The photoluminescence mechanism of CsPb2Br5 microplates revealed by spatially resolved single particle spectroscopy

Abstract

CsPb₂Br₅ is a new member of the all-inorganic lead halide perovskite family with unique structures and optoelectronic properties for various applications. As an indirect band gap semiconductor, the photoluminescence (PL) mechanism of CsPb₂Br₅ is still under debate. To resolve this issue, CsPb₂Br₅ microplates with strong green PL have been prepared by a hot-injection method. Characterization by transmission electron microscopy (TEM), X-ray diffraction (XRD) analysis and ultraviolet-visible (UV-vis) absorption spectroscopy indicates the existence of a small amount of embedded CsPbBr₃ phase. The removal of the embedded CsPbBr₃ phase by treatment with water containing ethanol solvent resulted in complete PL quenching, suggesting the origin of PL due to the embedded CsPbBr₃ phase. Spatially resolved PL and time-resolved PL mapping have been further employed to directly visualize the spatial distribution of different emission centers. Our single particle spectroscopic studies indicated the existence of three different emission centers with different PL lifetimes: two types of embedded CsPbBr₃ phases (clumped and randomly distributed CsPbBr₃ nanocrystals) and intrinsic defects of CsPb₂Br₅. The embedded CsPbBr₃ phases with fast and intermediate PL lifetimes are the primary contributors to PL of the CsPb₂Br₅ microplates while their intrinsic defects with slow PL lifetimes make only a minor contribution. These studies have unambiguously clarified the PL mechanisms of the CsPb₂Br₅ microplates and provided the direct mapping of different emission centers, which resolve the contradictory explanation and debate about the PL mechanism of the CsPb₂Br₅ microplates.