Low-dimensional organic conductors could establish themselves as model systems for the investigation of the physics in reduced dimensions. In the metallic state of a one-dimensional solid, Fermi-liquid theory breaks down and spin and charge degrees of freedom become separated. But the metallic phase is not stable in one dimension: as the temperature is reduced, the electronic charge and spin tend to arrange themselves in an ordered fashion due to strong correlations. The competition of the different interactions is responsible for which broken-symmetry ground state is eventually realized in a specific compound and which drives the system towards an insulating state.
Here we review the various ordering phenomena and how they can be identified by optic and magnetic measurements. While the final results might look very similar in the case of a charge density wave and a charge-ordered metal, for instance, the physical cause is completely different. When density waves form, a gap opens in the density of states at the Fermi energy due to nesting of the one-dimension Fermi surface sheets. When a one-dimensional metal becomes a charge-ordered Mott insulator, on the other hand, the short-range Coulomb repulsion localizes the charge on the lattice sites and even causes certain charge patterns.
We try to point out the similarities and conceptional differences of these phenomena and give an example for each of them. Particular emphasis will be put on collective phenomena which are inherently present as soon as ordering breaks the symmetry of the system.
It is known that the ground states of organic conductors have a diversity reflecting the spatial arrangement of the constituent molecules within the unit cell. A systematic theoretical search for the unifying view behind such possible ground states has been made based on the Hartree-Fock mean field approximation not only to the on-site but also to intersite Coulomb interactions with special emphasis on the families of typical organic conductors (TMTCF)$_2X$ and (ET)$_2X$.
We present experimental evidences for a ferro-electric transition in the family of quasi one- dimensional conductors (TMTTF)2X. We interpret this new transition in the frame of the combined Mott-Hubbard state taking into account the double action of the spontaneous charge disproportionation on the TMTTF molecular stacks and of the X anionic potentials.
Even though organic conductors have complicated crystalline structure with low symmetry and large unit cell, band structure calculations predict multiband quasi-two dimensional electronic structure yielding very simple Fermi surface in most cases. Although few puzzling experimental results are observed, data of numerous compounds are in agreement with calculations which make them suitable systems for studying magnetic quantum oscillations in networks of orbits connected by magnetic breakdown. The state of the art of this problematics is reviewed.
We study the Mott transition, antiferromagnetism and superconductivity in layered organic conductors using Cellular Dynamical Mean Field Theory for the frustrated Hubbard model. A d-wave superconducting phase appears between an antiferromagnetic insulator and a metal for $t^{\prime}/t=0.3-0.7 $, or between a nonmagnetic Mott insulator (spin liquid) and a metal for $t^{\prime}/t\geq 0.8$, in agreement with experiments on layered organic conductors including $κ$-(ET)$_{2}$Cu$_{2}$(CN)$_{3}$. These phases are separated by a strong first order transition. The phase diagram gives much insight into …
We present systematic magnetic torque studies of the ``magnetic field - temperature'' phase diagram of the layered organic conductor alpha-(BEDT-TTF)2KHg(SCN)4 at fields nearly perpendicular and nearly parallel to the highly conducting plane. The shape of the phase diagram is compared to that predicted for a charge-density-wave system in a broad field range.
We demonstrate a new method for determining the Fermi velocity in quasi-two-dimensional (Q2D) organic conductors. Application of a magnetic field parallel to the conducting layers results in periodic open orbit quasiparticle trajectories along the Q2D Fermi surface. Averaging of this motion over the Fermi surface leads to a resonance in the interlayer microwave conductivity. The resonance frequency is simply related to the extremal value of the Fermi velocity perpendicular to the applied field. Thus, angle dependent microwave studies enable a complete mapping of the Fermi velocity. We illustra…
On the basis of an analysis of a 3/4-filled two-dimensional (2D) extended Hubbard model under the fluctuation-exchange approximation, we find Coulomb frustrated phase separation (PS) in a region of nonzero temperature, where the quantum critical phenomenon of charge ordering (CO) dominates. In quasi-2D organic conductors on the verge of CO, this frustrated PS provides a mechanism for generating spatial inhomogeneity, which is characterized by an extremely slow relaxation and an intermediate length scale.
This is a broad reviw of some of the fundamental results of research on the Bechgaard salts.To a lesser extent Q2D salts will also be discussed.Apart from known results,based on the author's work and the literature,some open problems will also be presented.
Using the bosonization technique, which separates charge and spin degrees of freedom, we study a possibility of formation of the holon edge states in a one-dimensional electron system with an energy gap in the charge sector. The results are applied to the quasi-one-dimensional organic conductors (TMTTF)2X. The different roles of the bond and site dimerizations in this material are discussed. We predict that the holon edge states should appear below the temperature of the recently discovered ferroelectric transition, where the inorganic anions X displace to asymmetric positions.
We have investigated the magnetic field-induced metal-insulator transition in the tau-phase organic conductors, which occurs in fields above 35 T, and below 14 K, by magnetization, thermoelectric, and pressure dependent transport methods. Our results show that the transition is a bulk thermodynamic process where a magnetic field-dependent gap opens upon entry into the insulating state. We argue that the transition involves a magnetic field-induced change in the electronic structure.
Although the topological phases are difficult to be realized in organic molecular crystals, we demonstrate here that they can emerge in the τ-type organic layered conductors, τ-(EDO-S,S-DMEDT-TTF)_2X_{1+y} and τ-(P-S,S-DMEDT-TTF)_2X_{1+y} (X=AuBr_2, I_3, IBr_2), where EDO-S,S-DMEDT-TTF and P-S,S-DMEDT-TTF denote the planar donor molecules ethylenedioxy-S,S-dimethyl(ethylenedithio)tetrathiafulvalene and pyrazino-S,S-dimethyl(ethylenedithio)tetrathiafulvalene, respectively. The conducting layers of these conductors have a highly symmetric checkerboard structure, which can be regarded as a modifi…
We investigated the effect of magnetic field on the highly correlated metal near the Mott transition in the quasi-two-dimensional layered organic conductor, $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Cl, by the resistance measurements under control of temperature, pressure, and magnetic field. It was demonstrated that the marginal metallic phase near the Mott transition is susceptible to the field-induced localization transition of the first order, as was predicted theoretically. The thermodynamic consideration of the present results gives a conceptual pressure-field phase diagram of the Mott transiti…
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.
Measurements and calculations of magnetotransport in the molecular organic conductor (DMET)2I3 detect and simulate all known angular magnetoresistance oscillation (AMRO) phenomena for quasi-one dimensional (Q1D) systems. Employing the true triclinic crystal structure in the calculations, these results address the mystery of the putative vanishing of the primary AMRO phenomenon, the Lebed magic angle effect, for orientations in which it was expected to be strongest. They also show a common origin for Lebed and so-called "LN" oscillations, and confirm the generalized nature of AMRO in Q1D system…
We investigate the metallic transport in the organic superconductor (TMTSF)2PF6 under pressure within the framework of the spin density wave theory in the proximity of a Peierls quantum critical point (QCP). We use a simple transport model of hot and cold regions around the Fermi surface, driven by the proximity to the QCP in order to provide a template to fit the experimental results. Successful agreement with the data comforts the interpretation of extended criticality around the antiferromagnetic QCP in the normal phase of quasi one-dimensional organic superconductors.
We report inter-plane ($R_{zz}$) electrical transport measurements in the \tp series of organic conductors at very high magnetic fields. In the field range between 36 and 60 T $R_{zz}$ shows a very hysteretic first order phase transition from metallic to an insulating state. This transition does not affect the Shubnikov-de-Haas oscillations associated with the two-dimensional (2D) Fermi surface. We argue that this transition originates from inter-plane disorder which gives rise to incoherent transport along the least conducting axis. We conclude that this system becomes a strictly 2D Fermi-liq…
The magnetic susceptibility of the quarter-filled one-dimensional extended Hubbard model is calculated using the density-matrix renormalization group technique. It is found that in the charge gap regime of the model ($U> 4t $ and $V > 2t$), or in the metallic region with important superconductive fluctuations ($U<4t$ and $V>2t$), $χ(T)$ displays a singularity at T=0 and an inflection point at low temperatures that are similar to what occurs in the spin-half quantum spin chain. These results, whose accuracy outdoes that of any other available technique, are useful data which allow a comparison …
The temperature dependences of the Hall coefficient and electrical resistivity recently measured by Moser et al. [Phys. Rev. Lett. 84, 2674 (2000)] in the quasi-one-dimensional organic conductor (TMTSF)2PF6 are quantitatively compared with our previous theoretical calculations [Synth. Met. 103, 2202 (1999); Eur. Phys. J. B 11, 385 (1999)]. We find a good agreement, albeit not with a fully consistent set of parameters for the two quantities, without appealing to the Luttinger liquid concept.
The angle-resolved photoemission spectrum of the organic conductor TTF-TCNQ exhibits an unusual transfer of spectral weight over a wide energy range for temperatures 60K<T<260K. In order to investigate the origin of this finding, here we report numerical results on the single-particle spectral weight A(k,omega) for the one-dimensional (1D) Hubbard model and, in addition, for the 1D extended Hubbard and the 1D Hubbard-Holstein models. Comparisons with the photoemission data suggest that the 1D Hubbard model is not sufficient for explaining the unusual T dependence, and the long-range part of th…
Close to the Mott transition, lattice degrees of freedom react to the softening of electron degrees of freedom. This results in a change of lattice spacing, a diverging compressibility and a critical anomaly of the sound velocity. These effects are investigated within a simple model, in the framework of dynamical mean-field theory. The results compare favorably to recent experiments on the layered organic κ-(BEDT-TTF)_2Cu[N(CN)_2]Cl conductor . We predict that effects of a similar magnitude are expected for V2O3, despite the much larger value of the elastic modulus of this material.
This is a review of some aspects of theoretical studies of the Bechgaard salts,which also retraces the evolution of the author's interest in the field.It discusses the calculation of the condutivity,attempts at gaining some knowledge on the EOS and thermal properties of these materials,as well as some ideas on the possible future developement of the field.
Shubnikov-de Haas and angular dependent magnetoresistance oscillations have been used to explore the role of anion size, magnetic moment, and disorder in the organic conductors kappa-(BETS)_2GaBr_{4} and kappa-(BETS)_2FeCl_{2}_Br_{2} in the isomorphic class kappa-(BETS)_2Ga_{1-x}Fe_{x}Cl_{4-y}_Br_{y}. The results, combined with previous work, show correlations between the anion composition (Ga_{1-x}Fe_{x}Cl_{4-y}_Br_{y}) and the superconducting transition temperature, effective mass, Fermi surface topology, and the mean free path.
We have demonstrated transient charge localization effects with a driving high-frequency field of 7-fs, 1.5-cycle near infrared light in correlated organic conductors. In a layered organic conductor alpha-(BEDT-TTF)2I3 (BEDT-TTF: bis[ethylenedithio]-tetrathiafulvalene), a transient short-range charge order (CO) state is induced in a metallic phase. In contrast to such drastic change in the electronic state from the metal to the transient CO in alpha-(BEDT-TTF)2I3, dynamics of a field-induced reduction of a transfer integral are captured as a red shift of the plasma-like reflectivity edge in a …
We present a scenario for the peculiar coexistence of charge fluctuations observed in quasi-2D 1/4-filled organic conductors $θ$-(BEDT-TTF)$_2X$ in the quantum critical regime where the charge ordering is suppressed down to zero temperature. The scenario is explored in the extended Hubbard model including electron-phonon couplings on an anisotropic triangular lattice. We find that the coexisting fluctuations emerge from two different instabilities, the ``Wigner crystallization on lattice'' driven by the off-site Coulomb repulsion and the charge-density-wave formation due to the nesting of the …
We theoretically discuss the mechanism for the peculiar nonlinear conduction in quasi-two-dimensional organic conductors θ-(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, wherea…
This chapter reviews the effects of interactions in quasi-one dimensional systems, such as the Bechgaard and Fabre salts, and in particular the Luttinger liquid physics. It discusses in details how transport measurements both d.c. and a.c. allow to probe such a physics. It also examine the dimensional crossover and deconfinement transition occurring between the one dimensional case and the higher dimensional one resulting from the hopping of electrons between chains in the quasi-one dimensional structure.
The interlayer magnetoresistance of the low-dimensional organic metal α-(BEDT-TTF)2KHg(SCN)4 under pressure shows features which are likely associated with theoretically predicted field-induced charge-density-wave (FICDW) transitions. At ambient pressure, a magnetic field strongly tilted towards the conducting layers induces a series of hysteretic anomalies. We attribute these anomalies to a novel kind of FICDW originating from a superposition of the orbital quantization of the nesting vector and Pauli effect on the charge-density wave.
Confinement-deconfinement transition in quarter-filled two-coupled chains comprising dimerization, repulsive interactions and interchain hopping has been demonstrated by applying the renormalization group method to the bosonized Hamiltonian. The confinement given by the irrelevant interchain hopping occurs with increasing umklapp scattering which is induced by the dimerization leading to effectively half-filling. It is shown that the transition originates in a competition between a charge gap and the renormalized interchain hopping.
To verify the effect of geometrical frustration, we artificially distort the triangular lattice of quasi-two-dimensional organic conductor $κ$-(BEDT-TTF)$_2$Cu$_2$(CN)$_3$ [BEDT-TTF: bis(ethylenedithio)terathiofulvalene] by analogous-molecular substitution and apply $^{13}$C NMR of bulk and substituted sites, electric conductivity, and static magnetic susceptibility measurements. The results indicate that the magnetic characteristics of the substituted sample are quantitatively similar to those of the pure sample. Moreover the magnetic characteristics at the substituted sites are also the same…
A complex study of magnetic properties including dc magnetization, 1H NMR and magnetic torque measurements has been performed for the organic conductor kappa-(BETS)2Mn[N(CN)2]3 which undergoes a metal-insulator transition at T_MI~25K. NMR and the magnetization data indicate a transition in the manganese subsystem from paramagnetic to a frozen state at T_MI, which is, however, not a simple Neel type order. Further, a magnetic field induced transition resembling a spin flop has been detected in the torque measurements at temperatures below T_MI. This transition is most likely related to the spin…
An inductive method is used to follow the magnetic field-dependent susceptibility of the coupled charge density wave (CDW) and spin-Peierls (SP) ordered state behavior in the dual chain organic conductor Perylene$_2$[Pt(mnt)$_2$]. In addition to the coexisting SP-CDW state phase below 8 K and 20 T, the measurements show that a second spin-gapped phase appears above 20 T that coincides with a field-induced insulating phase. The results support a strong coupling of the CDW and SP order parameters even in high magnetic fields, and provide new insight into the nature of the magnetic susceptibility…
We study the continuous bandwidth-controlled Mott transition in the two-dimensional single-band Hubbard model with a focus on the critical scaling behavior of charge and spin degrees of freedom. Using plaquette cluster dynamical mean-field theory, we find charge and spin criticality consistent with experimental results for organic conductors. In particular, the charge degree of freedom measured via the local density of states at the Fermi level shows a smoother transition than expected for the Ising universality class and in single-site dynamical mean-field theory, revealing the importance of …
Superconductivity of quasi-one-dimensional organic conductors with a quarter-filled band is investigated using the two-loop renormalization group approach to the extended Hubbard model for which both the single electron hopping t_{\perp} and the repulsive interaction V_{\perp} perpendicular to the chains are included. For a four-patches Fermi surface with deviations to perfect nesting, we calculate the response functions for the dominant fluctuations and possible superconducting states. By increasing V_{\perp}, it is shown that a d-wave (singlet) to f-wave (triplet) superconducting state cross…
We study the Hall effect in a system of weakly coupled Luttinger Liquid chains, using a Memory function approach to compute the Hall constant in the presence of umklapp scattering along the chains. In this approximation, the Hall constant decomposes into two terms: a high-frequency term and a Memory function term. For the case of zero umklapp scattering, where the Memory function vanishes, the Hall constant is simply the band value, in agreement with former results in a similar model with no dissipation along the chains. With umklapp scattering along the chains, we find a power-law temperature…
Angle dependent magnetoresistance experiments on organic conductors exhibit a wide range of angular oscillations associated with the dimensionality and symmetry of the crystal structure and electron energy dispersion. In particular, characteristics associated with 1, 2, and 3 dimensional electronic motion are separately revealed when a sample is rotated through different crystal planes in a magnetic field. Originally discovered in the TMTSF based conductors, these effects are particularly pronounced in the related system (DMET)2I3. Here, experimental and computational results for magnetoresist…
The d-wave pairing correlations along with spin correlation are calculated with quantum Monte Carlo method for the two-dimensional Hubbard model on lattice structures representing organic superconductors $κ$-(BEDT-TTF)$_2$X and (TMTSF)$_2$X. In both cases the pairing correlations for superconducting order parameters with nodes are found to be enhanced. The symmetry and the enhancement of the pairing is systematically correlated with the spin structure factor, suggesting a spin-fluctuation mediated pairing. We have further found that, as we deform the Fermi surface to make the system approach t…
We derive effective Hubbard-type Hamiltonians of $κ$-(ET)$_2X$, using an {\em ab initio} downfolding technique, for the first time for organic conductors. They contain dispersions of the highest occupied Wannier-type molecular orbitals with the nearest neighbor transfer $t$$\sim$0.067 eV for a metal $X$=Cu(NCS)$_2$ and 0.055 eV for a Mott insulator $X$=Cu$_2$(CN)$_3$, as well as screened Coulomb interactions. It shows unexpected differences from the conventional extended Hückel results, especially much stronger onsite interaction $U$$\sim$0.8 eV ($U/t$$\sim$12-15) than the Hückel estimates ($U…
The quasi-two-dimensional organic semiconductor α-(BEDT-TTF)2I3 [BEDT-TTF=bis(ethylenedithio)tetrathiafulvalene] has an anisotropic linear dispersion with a zero energy gap near the Fermi level. Owing to the vanishing density of states at the Fermi level, the Coulomb interaction is unscreened in this material. We theoretically study the effect of the long-range Coulomb interaction and the low-energy/long-wavelength behavior of α-(BEDT-TTF)2I3 using the renormalization group analysis. The nearly logarithmic enhancement of the velocity reshapes tilted Dirac cones, and changes the low-temperature…
Phase-change memory (PCM), a promising candidate for next-generation non-volatile memories, exploits quenched glassy and thermodynamically stable crystalline states as reversibly switchable state variables. We demonstrate PCM functions emerging from a charge-configuration degree of freedom in strongly correlated electron systems. Non-volatile reversible switching between a high-resistivity charge-crystalline (or charge-ordered) state and a low-resistivity quenched state, charge glass, is achieved experimentally via heat pulses supplied by optical or electrical means in organic conductors $θ$-(…
We investigate the formation of density waves in the zero-gap state (ZGS) which has been found in the quasi-two-dimensional organic conductor $α$-(BEDT-TTF)$_2$I$_3$ salt under the hydrostatic pressure. The ZGS exhibits the cone-like dispersion for both the conduction band and the valence band which degenerate each other at the two-dimensional wave vectors, $\pm\mib{k}_0$ forming a zero gap. By using the extended Hubbard model with repulsive interaction we calculate the onset temperature of the spin density wave (SDW) as a function of the interlayer electron hopping, which by itself does not b…
We theoretically investigate charge order and nonlinear conduction in a quasi-two-dimensional organic conductor β-(meso-DMBEDT-TTF)2PF6 [DMBEDT-TTF=dimethylbis(ethylenedithio)tetrathiafulvalene]. Within the Hartree-Fock approximation, we study effects of structural distortion on the experimentally observed checkerboard charge order and its bias-induced melting by using an extended Hubbard model with Peierls- and Holstein-types of electron-lattice interactions. The structural distortion is important in realizing the charge order. The current-voltage characteristics obtained by a nonequilibrium …
Magnetic properties of the conduction pi-electron system of kappa-BETS)2Mn[N(CN)2]3 have been probed using 13C NMR. At ambient pressure, the metal-insulator transition observed in the resistivity measurements below T~23K is shown to be accompanied by ordering of the pi-spins in a long-range staggered structure. As the metal-insulator transition is suppressed by applying a small pressure of ~0.5 kbar, the pi-spin system maintains the properties of the metallic state down to 5K.
The magnetic structure of antiferromagnetically ordered phases of quasi-one-dimensional organic conductors is studied theoretically at absolute zero based on the mean field approximation to the quarter-filled band with on-site and nearest-neighbor Coulomb interaction. The differences in magnetic properties between the antiferromagnetic phase of (TMTTF)$_2$X and the spin density wave phase in (TMTSF)$_2$X are seen to be due to a varying degrees of roles played by the on-site Coulomb interaction. The nearest-neighbor Coulomb interaction introduces charge disproportionation, which has the same sp…
We reconsider the theory of dc and ac interchain conductivity in quasi-one dimensional systems. Our results are in good agreement with the measured c-axis optical conductivity of (TMTSF)_2{ClO}_4 and suggest that the c-axis dc-conductivity of (TMTSF)_2{PF}_6 in the 150K < T < 300Kd$ range is dominated by precursor effects of Mott localization. The crossover from a Luttinger liquid at high energy to a Fermi liquid at low energy is also addressed, within a dynamical mean-field theory. Implications for the inter-chain resistivity and Drude weight in the Fermi liquid regime are discussed.
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.
An organic Mott insulator, $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Cl, was investigated by resistance measurements under continuously controllable He gas pressure. The first-order Mott transition was demonstrated by observation of clear jump in the resistance variation against pressure. Its critical endpoint at 38 K is featured by vanishing of the resistive jump and critical divergence in pressure derivative of resistance, $|\frac{1}{R}\frac{\partial R}{\partial P}|$, which are consistent with the prediction of the dynamical mean field theory and have phenomenological correspondence with the liquid…
We study the magnetic-field-induced spin-density-wave (FISDW) phases in TMTSF organic conductors in the framework of the quantized nesting model. In agreement with recent suggestions, we find that the SDW wave-vector ${\bf Q}$ deviates from its quantized value near the transition temperature $T_c$ for all phases with quantum numbers $N>0$. Deviations from quantization are more pronounced at low pressure and higher $N$ and may lead to a suppression of the first-order transitions $N+1\to N$ for $N\ge 5$. Below a critical pressure, we find that the N=0 phase invades the entire phase diagram in ac…
A $^{13}$C NMR study of the normal and superconducting states of the all-organic charge-transfer salt $β"$-(BEDT-TTF)$_2$SF$_5$CH$_2$CF$_2$SO$_3$ is presented. We find that the normal state is a charge-ordered metal configured as vertical stripes, produced by a combination of 1/4-filling, correlations, and a polar counterion sublattice. The NMR properties associated with the superconducting state are consistent with gap nodes and singlet pairing, and therefore similar to other organic superconductors. Quite distinct, however, is the absence of evidence for low-energy antiferromagnetic spin flu…
Discontinuous changes of the lattice parameters at the Mott metal-insulator transition are detected by high-resolution dilatometry on deuterated crystals of the layered organic conductor $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Br. The uniaxial expansivities uncover a striking and unexpected anisotropy, notably a zero-effect along the in-plane c-axis along which the electronic interactions are relatively strong. A huge thermal expansion anomaly is observed near the end-point of the first-order transition line enabling to explore the critical behavior with very high sensitivity. The analysis yields c…
The organic charge-transfer salt $κ$-(BEDT-TTF)$_{2}$Hg(SCN)$_{2}$Br is a quasi two-dimensional metal with a half-filled conduction band at ambient conditions. When cooled below $T=80$ K it undergoes a pronounced transition to an insulating phase where the resistivity increases many orders of magnitude. In order to elucidate the nature of this metal-insulator transition we have performed comprehensive transport, dielectric and optical investigations. The findings are compared with other dimerized $κ$-(BEDT-TTF) salts, in particular the Cl-analogue, where a charge-order transition takes place a…
Dynamical localization, i.e., reduction of the intersite electronic transfer integral t by an alternating electric field, E(omega) , is a promising strategy for controlling strongly correlated systems with a competing energy balance between t and the Coulomb repulsion energy. Here we describe a charge localization induced by the 9.3 MV/cm instantaneous electric field of a 1.5 cycle (7 fs) infrared pulse in an organic conductor alpha-(bis[ethylenedithio]-tetrathiafulvelene)_2I_3. A large reflectivity change of > 25% and a coherent charge oscillation along the time axis reflect the opening of th…
Magnetooptical measurements of several quasi-two-dimensional (q2D) organic conductors, which have simple Fermi surface structure, have been performed by using a cavity perturbation technique. Despite of the simple Fermi surface structure, magnetooptical resonance results show a dramatic difference for each sample. Cyclotron resonances (CR) were observed for q-(BEDT-TTF)2I3 and (BEDT-TTF)3Br(pBIB), while periodic orbit resonances (POR) were observed for (BEDT-TTF)2Br(DIA) and (BEDT-TTF)3Cl(DFBIB). The selection of the resonance seems to correspond with the skin depth for each sample. The effect…
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 o…
In order to investigate charge ordering phenomena under electric field, static nonequilibrium Hartree approximation (SNHA) method is formulated on the basis of the nonequilibrium Green's functions introduced by Keldysh. By applying the SNHA to the 3/4-filling extended Hubbard model on anisotropic triangular lattice, we study the stabilities and amplitudes of 3-fold and horizontal charge orders in $θ$ and $θ_d$-(BEDT-TTF)$_2X$ salts under the electric field. The obtained results show that the electric field stabilizes the 3-fold state in comparison to the horizontal state. The amplitude of the …
The electronic properties of quarter-filled organic materials showing spin-Peierls transition are investigated theoretically. By studying the one-dimensional extended Peierls-Hubbard model analytically as well as numerically, we find that there is a competition between two different spin-Peierls states due to the tetramized lattice distortion in the strongly correlated regime. One is accompanied by lattice dimerization which can be interpreted as a spontaneous Mott insulator, while the other shows the existence of charge order of Wigner crystal-type. Results of numerical density matrix renorma…
We present a systematic investigation of the low-frequency charge carrier dynamics in different charge states of the organic conductors $θ$-(BEDT-TTF)$_2$$M$Zn(SCN)$_4$ with $M$=Rb,Tl, which result from quenching or relaxing the charge degrees of freedom on a geometrically frustrated triangular lattice. Due to strong electronic correlations these materials exhibit a charge-ordering transition, which can be kinetically avoided by rapid cooling resulting in a so-called charge-glass state without long-range order. The combination of fluctuation spectroscopy and a heat pulse method allows us to st…
We study the charge ordering (CO) in the one-dimensional (1D) extended Hubbard model at quarter filling where the nearest-neighbor Coulomb repulsion and dimerization in the hopping parameters are included. Using the cluster mean-field approximation to take into account the effect of quantum fluctuations, we determine the CO phase boundary of the model in the parameter space at T=0 K. We thus find that the dimerization suppresses the stability of the CO phase strongly, and in consequence, the realistic parameter values for quasi-1D organic materials such as (TMTTF)$_2$PF$_6$ are outside the reg…
The effects of electron correlation in the quasi-two-dimensional organic conductor α-(BEDT-TTF)2I3 are investigated theoretically by using an extended Hubbard model with on-site and nearest-neighbor Coulomb interactions. A variational Monte Carlo method is applied to study its ground-state properties. We show that there appears a nonmagnetic horizontal-stripe charge order in which nearest-neighbor correlation functions indicate a tendency toward a spin-singlet formation on the bonds with large transfer integrals along the charge-rich stripe. Under uniaxial pressure, a first-order transition fr…
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 cohe…