Spin-orbit coupling, strong correlation, and insulator-metal transitions: the J$_{\rm eff}$ =3\2 ferromagnetic Mott insulator Ba$_{2}$NaOsO$_{6}$

Abstract

The double perovskite Ba$_{2}$NaOsO$_{6}$ (BNOO), an exotic example of a very high oxidation state (heptavalent) osmium $d^1$ compound and also uncommon by being a ferromagnetic Mott insulator without Jahn-Teller (JT) distortion, is modeled using the density functional theory (DFT) hybrid functional based exact exchange for correlated electrons (oeeHyb) method and including spin-orbit coupling (SOC). The experimentally observed narrow gap ferromagnetic insulating ground state is obtained, with easy axis along [110] in accord with experiment, providing support that this approach provides a realistic method for studying this system. The predicted spin density for [110] spin orientation is nearly cubic (unlike for other directions), providing an explanation for the absence of JT distortion. An orbital moment of -0.4$\mu_B$ strongly compensates the +0.5$\mu_B$ spin moment on Os, leaving a strongly compensated moment more in line with experiment. Remarkably, the net moment lies primarily on the oxygen ions. An insulator-metal transition by rotating the magnetization direction with an external field under moderate pressure is predicted as one consequence of strong SOC, and metallization under moderate pressure is predicted. Comparison is made with the isostructural, isovalent insulator Ba$_2$LiOsO$_6$ which however orders antiferromagnetically.