Thermodynamic Stability, Structure, and Optical Properties of Perovskite-Related CsPb2Br5 Single Crystals under Pressure

CsPb2Br5 belongs to all inorganic perovskite-related quasi-two-dimensional materials that have attracted considerable attention due to their potential for optoelectronic applications. In this study, we solve numerous controversies on the physical properties of this material. We show that optical absorption in the visible spectrum and green photoluminescence are due to microcrystallites of the three-dimensional CsPbBr3 perovskite settled on the CsPb2Br5 plates and that carefully cleaned crystal plates are devoid of these features. The high-pressure structural and spectroscopic experiments, performed on the single crystals free of CsPbBr3 impurities, evidenced that the layered tetragonal structure of CsPb2Br5 is stable at least up to 6 GPa. The absorption edge is located in the ultraviolet at around 350 nm and continuously red shifts under pressure. Moderate band gap narrowing is well correlated to the pressure-induced changes in the crystal structure. Although the compressibility of CsPb2Br5 is much higher than for CsPbBr3, the response in optical properties is weaker because the Pb-Br layers responsible for the optical absorption are much less affected by hydrostatic pressure than those built of Cs+ cations. Our study clarifies the confusing data in the literature on the optical properties and thermodynamic stability of CsPb2Br5.

Automated summary

This study resolves controversies on the physical properties of CsPb2Br5, showing that optical absorption and photoluminescence are mainly caused by CsPbBr3 microcrystallites settled on the CsPb2Br5 plates. High-pressure experiments confirm the stability of the layered tetragonal structure of CsPb2Br5 and reveal a continuous red shift and moderate band gap narrowing under pressure.