Antiferromagnetic Kitaev Interactions in Polar Spin-Orbit Mott Insulators

Abstract: A bond-directional anisotropic exchange interaction, called the Kitaev interaction, is a promising route to realize quantum spin liquids. The Kitaev interactions were found in Mott insulators with the strong spin-orbit coupling, in the presence of quantum interference between indirect electron transfers. Here we theoretically propose a different scenario by introducing a polar structural asymmetry that unbalances the quantum interference. We show that the imbalance activates additional exchange processes and gives rise to a dominant antiferromagnetic Kitaev interaction, in stark contrast to the conventional ferromagnetic ones. We demonstrate by ab initio calculations that polar Ru trihalides with multiple anions, $\alpha$-RuH${3/2}X{3/2}$ ($X$=Cl and Br), exhibit the antiferromagnetic Kitaev interaction whose magnitude is several times larger compared to existing candidates. Our proposal opens the way for materializing the Kitaev spin liquids in unexplored parameter regions.