An ab-initio evaluation of the local effective interactions in the $\rm Na_{x} Co O_2$ familly

TL;DR

This study uses ab initio quantum chemical methods to evaluate effective Hubbard and $t-J$ model parameters in Na$_x$CoO$_2$, revealing how electronic correlations and magnetic interactions vary with sodium content and structural distortions.

Contribution

It provides the first ab initio determination of effective parameters for Na$_x$CoO$_2$, highlighting the evolution of correlation strength and magnetic interactions with composition.

Findings

The $a_{1g}$ orbitals are above the $e_g^ extprime$ orbitals by a few hundred meV.

Correlation strength increases with sodium content $x$.

Pure CoO$_2$ is close to a Mott transition with $U/t \\sim 15$.

Abstract

We used quantum chemical ab initio methods to determine the effective parameters of Hubbard and $t-J$ models for the $\rm Na_{x}CoO_2$ compounds (x=0 and 0.5). As for the superconducting compound we found the $a_{1g}$ cobalt orbitals above the $e_g^\prime$ ones by a few hundreds of meV due to the $e_g^\prime$--$e_g$ hybridization of the cobalt $3d$ orbitals. The correlation strength was found to increase with the sodium content $x$ while the in-plane AFM coupling decreases. The less correlated system was found to be the pure $CoO_2$, however it is still strongly correlated and very close to the Mott transition. Indeed we found $U/t\sim 15$, which is the critical value for the Mott transition in a triangular lattice. Finally, one finds the magnetic exchanges in the $\rm CoO_2$ layers, strongly dependant of the weak local structural distortions.