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Development of high‐performance wide‐bandgap perovskites is a key component to enable tandem solar cells with either a silicon or low‐bandgap perovskites. However, the presence of defects in the Br‐rich wide‐bandgap perovskites, especially in the grain boundaries (GBs) has been particularly challenging and limits its performance. Herein, to accomplish the passivation of these defects, a combination of cation management with rubidium (Rb) introduction into the triple cation combination of cesium/formamidinium/methylammonium (CsFAMA) is exercised. Passivation is further enhanced by secondary growth (SG) using guanidinium iodide. In‐depth assessments of GB defect passivation are performed using Kelvin probe force microscopy (KPFM) and nanoscale charge‐carrier dynamics mappings provide insightful details on the presence of GBs defects and their suppression by the cation management and SG techniques. Reduction of unreacted PbX2to realize a highly crystalline perovskite surface is achieved after incorporating Rb and SG treatment. As a result, a champion cell for 1.78 eV (FA0.79MA0.16Cs0.05)0.95Rb0.05Pb(I0.6Br0.4)3wide‐bandgap perovskite with an efficiency of 17.71% along with enhancement in all photovoltaic parameters is achieved. This study introduces a new way to analyze GB defects and reveals the consequence of defect passivation on charge‐carrier dynamics for realizing efficient perovskites.
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Abstract In recent years, hybrid perovskite solar cells (HPSCs) have received considerable research attention due to their impressive photovoltaic performance and low‐temperature solution processing capability. However, there remain challenges related to defect passivation and enhancing the charge carrier dynamics of the perovskites, to further increase the power conversion efficiency of HPSCs. In this work, the use of a novel material, phenylhydrazinium iodide (PHAI), as an additive in MAPbI3perovskite for defect minimization and enhancement of the charge carrier dynamics of inverted HPSCs is reported. Incorporation of the PHAI in perovskite precursor solution facilitates controlled crystallization, higher carrier lifetime, as well as less recombination. In addition, PHAI additive treated HPSCs exhibit lower density of filled trap states (1010cm−2) in perovskite grain boundaries, higher charge carrier mobility (≈11 × 10−4cm2V−1s), and enhanced power conversion efficiency (≈18%) that corresponds to a ≈20% improvement in comparison to the pristine devices.
