We investigate the effect of strong electronic correlation on the massless Dirac fermion system, $α$-(BEDT-TTF)$_2$I$_3$, under pressure. In this organic salt, one can control the electronic correlation by changing pressure and access the quantum critical point between the massless Dirac fermion phase and the charge ordering phase. We theoretically study the electronic structure of this system by applying the slave-rotor theory and find that the Fermi velocity decreases without creating a mass gap upon approaching the quantum critical point from the massless Dirac fermion phase. We show that the pressure-dependence of the Fermi velocity is in good quantitative agreement with the results of the experiment where the Fermi velocity is determined by the analysis of the Shubnikov-de Haas oscillations in the doped samples. Our result implies that the massless Dirac fermion system exhibits a quantum phase transition without creating a mass gap even in the presence of strong electronic correlations.
The effects of spin and charge fluctuations and electron-phonon couplings on charge ordering in α-(BEDT-TTF)_2I_3 (BEDT-TTF=bis(ethylenedithio)-tetrathiafulvalence) are investigated theoretically for an anisotropic triangular lattice at 3/4 filling. By the exact-diagonalization method, we have calculated the hole density distributions and the modulations of transfer integrals from high-temperature values as a function of electron-phonon coupling strength. The results clearly show that the lattice effect on α-(BEDT-TTF)_2I_3 is weak compared with that on θ-(BEDT-TTF)_2RbZn(SCN)_4, as previously…
We report the effect of Dirac cone tilting on interlayer magnetoresistance in α-(BEDT-TTF)$_2$I$_3$, which is a Dirac semimetal under pressure. Fitting of the experimental data by the theoretical formula suggests that the system is close to a type-II Dirac semimetal.
We compare the photoluminescence spectra of the low-temperature Mott insulator \etcl (T_{MIT}=40 K) with spectra of metallic κ-(BEDT-TTF)_2Cu[N(CN)_2]Br, which is superconducting below T_c=11.8 K, in the temperature range between 300 and 20 K. In the Mott insulating state of κ-(BEDT-TTF)_2Cu[N(CN)_2]Cl we observe a luminescence band at 1.95 eV due to the recombination of an exciton created by a HOMO-LUMO optical excitation. This luminescence is quenched both in the high-temperature bad metal state of κ-(BEDT-TTF)_2Cu[N(CN)_2]Cl and in metallic κ-(BEDT-TTF)_2Cu[N(CN)_2]Br. The observation of th…
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…
We investigated the interlayer magnetoresistance in an organic massless Dirac electron system $α$-(BEDT-TTF)$_2$I$_3$ under pressure. We experimentally demonstrate that the width of the zero mode owing to carrier scattering is much narrower than that of the other Landau levels.
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.
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 investigate the spin-orbit coupling (SOC) effects in $α$- and $κ$-phase BEDT-TTF and BEDT-TSF organic salts. Contrary to the assumption that SOC in organics is negligible due to light C, S, H atoms, we show the relevance of such an interaction in a few representative cases. In the weakly correlated regime, SOC manifests primarily in the opening of energy gaps at degenerate band touching points. This effect becomes especially important for Dirac semimetals such as $α$-(ET)$_2$I$_3$. Furthermore, in the magnetic insulating phase, SOC results in additional anisotropic exchange interactions, wh…
The organic salt $α$-(BEDT-TTF)$_2$I$_3$ is considered a model system for metal-insulator transition due to electronic charge ordering at $T_{\rm CO}=135$~K. The optical properties obtained from polarized reflection measurements above and below $T_{\rm CO}$ can be well described by calculations based on first-principle density-functional theory (DFT). We discuss the effect of electronic correlations on the metal-insulator transition.
Since the first observation of weak ferromagnetism in the charge-transfer salt kappa-(BEDT-TTF)2-Cu[N(CN)2]Cl [U. Welp et al., Phys. Rev. Lett. 69, 840 (1992)], no further evidence of ferromagnetism in this class of organic materials has been reported. Here we present static and dynamic spin susceptibility measurements on kappa-(BEDT-TTF)2Hg(SCN)2Br revealing weak ferromagnetism below about TWF = 20 K. We suggest that frustrated spins in the molecular dimers suppress long-range order, forming a spin-glass ground state in the insulating phase.
In spite of extensive experimental studies of the angular dependent magnetoresistance (ADMR) of the low temperature phase (LTP) of alpha-(BEDT-TTF)_2KHg(SCN)_4 about a decade ago, the nature of LTP remains elusive. Here we present a new study of ADMR of LTP in alpha-(ET)_2 salts assuming that LTP is unconventional charge density wave (UCDW). In the presence of magnetic field the quasiparticle spectrum in UCDW is quantized, which gives rise to striking ADMR in UCDW. The present model appears to account for many existing ADMR data of alpha-(BEDT-TTF)_2KHg(SCN)_4 remarkably well.
The low-temperature state of the quantum spin liquid candidate $κ$-(BEDT-TTF)$_{2}$Cu$_{2}$(CN)$_{3}$ emerges via an anomaly at $T^{*}\sim6$ K. Although signatures of this anomaly have been revealed in various quantities, its origin has remained unclear. Here we report inelastic neutron scattering measurements on single crystals of $κ$-(BEDT-TTF)$_{2}$Cu$_{2}$(CN)$_{3}$, aiming at studying phonon renormalization effects at $T^{*}$. A drastic change was observed in the phonon damping across $T^{*}$ for a breathing mode of BEDT-TTF dimers at $E=4.7$ meV. The abrupt change in the phonon damping i…
We examine the edge states of the Dirac electrons in the molecular material α-(BEDT-TTF)2I3 with electron-electron interactions. Based on the analysis of the extended Hubbard model with the Hartree-Fock approximation, we show that the charge-ordered phase has the gapless edge states only in the vicinity of the phase boundary between the zero-gap state and the charge-ordered phase. We also show a peculiar flux phase caused by the long-range Coulomb interaction with the same mechanism as topological Mott insulator phase.
The charge dynamics of spin-liquid states described by U(1) gauge theory coupling to fermionic spinons is discussed in this paper. We find that the gapless spinons give rise to a power law optical conductivity inside the charge gap. The theory is applied to explain the unusual optical conductivity observed recently in the organic compound $κ-(BEDT-TTF)_2Cu_2(CN)_3$. We also propose an optical experiment to search for the in-gap excitations in the Kagome spin liquid insulator.
K(BEDT-TTF)2Cu(NCS)2 has been investigated by Raman scattering in both bulk and nanoparticle compounds. Phonon modes from 20 to 1600 cm-1 have been assigned. Focusing on the unexplored low frequency phonons, a plateau in frequencies is observed in the bulk phonons between 50 and 100 K and assigned to the signature of the bad metal phase. Nanoparticles of K(BEDT-TTF)2Cu(NCS)2 exhibit anomalies at 50 K associated to the crossover from a bad metal to a Fermi liquid whose origins are discussed.
The spatial charge arrangement of a typical quasi-two-dimensional organic conductor alpha-(BEDT-TTF)2I3 is revealed by single crystal structure analysis using synchrotron radiation. The results show that the horizontal stripe type structure, which was suggested by mean field theory, is established. We also find the charge disproportion above the metal-insulator transition temperature and a significant change in transfer integrals caused by the phase transition. Our result elucidates the insulating phase of this material as a 2k_F charge density localization.
In most Dirac semimetals, time-reversal and inversion symmetries are believed to play a crucial role in their stability. We demonstrate that these symmetries are broken in Dirac fermions in the organic conductor $α$-(BEDT-TTF)$_2$I$_3$ due to the strong electronic correlation. The system is a three-dimensional type-II Dirac semimetal in the coherent inter-layer tunneling regime. A chiral anomaly is predicted to be observed in the magnetoresistance when the magnetic field is tuned to the inter-layer tunneling direction. Our result suggests that $α$-(BEDT-TTF)$_2$I$_3$ is a useful platform to ex…
The electronic properties of molecular conductors can be readily varied via physical or chemical pressure as it increases the bandwidth W; this enables crossing the Mott insulator-to-metal phase transition by reducing electronic correlations U/W. Here we introduce an alternative path by increasing the molecular orbitals when partially replacing sulfur by selenium in the constituting bis-(ethylenedithio)-tetrathiafulvalene (BEDT-TTF) molecules of the title compound. We characterize the tuning of the insulating quantum spin liquid state via a Mott transition to the metallic Fermi-liquid state by…
Recent experiments on the organic compound $κ-(BEDT-TTF)_2 Cu_2 (CN)_3$ raise the possibility that the system may be described as a quantum spin liquid. Here we propose a pairing state caused by the `Amperean' attractive interaction between spinons on a Fermi surface mediated by the U(1) gauge field. We show that this state can explain many of the observed low temperature phenomena and discuss testable consequences.
The electronic structure of weak charge-ordering (CO) state just below the critical pressure in an organic conductor α-(BEDT-TTF)_2I_3 was experimentally investigated using peak structure in the temperature dependence of interlayer magnetoresistance (MR). Based on a minimal model considering multiple Landau levels (LLs), we discuss herein the MR peak as characteristic to multilayer massless/massive Dirac fermion (DF) systems. MR measured in the weak CO state exhibited a clear MR peak, and its magnetic-field dependence was consistent with the LL behavior of a massive DF with a small gap. Result…
Recent experiments indicate that the spin-density waves (SDWs) in (TMTTF)_2Br, (TMTSF)_2PF_6 and alpha-(BEDT-TTF)_2MHg(SCN)_4 are highly unconventional and coexist with charge-density waves (CDWs). We present a microscopic theory of this unusual CDW-SDW coexistence. A complete understanding requires the explicit inclusion of strong Coulomb interactions, lattice discreteness, the anisotropic two-dimensional nature of the lattice, and the correct bandfilling within the starting Hamiltonian.
Theoretical and experimental studies have supported that the electronic structure of $α$-(BEDT-TTF)$_2$I$_3$ under pressure is described by two-dimensional Dirac fermions. When the interlayer tunneling is coherent, the electronic structure of the system becomes three-dimensional, and we expect the peak structure to appear in the interlayer resistivity under magnetic fields. We theoretically and experimentally show that the peak appears in the interlayer resistivity at low temperatures and high magnetic fields. From the experiment, we estimate that the magnitude of the interlayer tunneling is $…
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…
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…
We present ab initio two-dimensional extended Hubbard-type multiband models for EtMe_3Sb[Pd(dmit)_2]_2 and κ-(BEDT-TTF)_2Cu(NCS)_2, after a downfolding scheme based on the constrained random phase approximation (cRPA) and maximally-localized Wannier orbitals, together with the dimensional downfolding. In the Pd(dmit)_2 salt, the antibonding state of the highest occupied molecular orbital (HOMO) and the bonding/antibonding states of the lowest unoccupied molecular orbital (LUMO) are considered as the orbital degrees of freedom, while, in the κ-BEDT-TTF salt, the HOMO-antibonding/bonding states …
The critical cooling rate $R_{\rm c}$ above which charge ordering is kinetically avoided upon cooling, which results in charge-glass formation, was investigated for the geometrically frustrated system $θ$-(BEDT-TTF)$_2X$. X-ray diffraction experiments revealed that $θ$-(BEDT-TTF)$_2$TlCo(SCN)$_4$ exhibits a horizontally charge-ordered state, and kinetic avoidance of this state requires rapid cooling of faster than 150 K/min. This value is markedly higher than that reported for two other isostructural $θ$-type compounds, thus demonstrating the lower charge-glass-forming ability of $X$ $=$ TlCo(…
The Mott insulator κ-(BEDT-TTF)2Cu[N(CN)2]Cl consists of molecular dimers arranged on an anisotropic triangular lattice and develops a canted antiferromagnetic ground state. It has recently been suggested that this system features purely electronic ferroelectricity which requires an electric dipole moment. Optical spectroscopy clearly rules out charge imbalance in this system, which excludes the existence of quantum electric dipoles on the dimers and subsequently a dipolar spin coupling. We suggest that the prominent in-plane dielectric response in κ-(BEDT-TTF)2Cu[N(CN)2]Cl is due to short-ran…
Charge ordering phenomenon in $θ$-(BEDT-TTF)$_2$X is studied by using 1/4-filled extended Hubbard model on an anisotropic triangular lattice through mean-field approximation. It is found that a metallic charge ordered state with 3-periodicity on lattices (3-fold type charge order) is realized in the realistic parameter region where the nearest neighbor Coulomb interaction V$_{ij}$ is nearly isotropic. This 3-fold state survives up to high temperatures by estimating the free energy. Insulating state with diagonal or vertical-type charge ordering appears as increasing anisotropy of V$_{ij}$. Con…
We have measured details of the quasi one-dimensional Fermi-surface sections in the organic superconductor kappa-(BEDT-TTF)_2 Cu(NCS)_2 and its deuterated analogue using angle-dependent millimetre-wave techniques. There are significant differences in the corrugations of the Fermi surfaces in the deuterated and undeuterated salts. We suggest that this is important in understanding the inverse isotope effect, where the superconducting transition temperature rises on deuteration. The data support models for superconductivity which invoke electron-electron interactions depending on the topological…
The organic conductor $κ$-(BEDT-TTF)$_2$Cu$_2$(CN)$_{3}$ seems to form a quantum spin liquid, although at low temperatures unusual properties are seen in the charge, spin and lattice degrees of freedom. Here we report results of X-band ESR studies of $κ$-(BEDT-TTF)$_2$Cu$_2$(CN)$_{3}$ single crystals as a function of temperature and angle. We find indications of two anisotropic relaxation mechanisms at low temperatures and compare them to the spin-liquid behavior observed in other strongly correlated systems. In addition, we can recognize charge inhomogeneities in the copper ions of the anion …
In order to understand the physical properties of the series of organic conductors $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]$X$ with $X$ = Cl, Br, and I, not only electronic correlations but also the effect of disorder has to be taken into account. While for Cl- and Br-containing salts the influence of both parameters were investigated and a universal phase diagram was proposed, the position of $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]I is still not settled. Here we have conducted transport, infrared, and dielectric measurements on single crystals of the title compound to clarify its electronic state at low tempe…
We report the band structure calculations and the experimental results of resistivity and magnetic susceptibility in a spin-1/2 (BEDT-TTF)$^{\bullet +}$ monomer Mott insulator (BEDT-TTF)Cu[N(CN)$_2$]$_2$. The band calculations indicate a Dirac semimetal state with nodal lines at the Fermi level. The resistivity and the magnetic susceptibility as functions of temperature are well interpreted in terms of the monomer Mott insulating state instead of the expected semimetal state probably owing to strong electron correlation. In addition, we find that an Arrhenius-type steep reduction of the parama…
The charge-ordered insulator $α$-(BEDT-TTF)$_2$I$_3$ gradually evolves to a metal when pressure is applied, and at low temperatures the electronic bands form tilted Dirac-like cones. A metallic state with a frequency-independent optical conductivity indicates the coexistence of the trivial and massless Dirac electrons in the system. Our infrared investigations also reveal that at the boundary between insulating and metallic states an energy gap opens due to correlated massive Dirac fermions, which is gradually suppressed when pressure increases.
We have measured and analyzed the dielectric constant of the dimer Mott insulator $κ-$(BEDT-TTF)$_2$Cu$_2$(CN)$_3$, which is known as a playground for a spin-liquid state. Most unexpectedly, this particular organic salt has nontrivial charge degrees of freedom, being characterized by a dipole-glass-like dielectric relaxation below around 60 K. This is ascribed to the charge disproportionation within the dimer due to the intersite Coulomb repulsion. In this respect, the dipole observed here is purely quantum mechanical, and thereby exhibits unexpected responses.
The quasiparticle scattering rates in high-quality crystals of the quasi-two-dimensional superconductor $κ$-(BEDT-TTF)$_2$Cu(NCS)$_2$ ~are studied using the Shubnikov-de Haas effect and MHz penetration-depth experiments. There is strong evidence that the broadening of the Landau-levels is primarily caused by spatial inhomogeneities, indicating a quasiparticle lifetime for the Landau states $\gg 3$ ps. In contrast to the predictions of Fermi-liquid theory, the scattering time derived from the intralayer conductivity is found to be much shorter ($0.14-0.56$ ps).
We consider the millimeter-wave electrodynamics specific to quasi-two-dimensional conductors and superconductors based on the organic donor molecule BEDT-TTF. Using realistic physical parameters, we examine the current polarizations that result for different oscillating (GHz) electric and magnetic field polarizations. We show that, in general, it is possible to discriminate between effects (dissipation and dispersion) due to in-plane and interlayer ac currents. However, we also show that it is not possible to selectively probe any single component of the in-plane conductivity tensor, and that …
The ground state of $λ$-(BEDT-TTF)$_2$GaCl$_4$, which has the same structure as the organic superconductor $λ$-(BETS)$_2$GaCl$_4$, was investigated by magnetic susceptibility and $^{13}$C NMR measurements. The temperature dependence of the magnetic susceptibility revealed an antiferromagnetic (AF) correlation with $J/k_{\rm B} \simeq$ 98 K. NMR spectrum splitting and the divergence of $1/T_1$ were observed at approximately 13 K, which is associated with the AF transition. We found that the AF structure is commensurate according to discrete NMR peak splitting, suggesting that the ground state o…
Combined effects of electron correlations and lattice distortions are investigated on the charge ordering in θ-(BEDT-TTF)2RbZn(SCN)4 theoretically in a two-dimensional 3/4-filled extended Hubbard model with electron-lattice couplings. It is known that this material undergoes a phase transition from a high-symmetry metallic state to a low-symmetry insulating state with a horizontal-stripe charge order (CO) by lowering temperature. By means of the exact-diagonalization method, we show that electron-phonon interactions are crucial to stabilize the horizontal-stripe CO and to realize the low-symme…
By applying measurements of the dielectric constants and relative length changes to the dimerized molecular conductor $κ$-(BEDT-TTF)$_2$Hg(SCN)$_2$Cl, we provide evidence for order-disorder type electronic ferroelectricity which is driven by charge order within the (BEDT-TTF)$_2$ dimers and stabilized by a coupling to the anions. According to our density functional theory calculations, this material is characterized by a moderate strength of dimerization. This system thus bridges the gap between strongly dimerized materials, often approximated as dimer-Mott systems at 1/2 filling, and non- or …
We formulate a U(1) gauge theory of the Hubbard model in the slave-rotor representation. From this formalism it is argued that spin liquid phases may exist near the Mott transition in the Hubbard model on triangular and honeycomb lattices at half filling. The organic compound k-(BEDT-TTF)_2 Cu_2 (CN)_3 is a good candidate for the spin liquid state on a triangular lattice. We predict a highly unusual temperature dependence for the thermal conductivity of this material.
The origin of the spin gap behavior in the low-temperature dimerized phase of theta-(BEDT-TTF)_2RbZn(SCN)_4 has been theoretically studied based on the Hartree-Fock approximation for the on-site Coulomb interaction at absolute zero. Calculations show that, in the parameter region considered to be relevant to this compound, antiferromagnetic ordering is stabilized between dimers consisting of pairs of molecules coupled with the largest transfer integral. Based on this result an effective localized spin 1/2 model is constructed which indicates the existence of the frustration among spins. This f…
Photoinduced melting of horizontal-stripe charge orders in quasi-two-dimensional organic conductors θ-(BEDT-TTF)2RbZn(SCN)4[BEDT-TTF=bis(ethylenedithio)tetrathiafulvalene] and α-(BEDT-TTF)2I3 is investigated theoretically. By numerically solving the time-dependent Schrödinger 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 θ-(BEDT-TTF)2RbZn(SCN)4 than for α-(BEDT-TTF)2I3, which is a consequence of the larger stabilization energy in θ-(B…
The pressure dependence of the interlayer magnetoresistance of the quasi-two dimensional organic metal beta''-(BEDT-TTF)4(NH4)[Fe(C2O4)3].DMF has been investigated up to 1 GPa in pulsed magnetic fields up to 55 T. The Shubnikov-de Haas oscillations spectra can be interpreted on the basis of three compensated orbits in all the pressure range studied, suggesting that the Fermi surface topology remains qualitatively the same as the applied pressure varies. In addition, all the observed frequencies, normalized to their value at ambient pressure, exhibit the same sizeable pressure dependence. Despi…
We interpret the optical spectra of $α$-(BEDT-TTF)$_2M$Hg(SCN)$_4$ (M=NH$_4$ and Rb) in terms of a 1/4 filled metallic system close to charge ordering and show that in the conductivity spectra of these compounds a fraction of the spectral weight is shifted from the Drude-peak to higher frequencies due to strong electronic correlations. Analyzing the temperature dependence of the electronic parameters, we distinguish between different aspects of the influence of electronic correlations on optical properties. We conclude, that the correlation effects are slightly weaker in the NH$_4$ compound co…
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…
The emergence of photo-induced topological phases and their phase transitions are theoretically predicted in organic salt $α$-(BEDT-TTF)$_2$I$_3$, which possesses inclined Dirac cones in its band structure. By analyzing a photo-driven tight-binding model describing conduction electrons in the BEDT-TTF layer using the Floquet theorem, we demonstrate that irradiation with circularly polarized light opens a gap at the Dirac points, and the system eventually becomes a Chern insulator characterized by a quantized topological invariant. A rich phase diagram is obtained in plane of amplitude and freq…
The charge response of charge-ordered state in the organic conductor alpha-(BEDT-TTF)2I3 is characterized by dc resistivity, dielectric and optical spectroscopy in different crystallographic directions within the two-dimensional conduction layer. Two dielectric modes are detected. The large mode is related to the phason-like excitation of the 2kF bond-charge density wave which forms in the ab plane. The small dielectric mode is associated with the motion of domain-wall pairs along the a- and b-axes between two types of domains which are created due to inversion symmetry breaking.
The dimer Mott insulator $κ$-(BEDT-TTF)$_2$Cu$_2$(CN)$_3$ exhibits unusual electrodynamic properties. Numerical investigations of the electronic ground state and the molecular and lattice vibrations reveal the importance of the Cu$_2$(CN)$_3^-$ anion network coupled to the BEDT-TTF molecules: The threefold cyanide coordination of copper and linkage isomerism in the anion structure cause a loss of symmetry, frustration, disorder, and domain formation. Our findings consistently explain the temperature and polarization-dependent THz and infrared measurements, reinforce the understanding of dielec…
De Haas-van Alphen oscillations are studied for Fermi surfaces illustrating the Pippard's model, commonly observed in multiband organic metals. Field- and temperature-dependent amplitude of the various Fourier components, linked to frequency combinations arising from magnetic breakdown between different bands, are considered. Emphasis is put on the Onsager phase factor of these components. It is demonstrated that, in addition to the usual Maslov index, field-dependent phase factors must be considered to precisely account for the data at high magnetic field. We present compelling evidence of th…
We show that Shubnikov-de Haas oscillations in the interlayer resistivity of the organic superconductor $β''$-(BEDT-TTF)$_{2}$SF$_{5}$ CH$_{2}$CF$_{2}$SO$_{3}$ become very pronounced in magnetic fields $\sim$~60~T. The conductivity minima exhibit thermally-activated behaviour that can be explained simply by the presence of a Landau gap, with the quasi-one-dimensional Fermi surface sheets contributing negligibly to the conductivity. This observation, together with complete suppression of chemical potential oscillations, is consistent with an incommensurate nesting instability of the quasi-one-d…
Temperature-driven metal-insulator and pressure-driven insulator-metal transitions observed in(BEDT-TTF)8[Hg4X12(C6H5Y)2]] with X = Y = Br are studied through band structure calculations based on X-ray crystal structure determination and Shubnikov-de Haas (SdH) oscillations spectra, respectively. In connection with chemical pressure effect, the transition, which is not observed for X = Cl, is due to gap opening linked to structural changes as the temperature decreases. Even though many body interactions can be inferred from the pressure dependence of the SdH oscillations spectra, all the data …
Within the framework of the density functional theory, we calculate the electronic structure of $α$-(BEDT-TTF)$_2$I$_3$ at 8K and room temperature at ambient pressure and with uniaxial strain along the $a$- and $b$-axes. We confirm the existence of anisotropic Dirac cone dispersion near the chemical potential. We also extract the orthogonal tight-binding parameters to analyze physical properties. An investigation of the electronic structure near the chemical potential clarifies that effects of uniaxial strain along the a-axis is different from that along the b-axis. The carrier densities show …
We present a theoretical study on the superconductivity in β'-(BEDT-TTF)_2ICl_2 at Tc=14.2K under high hydrostatic pressure found by Taniguchi et al., which is the highest record among organic superconductors. Its electronic structure is well expressed by the anisotropic triangular lattice Hubbard model at half filling. In the present work, we study this effective model by using the fluctuation-exchange (FLEX) approximation. In the obtained phase diagram, the superconductivity with d_{x^2-y^2} like symmetry is realized next to the antiferromagnetic (AF) insulating phase, as a result of the 1D-…
In the field of interacting electron systems the Mott metal-to-insulator (MI) transition represents one of the pivotal issues. The role played by lattice degrees of freedom for the Mott MI transition and the Mott criticality in a variety of materials are current topics under debate. In this context, molecular conductors of the $κ$-(BEDT-TTF)$_2$X type constitute a class of materials for unraveling several aspects of the Mott physics. In this review, we present a synopsis of literature results with focus on recent expansivity measurements probing the Mott MI transition in this class of material…
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 determine the pressure dependence of the electron-phonon coupling in $κ$-(BEDT-TTF)$_{2}$Cu(SCN)$_{2}$ by comparison of high pressure Raman scattering and high pressure infrared (IR) reflectivity measurements. The Raman active molecular vibrations of the BEDT-TTF dimers stiffen by 0.1-1 %GPa$^{-1}$. In contrast, the corresponding modes in the IR spectrum are observed at lower frequency, with a pressure dependence of 0.5-5.5 %GPa$^{-1}$, due to the influence of the electron-phonon interaction. Both dimer charge-oscillation and phase-phonon models are employed to extract the pressure dependen…
We investigate theoretically charge ordered states on the anisotropic triangular lattice characteristic of the theta-(BEDT-TTF)_2 X materials. Using exact diagonalization studies, we establish that the charge order (CO) pattern corresponds to a ``horizontal'' stripe structure, with ...1100... CO along the two directions with larger electron hopping (p-directions), and ...1010... CO along the third direction (c-direction). The CO is accompanied by co-operative bond dimerizations along all three directions in the highest spin state. In the lowest spin state bonds along the p-directions are tetra…
Pairing symmetry in $κ$-(BEDT-TTF)$_2$X is re-examined by applying fluctuation exchange method to the Hubbard model on the original four band lattice for the first time. Our study is motivated by the discrepancy between a recent thermal conductivity/tunneling spectroscopy experiments and the previous theories based on the effective single or two band model. In contrast to the previous theories, we find that $d_{x^2-y^2}$-like pairing dominates over $d_{xy}$ in agreement with recent experiments. Our study provides a general lesson that even if the Fermi surface seems to be reproduced by an effe…
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…
Successive magnetic-field-induced charge-density-wave transitions in the molecular conductor $α$-(BEDT-TTF)$_2$KHg(SCN)$_4$ are studied in the hydrostatic pressure regime, in which the zero field charge-density wave (CDW)state is completely suppressed. The orbital effect of the magnetic field is demonstrated to restore the density wave, while the orbital quantization induces different CDW states in different field intervals. In particular, we have found that at certain field orientations the hysteretic first order transitions between field-induced CDW subphases become visible at much higher te…
