs(0.07)MA(0.14)FA(0.79)Pb(I0.83Br0.17)(3) through an analysis of X-ray and electron diffraction and microscopy data. An optimum GAI solution concentration at 10 mg mL(-1) can eliminate excess PbI2, improve crystallinity, and increase grain size of the as-prepared perovskite films. However, a further increase to 20-40 mg mL(-1) induces new (FAPbI(3))(x)(GA(2)PbI(4))(x) phases and a reduction in crystallinity and grain size. In addition, from confocal photoluminescence imaging, it is observed that 10 mg mL(-1) GAI also helps to remove the microscale spatial heterogeneities, demonstrating optimum device performance. These results show that understanding the impact on structure and microstructure of the selection and concentration of surface treatment agents is critical for the homogenization of perovskite optoelectronic properties and achieving efficient device.

Automated summary

The use of guanidinium iodide (GAI) cation as an interface engineering technique in perovskite solar cells improves stability by passivating defects on surfaces and grain boundaries. However, the relationship between structural and photophysical properties is not well understood. This study demonstrates that an optimal concentration of GAI can eliminate excess PbI2, improve crystallinity, and increase grain size. Higher concentrations induce the formation of new phases and reduce crystallinity and grain size. GAI treatment also helps remove microscale heterogeneities, resulting in optimum device performance.