High-temperature electronic materials are in constant demand as the required operational range for various industries increases. Here we design ($A$,$A^{\prime }$)$B_2{\mathrm{O}}_6$ perovskite oxides with [111] “rock salt” $A$-site cation order and predict them to be potential high-temperature piezoelectric materials. By selecting bulk perovskites which have a tendency towards only out-of-phase $B{\mathrm{O}}_6$ rotations, we avoid possible staggered ferroelectric to paraelectric phase transitions while also retaining noncentrosymmetric crystal structures necessary for ferro- and piezoelectricity. Using density functional theory calculations, we show that (La,Pr)${\mathrm{Al}}_2{\mathrm{O}}_6$ and (Ce,Pr)${\mathrm{Al}}_2{\mathrm{O}}_6$ display spontaneous polarizations in their polar ground state structures; we also compute the dielectric and piezoelectric constants for each phase. Additionally, we predict the critical phase transition temperatures for each material from first-principles to demonstrate that the piezoelectric responses, which are comparable to traditional lead-free piezoelectrics, should persist to high temperature. These features make the rock salt $A$-site-ordered aluminates candidates for high-temperature sensors, actuators, or other electronic devices.

• Received 1 March 2014
• Revised 4 May 2014

DOI:https://doi.org/10.1103/PhysRevB.89.174110