Compositional Engineering for Efficient Wide Band Gap Perovskites with Improved Stability to Photoinduced Phase Segregation

Metal halide perovskites are attractive candidates for the wide band gap absorber in tandem solar cells. While their band gap can be tuned by partial halide substitution, mixed halide perovskites often have lower open-circuit voltage than would be expected and experience photoinduced trap formation caused by halide segregation. We investigate solar cell performance and photostability across a compositional space of formamidinium (FA) and cesium (Cs) at the A-site at various halide compositions and show that using more Cs at the A-site rather than more Br at the X-site to raise band gap is more ideal as it improves both V OC and photostability. We develop band gap maps and design criteria for the selection of perovskite compositions within the Cs x FA1–x Pb­(Br y I1–y )3, space. With this, we identify perovskites with tandem-relevant band gaps of 1.68 and 1.75 eV that demonstrate high device efficiencies of 17.4 and 16.3%, respectively, and significantly improved photostability compared to that of the higher Br-containing compositions.