Pattern of charge ordering in quasi-one-dimensional organic charge-transfer solids

We examine two recently proposed models of charge ordering (CO) in the nominally (formula presented)-filled, quasi-one-dimensional (1D) organic charge-transfer solids (CTS). The two models are characterized by site charge density “cartoons” (formula presented) and (formula presented) respectively. We use the Peierls-extended Hubbard model to incorporate both electron-electron (formula presented) and electron-phonon (formula presented) interactions. We first compare the results, for the purely electronic Hamiltonian, of exact many-body calculations with those of Hartree-Fock (HF) mean-field theory. We find that HF gives qualitatively and quantitatively incorrect values for the critical nearest-neighbor Coulomb repulsion (formula presented) necessary for (formula presented) order to become the ground state. Second, we establish that spin-Peierls order can occur in either the (formula presented) and (formula presented) states and calculate the phase diagram including both on-site and intrasite (formula presented) interactions. Third, we discuss the expected temperature dependence of the CO and metal-insulator transitions for both (formula presented) and (formula presented) CO states. Finally, we show that experimental observations clearly indicate the (formula presented) CO in the 1:2 anionic CTS and the (formula presented) materials, while the results for (formula presented) with narrower one-electron bandwidths are more ambiguous, likely because the nearest-neighbor Coulomb interaction in these materials is near (formula presented).