High-throughput first-principles screening of layered magnetic double perovskites Cs₄MSb₂X₁₂ for spintronic...

Double perovskite halides have drawn great attention due to characteristics of non-toxicity, stability and broad elemental compositions compared to CH₃NH₃PbI₃. Among them, layered double perovskite halides have been proposed as promising photovoltaic materials. Noteworthily, layered materials have been extensively explored as spintronic materials. Can layered double perovskites act as spintronic material and thus extend the application from optoelectronics to spintronics? In this paper, we investigated a series of 〈1 1 1〉-oriented layered magnetic double perovskites by high-throughput first-principles calculations to find suitable spintronic candidates. Three thermodynamically stable layered double perovskites Cs₄MnSb₂Cl₁₂, Cs₄CuSb₂Cl₁₂ and Cs₄ScSb₂Br₁₂ are identified. The ground state structure of Cs₄MnSb₂Cl₁₂ has the R-3m symmetry and exhibits antiferromagnetic (AFM) ordering, while Cs₄CuSb₂Cl₁₂ favors the C2/m symmetry and shows AFM ordering, which are in line with the experimental observations. Cs₄MnSb₂Cl₁₂ and Cs₄CuSb₂Cl₁₂ are AFM semiconductors. Additionally, a new layered double perovskite Cs₄ScSb₂Br₁₂ is predicted for the first time, favoring the C2/m symmetry and showing metallicity and AFM ordering, which may be synthesized experimentally in the future.