Intersite Coulomb repulsion driven quadrupole instability and magnetic ordering in the orbital frustrated Ba$_2$MgReO$_6$

Abstract

We develop an unrestricted Hartree-Fock mean-field method including Coulomb repulsion $U$, $V$ and spin-orbital coupling $\lambda$ self-consistently to investigate the mechanism of structural instability and magnetic ordering in Ba$_2$MgReO$_6$. A comprehensive quadrupole phase diagram versus $U$ and $V$ with $\lambda$=0.28eV is calculated. Our results demonstrate that the easy-plane anisotropy and the intersite Coulomb repulsion $V$ must be considered to remove the orbital frustration. The increasing of $V$ to $>$20meV would arrange quadrupole $Q_{x^2-y^2}$ antiparallelly, accompanied with small parallel $Q_{3z^2-r^2}$, and stabilize Ba$_2$MgReO$_6$ into the body-centered tetragonal structure. Such antiparallel $Q_{x^2-y^2}$ provides a new mechanism of Dzyaloshinskii-Moriya interaction, and gives rise to the canted antiferromagnetic (CAF) state along [110] axis. Moreover, sizable octupoles such as $O_{21}^{31}$, $O_{21}^{33}$, $O_{21}^{34}$ and $O_{21}^{36}$ are discovered for the first time in CAF state. Our study not only provides a comprehensive understanding of the experiment results in Ba$_2$MgReO$_6$, but also reveals some commonalities of 5d compounds.