Synthesis of Two-Dimensional CsPb 2 X 5 (X = Br and I) with a Stable Structure and Tunable Bandgap by CsPbX 3 Phase Separation.

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) CsPb 2 I 5 perovskite has been synthesized by the conversion of CsPbI 3 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 CsPbI 3 converts into tetragonal CsPb 2 I 5 and cubic CsI at 8.7 GPa upon heating from 644 to 666 K. Keeping the tetragonal structure stable, CsPb 2 I 5 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 CsPbBr 3 perovskite into 2D CsPb 2 Br 5 at high P - T conditions, indicating that the conversion of CsPbX 3 (X = Br and I) into CsPb 2 X 5 is ubiquitous.