Excess Cesium Iodide Induces Spinodal Decomposition of CsPbI₂Br Perovskite Films

We report an exploratory study on the crystal formation behavior of CsPbI₂Br perovskite films by adding excess cesium iodide (CsI). Surprisingly, facile co-crystallization of CsI and CsPbI₂Br in the form of spinodal decomposition is observed. Significantly, the two phases spontaneously form morphing into a remarkably uniform bicontinuous nanoscale blend with high orientational correlation through the well-matched (110) plane of CsI and the (200) plane of CsPbI₂Br. The CsPbI₂Br films produced by the spinodal decomposition method not only enjoy a compact surface, low defect concentration, and long carrier lifetimes, they also retain their excellent charge transport property. By employing such a CsPbI₂Br film for carbon-based perovskite solar cells, power conversion efficiency exceeding 10% is achieved with remarkable thermal stability. Our results provide valuable insight into the role of CsI in perovskite crystallization and a promising approach for designing inorganic halide perovskite-based devices.