A semiconductor that can be processed on a large scale with a bandgap around 1.8 eV could enable the manufacture of highly efficient low cost double-junction solar cells on crystalline Si. Solution-processable organic-inorganic halide perovskites have recently generated considerable excitement as absorbers in single-junction solar cells, and though it is possible to tune the bandgap of (CH3NH3)Pb(BrxI1-x)3 between 2.3 and 1.6 eV by controlling the halide concentration, optical instability due to photoinduced phase segregation limits the voltage that can be extracted from compositions with appropriate bandgaps for tandem applications. Moreover, these materials have been shown to suffer from thermal degradation at temperatures within the processing and operational window. By replacing the volatile methylammonium cation with cesium, it is possible to synthesize a mixed halide absorber material with improved optical and thermal stability, a stabilized photoconversion efficiency of 6.5%, and a bandgap of 1.9 eV.

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 FA 1−x Pb-(Br y I 1−y ) 3 , space. With this, we identify perovskites with tandemrelevant 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 Brcontaining compositions.

Rational design approaches bring perovskite solar cells closer to meeting industrial stability criteria.

Light-induced phase segregation in mixed-halide perovskite photovoltaic materials results in the formation of low-band-gap regions that limit the voltage of devices. This work explores the dependence of this light instability on crystal structure and maps it across the cubic-tetragonal solvus in the (Cs y FA 1Ày ) Pb(Br x I 1Àx ) 3 phase diagram.