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

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.