Electronic properties of Fabre charge-transfer salts under various temperature and pressure conditions

Abstract

Using density functional theory, we determine parameters of tight-binding Hamiltonians for a variety of Fabre charge transfer salts, focusing in particular on the effects of temperature and pressure. Besides relying on previously published crystal structures, we experimentally determine two new sets of structures; (TMTTF)$_2$SbF$_6$ at different temperatures and (TMTTF)$_2$PF$_6$ at various pressures. We find that a few trends in the electronic behavior can be connected to the complex phase diagram shown by these materials. Decreasing temperature and increasing pressure cause the systems to become more two-dimensional. We analyze the importance of correlations by considering an extended Hubbard model parameterized using Wannier orbital overlaps and show that while charge order is strongly activated by the inter-site Coulomb interaction, the magnetic order is only weakly enhanced. Both orders are suppressed when the effective pressure is increased.