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

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)₂SbF₆ at different temperatures and (TMTTF)₂PF₆ under various hydrostatic 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 intersite Coulomb interaction, the magnetic order is only weakly enhanced. Both orders are suppressed when the effective pressure is increased.