Varying magnetism in the lattice distorted Y2NiIrO6 and La2NiIrO6 (2310.18641v2)

Abstract: We investigate the electronic and magnetic properties of the newly synthesized double perovskites Y${2}$NiIrO${6}$ and La${2}$NiIrO${6}$, using density functional calculations, crystal field theory, superexchange pictures, and Monte Carlo simulations. We find that both systems are antiferromagnetic (AFM) Mott insulators, with the high-spin Ni$^{2+}$ $t_{2g}$$^{6}e_{g}$$^{2}$ ($S=1$) and the low-spin Ir$^{4+}$ $t_{2g}$$^{5}$ ($S=1/2$) configurations. We address that their lattice distortion induces $t_{2g}$-$e_{g}$ orbital mixing and thus enables the normal Ni$^{+}$-Ir$^{5+}$ charge excitation with the electron hopping from the Ir $t_{2g}$' to Ni$e_g$' orbitals, which promotes the AFM Ni$^{2+}$-Ir$^{4+}$ coupling. Therefore, the increasing $t_{2g}$-$e_{g}$ mixing accounts for the enhanced $T_{\rm N}$ from the less distorted La${2}$NiIrO${6}$ to the more distorted Y${2}$NiIrO${6}$. Moreover, our test calculations find that in the otherwise ideally cubic Y${2}$NiIrO${6}$, the Ni$^{+}$-Ir$^{5+}$ charge excitation is forbidden, and only the abnormal Ni$^{3+}$-Ir$^{3+}$ excitation gives a weakly ferromagnetic (FM) behavior. Furthermore, we find that owing to the crystal field splitting, Hund exchange, and broad band formation in the highly coordinated fcc sublattice, Ir$^{4+}$ ions are not in the $j_{\rm eff}=1/2$ state but in the $S=1/2$ state carrying a finite orbital moment by spin-orbit coupling (SOC). This work clarifies the varying magnetism in Y${2}$NiIrO${6}$ and La${2}$NiIrO${6}$ associated with the lattice distortions.