Synthesis of Two-Dimensional CsPb₂X₅ (X = Br and I) with a Stable Structure and Tunable Bandgap by CsPbX₃ Phase...

Perovskite-related materials with various dimensionalities have attracted sustained attention owing to their extraordinary electronic and optoelectronic properties, but it is still challenging in the synthesis of compounds with desired compositions and structures. Herein, a two-dimensional (2D) CsPb₂I₅ perovskite has been synthesized by the conversion of CsPbI₃ at high-pressure and high-temperature (high P-T) conditions, which is quenchable at ambient conditions. In situ synchrotron X-ray diffraction shows that high-pressure monoclinic CsPbI₃ converts into tetragonal CsPb₂I₅ and cubic CsI at 8.7 GPa upon heating from 644 to 666 K. Keeping the tetragonal structure stable, CsPb₂I₅ exhibits tunable optical properties with the bandgap changing from ∼2.4 eV at ambient pressure to ∼1.4 eV at 36.9 GPa. Further experiments demonstrate similar structural evolution in the typical three-dimensional CsPbBr₃ perovskite into 2D CsPb₂Br₅ at high P-T conditions, indicating that the conversion of CsPbX₃ (X = Br and I) into CsPb₂X₅ is ubiquitous.