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Register a new userConduction anisotropy and Hall effect in the organic conductor (TMTTF)2AsF6: evidence for Luttinger liquid and charge ordering
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We present the high-temperature (70 K < T < 300 K) resistivity anisotropy and Hall effect measurements of the quasi-one-dimensional (1D) organic conductor (TMTTF)2AsF6. The temperature variations of the resistivity are pronouncedly different for the three different directions, with metallic-like at high temperatures for the a-axis only. Above 220 K the Hall coefficient R_H is constant, positive and strongly enhanced over the expected value; and the corresponding carrier concentration is almost 100 times lower than calculated for one hole/unit cell. Our results give evidence for the existence of a high-temperature regime above 200 K where the 1D Luttinger liquid features appear in the transport properties. Our measurements also give strong evidence of charge ordering in (TMTTF)2AsF6. At the charge-ordering transition T_{CO} approx 100 K, R_H(T) abruptly changes its behavior, switches sign and rapidly increases with further temperature decrease.
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Long missing basic experiments in the normal phase of the anisotropic electron system of TMTSF2PF6 were performed. Both the Hall effect and the ab-plane conduction anisotropy are directly addressing the unconventional electrical properties of this Bechgaard salt. We found that the dramatic reduction of the carrier density deduced from recent optical data is not reflected in an enhanced Hall-resistance. The pressure- and temperature dependence of the b-direction resitivity reveal isotropic relaxation time and do not require explanations beyond the Fermi liquid theory. Our results allow a coherent-diffusive transition in the interchain carrier propagation, however the possible crossover to Luttinger liquid behavior is placed to an energy scale above room temperature.
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.
(TMTTF)2AsF6 undergoes two phase transitions upon cooling from 300 K. At Tco=103 K a charge-ordering (CO) occurs, and at Tsp(B=9 T)=11 K the material undergoes a spin-Peierls (SP) transition. Within the intermediate, CO phase, the charge disproportionation ratio is found to be at least 3:1 from carbon-13 NMR 1/T1 measurements on spin-labeled samples. Above Tsp, up to about 3Tsp, 1/T1 is independent of temperature, indicative of low-dimensional magnetic correlations. With the application of about 0.15 GPa pressure, Tsp increases substantially, while Tco is rapidly suppressed, demonstrating that the two orders are competing. The experiments are compared to results obtained from calculations on the 1D extended Peierls-Hubbard model.
The quasi-one-dimensional organic conductors (TMTTF)$_2X$ with non-centrosymmetric anions commonly undergo charge- and anion-order transitions upon cooling. While for compounds with tetrahedral anions ($X$ = BF$_4^-$, ReO$_4^-$, and ClO$_4^-$) the charge-ordered phase is rather well understood, the situation is less clear in the case of planar triangular anions, such as (TMTTF)$_2$NO$_3$. Here we explore the electronic and structural transitions by transport experiments, optical and magnetic spectroscopy. This way we analyze the temperature dependence of the charge imbalance 2$delta$ and an activated behavior of $rho(T)$ with $Delta_{rm CO}approx 530$~K below $T_{rm CO} = 250$~K. Since (TMTTF)$_2$NO$_3$ follows the universal relation between charge imbalance 2$delta$ and size of the gap $Delta_{rm CO}$, our findings suggest that charge order is determined by TMTTF stacks with little influence of the anions. Clear signatures of anion ordering are detected at $T_{rm AO}=50$~K. The tetramerization affects the dc transport, the vibrational features of donors and acceptors, and leads to formation of spin singlets.
High-resolution thermal expansion measurements have been performed for exploring the mysterious structureless transition in (TMTTF)$_{2}$X (X = PF$_{6}$ and AsF$_{6}$), where charge ordering at $T_{CO}$ coincides with the onset of ferroelectric order. Particularly distinct lattice effects are found at $T_{CO}$ in the uniaxial expansivity along the interstack $textbf{textit{c*}}$-direction. We propose a scheme involving a charge modulation along the TMTTF stacks and its coupling to displacements of the counteranions X$^{-}$. These anion shifts, which lift the inversion symmetry enabling ferroelectric order to develop, determine the 3D charge pattern without ambiguity. Evidence is found for another anomaly for both materials at $T_{int}$ $simeq$ 0.6 $cdot$ $T_{CO}$ indicative of a phase transition related to the charge ordering.
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