Defect passivation engineering for achieving 4.29% light utilization efficiency MA-free wide-bandgap semi-transparent perovskite solar cells

Wide-bandgap perovskite materials are a great candidate for semitransparent perovskite solar cells (ST-PSCs) due to their tunable bandgap, outstanding transparency, and excellent photovoltaic performance. Though Br-rich perovskite can widen the bandgap, Br influences the crystallization dynamic speed leaving small perovskite grain sizes and high defects. Surface passivation engineering has been one of the best choices to suppress defects caused by the rapid crystallization of Br-rich perovskites. Herein, we applied MA-free perovskite as a light absorber because of the erratic thermal aging of MA-containing perovskites and selected phenethylammonium iodide (PEAI) and 4-trifluoro phenylethylammonium iodide (CF 3 PEAI) as passivation materials for improving the performance of opaque PSCs and ST-PSCs. Consequently, CF 3 PEA possesses a larger dipole moment. It has been demonstrated to exhibit a stronger binding energy with the substrate than PEA by density functional theory (DFT) calculations. This enhanced molecular interaction underpins the performance improvements in our solar cells, which manifests as an inverted planar structure opaque PSCs with 1.78 eV bandgap achieve a power conversion efficiency (PCE) of 17.09 % with excellent stability. A PCE of 17.17 % with 25 % average visible-light transmittance (AVT) and 4.29 % light utilization efficiency (LUE) of ST-PSCs is achieved by further optimizing the fabrication process of the buffer layer for protecting the perovskites from the damage of ITO sputter. Meanwhile, a four-terminal tandem solar cell with ST-PSC and silicon-based passivated emitter rear cell (PERC) obtains a PCE of 26.28 %. This work provides a feasible way to fabricate high-performance ST-PSCs with limited materials and preparation conditions.