Impact of cesium on the phase and device stability of triple cation Pb-Sn double halide perovskite films and solar cells

Triple cation Cs/methylammonium (MA)/formamidinium (FA) and double halide Br/I lead perovskites improved the stability and efficiency of perovskite solar cells (PVSCs). However, their effects on alloyed Pb-Sn perovskites are unexplored. In this work, perovskite thin films with the composition Cs-x(MA(0.17)FA(0.83))(1-x)Pb1-ySny(I0.83Br0.17)(3) are synthesized utilizing a one-step solution process plus an anti-solvent wash technique and deployed in PVSCs with an inverted architecture. All films show a cubic crystal structure, demonstrating that compositional tuning of both the tolerance factor and crystallization rate allows for dense, single phase formation. The band gaps, affected by both lattice constriction and octahedral tilting, show opposite trends in Pb-rich or Sn-rich perovskites with the increase of Cs for fixed Sn compositions. The Cs-0.05(MA(0.17)FA(0.83))(0.95)Pb0.25Sn0.75(I0.83Br0.17)(3) PVSCs achieve a power conversion efficiency (PCE) of 11.05%, a record for any PVSC containing 75% Sn perovskites, and the Cs-0.10(MA(0.17)FA(0.83))(0.90)Pb0.75Sn0.25(I0.83Br0.17)(3) PVSCs reach a record PCE of 15.78%. Moreover, the triple cation and double halide alloyed Pb-Sn perovskites exhibit improved device stability under inert and ambient conditions. This study, which illustrates the impact of cation and halide tuning on alloyed Pb-Sn perovskites, can be used to further eliminate Pb and improve device performance of high Sn PVSCs and other optoelectronic devices.