Optoelectronic Properties of Double Perovskites: Influence of Fe/Co Substitution and Magnetic Ordering on Band Structures and Bandgaps
摘要
Magnetism-assisted photovoltaic technology has emerged as a promising avenue for boosting the efficiency of photovoltaic cells, making it a significant research topic. Despite notable advancements in the industrial development of these materials, there are still critical challenges to overcome, including achieving tailored bandgaps, utilizing non-toxic and earth-abundant constituent elements, attaining high power conversion efficiency (PCE), and ensuring superior optical properties. In this study, spin-polarized hybrid functional calculations were employed to investigate the electronic and magnetic properties of halide double perovskites (HDPs), specifically Cs2AgFeX6 and Cs2AgCoX6 (where X = Cl, Br, I), to identify magnetically active materials containing abundant components that can enhance PCE in perovskite solar cells. Our results reveal two key findings. Firstly, both the Fe- and Co-based perovskites are more stable in the antiferromagnetic state than in the ferromagnetic state. Secondly, the exact exchange fraction significantly impacts the electronic and magnetic properties of HDPs. Further analysis of Cs2AgFeX6 and Cs2AgCoX6 shows that their bandgaps span a range of 0.59 eV to 1.66 eV, making them well suited to photovoltaic applications. These findings demonstrate that Cs2AgFeX6 and Cs2AgCoX6 are promising candidates for next-generation perovskite solar cells.
Graphical Abstract