The electronic structure of the quasi-one-dimensional organic conductor TTF-TCNQ is studied by angle-resolved photoelectron spectroscopy (ARPES). The experimental spectra reveal significant discrepancies to band theory. We demonstrate that the measured dispersions can be consistently mapped onto the one-dimensional Hubbard model at finite doping. This interpretation is further supported by a remarkable transfer of spectral weight as function of temperature. The ARPES data thus show spectroscopic signatures of spin-charge separation on an energy scale of the conduction band width.
We study the electronic structure of the quasi-one-dimensional organic conductor TTF-TCNQ by means of density-functional band theory, Hubbard model calculations, and angle-resolved photoelectron spectroscopy (ARPES). The experimental spectra reveal s
ignificant quantitative and qualitative discrepancies to band theory. We demonstrate that the dispersive behavior as well as the temperature-dependence of the spectra can be consistently explained by the finite-energy physics of the one-dimensional Hubbard model at metallic doping. The model description can even be made quantitative, if one accounts for an enhanced hopping integral at the surface, most likely caused by a relaxation of the topmost molecular layer. Within this interpretation the ARPES data provide spectroscopic evidence for the existence of spin-charge separation on an energy scale of the conduction band width. The failure of the one-dimensional Hubbard model for the {it low-energy} spectral behavior is attributed to interchain coupling and the additional effect of electron-phonon interaction.
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 ch
arge-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.
We have measured the high field magnetoresistence and magnetization of quasi-one- dimensional (Q1D) organic conductor (Per)2Pt(mnt)2 (where Per = perylene and mnt = maleonitriledithiolate), which has a charge density wave (CDW) ground state at zero m
agnetic field below 8 K. We find that the CDW ground state is suppressed with moderate magnetic fields of order 20 T, as expected from a mean field theory treatment of Pauli effects[W. Dieterich and P. Fulde, Z. Physik 265, 239 - 243 (1973)]. At higher magnetic fields, a new, density wave state with sub-phases is observed in the range 20 to 50 T, which is reminiscent of the cascade of field induced, quantized, spin density wave phases (FISDW) observed in the Bechgaard salts. The new density wave state, which we tenatively identify as a field induced charge density wave state (FICDW), is re-entrant to a low resistance state at even higher fields, of order 50 T and above. Unlike the FISDW ground state, the FICDW state is only weakly orbital, and appears for all directions of magnetic field. Our findings are substantiated by electrical resistivity, magnetization, thermoelectric, and Hall measurements. We discuss our results in light of theoretical work involving magnetic field dependent Q1D CDW ground states in high magnetic fields [D. Zanchi, A. Bjelis, and G. Montambaux, Phys. Rev. B 53, (1996)1240; A. Lebed, JETP Lett. 78,138(2003)].
We have measured the Hall effect on recently synthesized single crystals of quasi-one-dimensional organic conductor TTF-TCNQ, a well known charge transfer complex that has two kinds of conductive stacks: the donor (TTF) and the acceptor (TCNQ) chains
. The measurements were performed in the temperature interval 30 K < T < 300 K and for several different magnetic field and current directions through the crystal. By applying the equivalent isotropic sample (EIS) approach, we have demonstrated the importance of the choice of optimal geometry for accurate Hall effect measurements. Our results show, contrary to past belief, that the Hall coefficient does not depend on the geometry of measurements and that the Hall coefficient value is around zero in high temperature region (T > 150 K), implying that there is no dominance of either TTF or TCNQ chain. At lower temperatures, our measurements clearly prove that all three phase transitions of TTF-TCNQ could be identified from Hall effect measurements.
The low temperature phase (LTP) of alpha-(BEDT-TTF)_2KHg(SCN)_4 salt is known for its surprising angular dependent magnetoresistance (ADMR), which has been studied intensively in the last decade. However, the nature of the LTP has not been understood
until now. Here we analyse theoretically ADMR in unconventional (or nodal) charge density wave (UCDW). In magnetic field the quasiparticle spectrum in UCDW is quantized, which gives rise to spectacular ADMR. The present model accounts for many striking features of ADMR data in alpha-(BEDT-TTF)_2KHg(SCN)_4.
R. Claessen
,M. Sing
,U. Schwingenschloegl
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(2002)
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"Spectroscopic signatures of spin-charge separation in the quasi-one-dimensional organic conductor TTF-TCNQ"
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Ralph Claessen
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