Effects of Electron–Lattice Coupling on Charge Order in θ-(ET)₂X

Abstract

Charge ordering accompanied by lattice distortion in quasi-two dimensional organic conductors θ-(ET)₂X (ET = BEDT-TTF) is studied by using an extended Hubbard model with Peierls-type electron–lattice couplings within the Hartree–Fock approximation. It is found that the horizontal-stripe charge-ordered state, which is experimentally observed in θ-(ET)₂RbZn(SCN)₄, is stabilized by the self-consistently determined lattice distortion. Furthermore, in the presence of the anisotropy in nearest-neighbor Coulomb interactions V_ij, the horizontal charge order becomes more stable than any other charge patterns such as diagonal, vertical and 3-fold-type states. At finite temperatures, we compare the free energies of various charge-ordered states and find a first-order transition from a metallic state with 3-fold charge order to the insulating state with the horizontal charge order. The role of lattice degrees of freedom in the realization of the horizontal charge order and the relevance to experiments on θ-(ET)₂X are discussed.