Two-site fluctuations and multipolar intersite exchange interactions in strongly correlated systems

Abstract

An approach is proposed for evaluating dipolar and multipolar intersite interactions in strongly correlated materials. This approach is based on the single-site dynamical mean-field theory (DMFT) in conjunction with the atomic approximation for the local self-energy. Starting from the local-moment paramagnetic state described by DMFT, we derive intersite interactions by considering the response of the DMFT grand potential to small fluctuations of atomic configurations on two neighboring sites. The present method is validated by applying it to one-band and two-band ${e}_{g}$ Hubbard models on the simple-cubic $3d$ lattice. It is also applied to study the spin-orbital order in the parent cubic structure of ternary chromium fluoride ${\mathrm{KCrF}}_{3}$. We obtain the onset of a G-type antiferro-orbital order at a significantly lower temperature compared to that in real distorted ${\mathrm{KCrF}}_{3}$. In contrast, its layered A-type antiferromagnetic order and N\'eel temperature are rather well reproduced. The calculated full Kugel-Khomskii Hamiltonian contains spin-orbital coupling terms inducing a misalignment in the antiferro-orbital order upon the onset of antiferromagnetism.