Computational design of layered-oxide materials

Layered-oxides have been known to host high temperature superconductivity since the discovery of cuprates. The coupling between structure and magnetism has been suggested as important factor for defining the functional properties of these materials. Despite the potential impacts, there are only a few synthesized layered oxides. Recent success in the synthesis of layered structures from three-dimensional perovskites have aimed to fill this knowledge gap by providing novel routes to synthesizing materials with desired properties. We present the feasibility of creating layered ABO₂ structures from ABO₃ (A=Ca, La, Sr, Li, Na, Nd, Pr, Y; B=Fe, Mn, Mo, V, Ni, Ru) perovskites. The oxygen vacancy formation energetics from high-throughput first-principles calculations are used as descriptors for phase transformation. The stability against decomposition into binary oxides and thermodynamic analyses of the formation conditions in terms of chemical potential of the components are presented to guide the experimental synthesis. The magnetic ground state of the ABO₂ structures, the exchange interaction parameters, and the Neel temperature from Monte Carlo simulations are explored as potential indicators of superconductivity.