Designing a robustly metallic noncenstrosymmetric ruthenate oxide with large thermopower anisotropy

Abstract

The existence of ~30 noncentrosymmetric metals (NCSM) suggests a contraindication between crystal structures without inversion symmetry and metallic behaviour. Those containing oxygen are especially scarce. Here we propose and demonstrate a design framework to remedy this property disparity and accelerate NCSM oxide discovery. The primary ingredient relies on the removal of inversion symmetry through displacements of atoms whose electronic degrees of freedom are decoupled from the states at the Fermi level. Density functional theory calculations validate this crystal-chemistry strategy, and we predict a new polar ruthenate exhibiting robust metallicity. We demonstrate that the electronic structure is unaffected by the inclusion of spin-orbit interactions, and that cation-ordered SrCaRu2O6 exhibits a large thermopower anisotropy (|ΔS⊥|~6.3 μV K(-1) at 300 K) derived from its polar structure. Our findings provide chemical and structural selection guidelines to aid in the search of NCSM with enhanced thermopower anisotropy.