Comment on "Direct evidence for hidden one-dimensional Fermi surface of hexagonal K0.25WO3"

We comment a recent work titled "Direct evidence for hidden one-dimensional Fermi surface of hexagonal K0.25WO3". In this paper the authors report photoemission and theoretical results on the K0.25WO3 system which led them to propose that a Charge Density Wave (CDW), associated with hidden one-dimensional bands, was responsible for the well known resistivity anomaly in such system. In the present comment we report the results of a first principles density functional theory (DFT) study showing that there are no one-dimensional bands as suggested by these authors

Magnetism and Charge ordering in TMTTF2_2-PF6_6 organic crystals

Using a combination of Density Functional Theory, mean-field analysis and exact diagonalization calculations we reveal the emergence of a dimerized charge ordered state in TMTTF$_2$-PF$_6$ organic crystal. The interplay between charge and spin order leads to a rich phase diagram. Coexistence of charge ordering with a structural dimerization results in a ferroelectric phase, which has been observed experimentally. The tendency to the dimerization is magnetically driven revealing TMTTF$_2$-PF$_6$ as a multiferroic material

The Peierls instability and charge density wave in one-dimensional electronic conductors

AbstractWe review salient structural and electronic features associated with the concomitant Peierls–charge density wave (CDW) instabilities observed in most one-dimensional (1D) inorganic and organic electronic conductors. First of all, the genesis of these concepts is placed in an historical perspective. We then present basic experimental facts supporting the general description of these 1D electron–phonon coupled systems developed in the 1970s. In this framework we shall consider in particular the role of 1D fluctuations on both lattice and electronic degrees of freedom, and of the inter-chain Coulomb coupling between CDWs in stabilizing in 3D the Peierls transition at finite temperature. We also clarify, in relation with experimental findings, the various conditions of adiabaticity of the electron–phonon coupling. Finally we illustrate by recent structural measurements the pioneering work of Jacques Friedel on CDW elasticity and plasticity and CDW pinning to defects through the appearance of Friedel oscillations

Probing the Ionic Dielectric Constant Contribution in the Ferroelectric Phase of the Fabre-Salts

In strongly correlated organic materials it has been pointed out that charge-ordering could also achieve electronic ferroelectricity at the same critical temperature $T_{co}$. A prototype of such phenomenon are the quasi-one dimensional (TMTTF)$_2X$ Fabre-salts. However, the stabilization of a long-range ferroelectric ground-state below $T_{co}$ requires the break of inversion symmetry, which should be accompanied by a lattice deformation. In this work we investigate the role of the monovalent counter-anion $X$ in such mechanism. For this purpose, we measured the quasi-static dielectric constant along the $c^{*}$-axis direction, where layers formed by donors and anions alternate. Our findings show that the ionic charge contribution is three orders of magnitude lower than the intra-stack electronic response. The $c^{*}$ dielectric constant ($\epsilon'_{c^*}$) probes directly the charge response of the monovalent anion $X$, since the anion mobility in the structure should help to stabilize the ferroelectric ground-state. Furthermore, our $\epsilon'_{c^*}$ measurements %conjugated with earlier investigations of the $c^*$ lattice thermal expansion, show that the dielectric response is thermally broaden below $T_{co}$ if the ferroelectric transition occurs in the temperature range where the anion movement begin to freeze in their methyl groups cavity. In the extreme case of the PF$_6$-H$_{12}$ salt, where $T_{co}$ occurs at the freezing point, a relaxor-type ferroelectricity is observed. Also, because of the slow kinetics of the anion sub-lattice, global hysteresis effects and reduction of the charge response upon successive cycling are observed. In this context, we propose that anions control the order-disorder or relaxation character of the ferroelectric transition of the Fabre-salts.Comment: 8 pages, 7 figures. To appear in Physical Review

Donor-anion interactions in quarter-filled low-dimensional organic conductors

Anions have often been considered to act essentially as electron donors or acceptors in molecular conductors. However there is now growing evidence that they play an essential role in directing the structural and hence electronic properties of many of these systems. After reviewing the basic interactions and different ground states occurring in molecular conductors we consider in detail how anions influence the structure of donor stacks and often guide them toward different types of transitions. Consideration of the Bechgaard and Fabre salts illustrates how anions play a crucial role in directing these salts through complex phase diagrams where different conducting and localized states are in competition. We also emphasize the important role of hydrogen bonding and conformational flexibility of donors related to BEDT-TTF and we discuss how anions have frequently a strong control of the electronic landscape of these materials. Charge ordering, metal to metal and metal to insulator transitions occurring in these salts are considered

Anion ordering transition and Fermi surface electron-hole instabilities in the (TMTSF)2ClO4and (TMTSF)2NO3Bechgaard salts analyzed through the first-principles Lindhard response function

The first-principles electron-hole Lindhard response function has been calculated and analyzed in detail for two (TMTSF)2 X (X = ClO4 and NO3) Bechgaard salts undergoing different anion-ordering (AO) transitions. The calculation was carried out using the real triclinic low-temperature structures. The evolution of the electron-hole response with temperature for both relaxed and quenched salts is discussed. It is shown that the 2k F response of the quenched samples of both salts display a low temperature curved and tilted triangular continuum of maxima. This is not the case for the relaxed samples. (TMTSF)2ClO4 in the AO state exhibits a more quasi-1D response than in the non AO state and relaxed (TMTSF)2NO3 shows a sharp maximum. The curved triangular plateau of the quenched samples results from multiple nesting of the warped quasi-1D Fermi surface which implies the existence of a large q range of electron-hole fluctuations. This broad maxima region is around 1% of the Brillouin zone area for the X = ClO4 salt (and X = PF6) but only 0.1% for the X = NO3 salt. It is suggested that the strong reduction of associated SDW fluctuations could explain the non detection of the SDW-mediated superconductivity in (TMTSF)2NO3. The calculated maxima of the Lindhard response nicely account for the modulation wave vector experimentally determined by NMR in the SDW ground state of the two salts. The critical AO wave vector for both salts is located in regions where the Lindhard response is a minimum so that they are unrelated to any electron-hole instability. The present first-principles calculation reveals 3D effects in the Lindhard response of the two salts at low temperature which are considerably more difficult to model in analytical approaches

Fermi surface electron-hole instability of the (TMTSF)2PF6 Bechgaard salt revealed by the first-principles Lindhard response function

Altres ajuts: CERCA Programme/Generalitat de CatalunyaWe report the first-principles DFT calculation of the electron-hole Lindhard response function of the (TMTSF)PF Bechgaard salt using the real triclinic low-temperature structure. The Lindhard response is found to change considerably with temperature. Near the 2k spin density wave (SDW) instability it has the shape of a broad triangular plateau as a result of the multiple nesting associated with the warped quasi-one-dimensional Fermi surface. The evolution of the 2k broad maximum as well as the effect of pressure and deuteration is calculated and analyzed. The thermal dependence of the electron-hole coherence length deduced from these calculations compares very well with the experimental thermal evolution of the 2k bond order wave correlation length. The existence of a triangular plateau of maxima in the low-temperature electron-hole Lindhard response of (TMTSF)PF should favor a substantial mixing of q-dependent fluctuations which can have important consequences in understanding the phase diagram of the 2k SDW ground state, the mechanism of superconductivity and the magneto-transport of this paradigmatic quasi-one-dimensional material. The first-principles DFT Lindhard response provides a very accurate and unbiased approach to the low-temperature instabilities of (TMTSF)PF which can take into account in a simple way 3D effects and subtle structural variations, thus providing a very valuable tool in understanding the remarkable physics of molecular conductors