Mean-field study of charge order with long periodicity in $\theta$-(BEDT-TTF)$_2$X

TL;DR

This study uses a mean-field approach to explore charge order phenomena in $ heta$-(BEDT-TTF)$_2$X, revealing how different charge order patterns emerge depending on Coulomb interactions and structural distortions, aligning with experimental observations.

Contribution

It provides a theoretical phase diagram showing the stability of various charge-ordered states in $ heta$-(BEDT-TTF)$_2$X based on extended Hubbard model calculations.

Findings

3-fold charge order state is stable with isotropic Coulomb interactions.

Horizontal charge order stabilizes with structural distortion at low temperatures.

Multiple charge-ordered states compete in $ heta$-(BEDT-TTF)$_2$CsZn(SCN)$_4$, suggesting inhomogeneous phases.

Abstract

Charge ordering phenomenon in $\theta$-(BEDT-TTF)$_2$X is studied by using 1/4-filled extended Hubbard model on an anisotropic triangular lattice through mean-field approximation. It is found that a metallic charge ordered state with 3-periodicity on lattices (3-fold type charge order) is realized in the realistic parameter region where the nearest neighbor Coulomb interaction V$_{ij}$ is nearly isotropic. This 3-fold state survives up to high temperatures by estimating the free energy. Insulating state with diagonal or vertical-type charge ordering appears as increasing anisotropy of V$_{ij}$. Considering the effect of the structural distortion observed in $\theta$-(BEDT-TTF)$_2$RbZn(SCN)$_4$ at low temperatures, horizontal-type charge ordered insulating phase tends to be stabilized and the region where 3-fold type exists becomes narrower. Our results are consistent with the metallic state with long periodic charge order which can be related to 3-fold type in $\theta$-(BEDT-TTF)$_2$RbZn(SCN)$_4$ at high temperatures and insulating state with horizontal charge order at low temperatures. For $\theta$-(BEDT-TTF)$_2$CsZn(SCN)$_4$, we speculate several kinds of charge-ordered states are energetically competing with each other leading to an inhomogeneous state at low temperatures.