Roles of defects in perovskite CsPbX3 (X=I, Br, Cl): A first- principles investigation

Abstract Inorganic lead halide perovskite CsPbX3 (X=I, Br, Cl) have a promising application in optoelectronic fields due to their excellent photovoltaic properties. The defects, which have a significant impact on the performance of materials, are often introduced during the synthesis process. However, there is still a lack of systematic theoretical investigation of the effects of these defects. In this study, the effects of vacancies and H-atom interstitial point defects on the structural, electronic and optical properties of CsPbX3 are systematically investigated by using first-principles approach based on density-functional theory. The calculated results show that the introduction of different defects have significantly effect on the band gap, effective mass, semiconductor properties, ion migration and optical absorption coefficient of the perovskite materials. It is also found that VCs and VPb defects introduce shallow transition levels that do not negatively impact the optoelectronic properties. However, VX and interstitial H defects generate deep transition levels within the bandgap, which acts as non-radiative recombination centers and reduce the optoelectronic performance of the perovskite material. This study contributes to the understanding of the nature of halide chalcogenides and optimally regulating the performance of optoelectronic devices.