Regulating Crystal Orientation via Ligand Anchoring Enables Efficient Wide-Bandgap Perovskite Solar Cells and Tandems

Wide-bandgap (WBG) perovskite solar cells have attracted considerable interest for their potential applications in tandem solar cells. However, the predominant obstacles impeding their widespread adoption are substantial open-circuit voltage (VOC) deficit and severe photo-induced halide segregation. To tackle these challenges, a crystal orientation regulation strategy by introducing dodecyl-benzene-sulfonic-acid as an additive in perovskite precursors is proposed. This method significantly promotes the desired crystal orientation, passivates defects, and mitigates photo-induced halide phase segregation in perovskite films, leading to substantially reduced nonradiative recombination, minimized VOC deficits, and enhanced operational stability of the devices. The resulting 1.66 eV bandgap methylamine-free perovskite solar cells achieve a remarkable power conversion efficiency (PCE) of 22.40% (certified at 21.97%), with the smallest VOC deficit recorded at 0.39 V. Furthermore, the fabricated semitransparent WBG devices exhibit a competitive PCE of 20.13%. Consequently, four-terminal tandem cells comprising WBG perovskite top cells and 1.25 eV bandgap perovskite bottom cells showcase an impressive PCE of 28.06% (stabilized 27.92%), demonstrating great potential for efficient multijunction tandem solar cell applications. A crystal orientation regulation strategy by introducing dodecyl-benzene-sulfonic-acid as an additive in perovskite precursors is proposed, which significantly promotes the desired (001) crystal orientation. Thus, opaque and semitransparent 1.66 eV bandgap methylamine-free perovskite solar cells realize efficiencies of 22.40% and 20.13%, respectively. Furthermore, four-terminal all-perovskite tandem cells deliver a remarkable efficiency of 28.06%.image