Nonlinear Conduction by Melting of Stripe-Type Charge Order in Organic Conductors with Triangular Lattices

We theoretically discuss the mechanism for the peculiar nonlinear conduction in quasi-two-dimensional organic conductors \theta-(BEDT-TTF)2X [BEDT-TTF=bis(ethylenedithio)tetrathiafulvalene] through the melting of stripe-type charge order. An extended Peierls-Hubbard model attached to metallic electrodes is investigated by a nonequilibrium Green's function technique. A novel current-voltage characteristic appears in a coexistent state of stripe-type and nonstripe 3-fold charge orders, where the applied bias melts mainly the stripe-type charge order through the reduction of lattice distortion, whereas the 3-fold charge order survives. These contrastive responses of the two different charge orders are consistent with the experimental observations.Comment: 5 pages, 4 figures, to appear in J. Phys. Soc. Jp

Multi-Orbital Molecular Compound (TTM-TTP)I_3: Effective Model and Fragment Decomposition

The electronic structure of the molecular compound (TTM-TTP)I_3, which exhibits a peculiar intra-molecular charge ordering, has been studied using multi-configuration ab initio calculations. First we derive an effective Hubbard-type model based on the molecular orbitals (MOs) of TTM-TTP; we set up a two-orbital Hamiltonian for the two MOs near the Fermi energy and determine its full parameters: the transfer integrals, the Coulomb and exchange interactions. The tight-binding band structure obtained from these transfer integrals is consistent with the result of the direct band calculation based on density functional theory. Then, by decomposing the frontier MOs into two parts, i.e., fragments, we find that the stacked TTM-TTP molecules can be described by a two-leg ladder model, while the inter-fragment Coulomb energies are scaled to the inverse of their distances. This result indicates that the fragment picture that we proposed earlier [M.-L. Bonnet et al.: J. Chem. Phys. 132 (2010) 214705] successfully describes the low-energy properties of this compound.Comment: 5 pages, 4 figures, published versio

The Origin of the Charge Ordering and Its Relevance to Superconductivity in θ\theta-(BEDT-TTF)2_2X: The Effect of the Fermi Surface Nesting and the Distant Electron-Electron Interactions

The origin of the charge ordering in organic compounds $\theta$-(BEDT-TTF)$_2 X$ ($X=MM'$(SCN)$_4$, $M=$Tl,Rb,Co, $M'=$Cs,Zn) is studied using an extended Hubbard model. Calculating the charge susceptibility within random phase approximation (RPA), we find that the $(3\times 3)\sim (3\times 4)$ charge ordering observed at relatively high temperatures can be considered as a consequence of a cooperation between the Fermi surface nesting, controlled by the hopping integral in the $c$ direction, and the electron-electron interactions, where the distant (next nearest neighbor) interactions that have not been taken into account in most of the previous studies play an important role.Mean field analysis at T=0 also supports the RPA results, and further shows that in the $3\times 3$ charge ordered state, some portions of the Fermi surface remain ungapped and are nested with a nesting vector close to the modulation wave vector of the horizontal stripe ordering observed at low temperatures in $X=MM'$(SCN)$_4$. We further study the possibility of superconductivity by taking into account the distant off-site repulsions and the band structure corresponding to $X=$I$_3$, in which superconductivity is experimentally observed. We find that there is a close competition between $d_{xy}$-wave-like singlet pairing and $p_{x+2y}$-wave-like triplet pairing due to a cooperation between the charge and the spin fluctuations. The present analysis provides a possible unified understanding of the experimental phase diagram of the $\theta$-(BEDT-TTF)$_2 X$ family, ranging from a charge ordered insulator to a superconductor.Comment: 13 pages, 18 figures (Figs.5,6,7,14,15,18 compressed using jpeg2ps

Growth Dynamics of Photoinduced Domains in Two-Dimensional Charge-Ordered Conductors Depending on Stabilization Mechanisms

Photoinduced melting of horizontal-stripe charge orders in quasi-two-dimensional organic conductors \theta-(BEDT-TTF)2RbZn(SCN)4[BEDT-TTF=bis(ethylenedithio)tetrathiafulvalene] and \alpha-(BEDT-TTF)2I3 is investigated theoretically. By numerically solving the time-dependent Schr\"odinger equation, we study the photoinduced dynamics in extended Peierls-Hubbard models on anisotropic triangular lattices within the Hartree-Fock approximation. The melting of the charge order needs more energy for \theta-(BEDT-TTF)2RbZn(SCN)4 than for \alpha-(BEDT-TTF)2I3, which is a consequence of the larger stabilization energy in \theta-(BEDT-TTF)2RbZn(SCN)4. After local photoexcitation in the charge ordered states, the growth of a photoinduced domain shows anisotropy. In \theta-(BEDT-TTF)2RbZn(SCN)4, the domain hardly expands to the direction perpendicular to the horizontal-stripes. This is because all the molecules on the hole-rich stripe are rotated in one direction and those on the hole-poor stripe in the other direction. They modulate horizontally connected transfer integrals homogeneously, stabilizing the charge order stripe by stripe. In \alpha-(BEDT-TTF)2I3, lattice distortions locally stabilize the charge order so that it is easily weakened by local photoexcitation. The photoinduced domain indeed expands in the plane. These results are consistent with recent observation by femtosecond reflection spectroscopy.Comment: 9 pages, 8 figures, to appear in J. Phys. Soc. Jpn. Vol. 79 (2010) No.

Charge Order with Structural Distortion in Organic Conductors: Comparison between \theta-(ET)2RbZn(SCN)4 and \alpha-(ET)2I3

Charge ordering with structural distortion in quasi-two-dimensional organic conductors \theta-(ET)2RbZn(SCN)4 (ET=BEDT-TTF) and \alpha-(ET)2I3 is investigated theoretically. By using the Hartree-Fock approximation for an extended Hubbard model which includes both on-site and intersite Coulomb interactions together with Peierls-type electron-lattice couplings, we examine the role of lattice degrees of freedom on charge order. It is found that the experimentally observed, horizontal charge order is stabilized by lattice distortion in both compounds. In particular, the lattice effect is crucial to the realization of the charge order in \theta-(ET)2RbZn(SCN)4, while the peculiar band structure whose symmetry is lower than that of \theta-(ET)2RbZn(SCN)4 in the metallic phase is also an important factor in \alpha-(ET)2I3 together with the lattice distortion. For \alpha-(ET)2I3, we obtain a phase transition from a charge-disproportionated metallic phase to the horizontal charge order with lattice modulations, which is consistent with the latest X-ray experimental result.Comment: 10 pages, 13 figures, to appear in J. Phys. Soc. Jpn. Vol. 77 (2008) No.

Theory of the beta-type Organic Superconductivity under Uniaxial Compression

We study theoretically the shift of the superconducting transition temperature (Tc) under uniaxial compression in beta-type organic superconductors, beta-(BEDT-TTF)2I3 and beta-(BDA-TTP)2X[X=SbF6,AsF6], in order to clarify the electron correlation, the spin frustration and the effect of dimerization. The transfer integrals are calculated by the extended Huckel method assuming the uniaxial strain and the superconducting state mediated by the spin fluctuation is solved using Eliashberg's equation with the fluctuation-exchange approximation. The calculation is carried out on both the dimerized (one-band) and nondimerized (two-band) Hubbard models. We have found that (i) the behavior of Tc in beta-(BEDT-TTF)2I3 with a stronger dimerization is well reproduced by the dimer model, while that in weakly dimerized beta-BDA-TTP salts is rather well reproduced by the two-band model, and (ii) the competition between the spin frustration and the effect induced by the fluctuation is important in these materials, which causes nonmonotonic shift of Tc against uniaxial compression.Comment: 18 pages, 16 figures, 2 tabl