Energetic and electronic properties of CsPbBr3 surfaces: a first-principles study

Abstract

Surface properties of all-inorganic halide perovskites play a crucial role in determining optoelectronic performance of these materials. We investigate the surface energies and electronic structures of cubic CsPbBr₃ surfaces systematically using density functional theory (DFT) methods. We calculate the surface phase diagrams of low-index surfaces of CsPbBr₃, i.e., (100), (110), (111) surfaces. We found that nonpolar (100) surfaces are more stable than polar (110) and (111) surfaces. The nonpolar CsBr-terminated (100) surface shows the best stability, which is attributed to the effect of surface relaxation and high ionicity of the surface layer. The electronic structures reveal that charge transfer to compensate the polarity raises the energy of polar surfaces, which makes polar surfaces unstable. Furthermore, we found that the modulation of surface chemical composition provides an effective way to compensate polarity and thus make polar surfaces of CsPbBr₃ stable. Our results provide physical insights into understanding and further enhancing the surface stability of all-inorganic halide perovskites. This would be helpful in promoting the advancement of all-inorganic halide perovskite-based materials and devices.