The magnetic field effect on the phase diagram of the organic Mott system $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Br in which the bandwidth was tuned by the substitution of deuterated molecules was studied by means of the resistivity measurements performed in magnetic fields. The lower critical point of the first-order Mott transition, which ended on the upper critical field $H_{\rm c2}$-temperature plane of the superconductivity, was determined experimentally in addition to the previously observed upper critical end point. The lower critical end point moved to a lower temperature with the suppression of $T_{\rm c}$ in magnetic fields and the Mott transition recognized so far as the $S$-shaped curve reached $T =$ 0 when $H > H_{\rm c2}$ in the end.
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-…
Systematic investigation of the electronic phase separation on macroscopic scale is reported in the organic Mott system $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Br. Real space imaging of the phase separation is obtained by means of scanning micro-region infrared spectroscopy using the synchrotron radiation. The phase separation appears near the Mott boundary and changes its metal-insulator fraction with the substitution ratio $x$ in $κ$-[($h$-BEDT-TTF)$_{1-x}$($d$-BEDT-TTF)$_{x}$]$_{2}$Cu[N(CN)$_{2}$]Br, of which band width is controlled by the substitution ratio $x$ between the hydrogenated BEDT-TT…
Low temperature scanning tunneling spectroscopy reveals the local density of states of the organic superconductor $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Br, that was cut in-situ in ultra-high vacuum perpendicular to the superconducting BEDT-TTF layers. The spectra confirm that superconductivity is confined to the conducting BEDT-TTF layers, while the Cu[N(CN)$_2$]Br anion layers are insulating. The density of states comprises a twofold superconducting gap, which is attributed to the two separated bands crossing the Fermi surface.
Utilizing infrared vibrational spectroscopy we have investigated dimerized two-dimensional organic salts in order to search for possible charge redistribution that might cause electronic dipoles and ferroelectricity: the quantum spin liquid κ-(BEDT-TTF)2Cu2(CN)3, the antiferromagnetic Mott insulator κ-(BEDT-TTF)2$Cu[N(CN)2]Cl, and the superconductor κ-(BEDT-TTF)2$Cu[N(CN)2]Br. None of them exhibit any indication of charge disproportionation upon cooling down to low temperatures. No modification in the charge distribution is observed around T = 6 K where a low-temperature anomaly has been repor…
We report measurements of the de Haas-van Alphen (DHVA) effect and AC susceptibility in the layered organic superconductor $κ$-(BEDT-TTF)$_{2}$Cu(NCS)$_{2}$. The amplitude of the DHVA oscillations is attenuated over a wide field range above the irreversibility line, B_irr(B), below which a rigid flux lattice is formed. Thus the DHVA effect provides a unique probe of the superconducting fluctuations at high fields in this material. We compare our measurements with other determinations of the superconducting phase diagram of $κ$-(BEDT-TTF)$_{2}$Cu(NCS)$_{2}$.
Raman and IR spectra of k-(BEDT-TTF)_2Cu[N(CN)_2]Br [BEDT-TTF denotes bis(ethylenedithiolo)tetrathiafulvalene] and its deuterated and partially deuterated analogues were measured at temperatures between 5 and 300 K and cooling rates from 1 to 20 K/min. It was found that, in partially deuterated samples, the interdimer electron-molecular vibration splitting of nu_3 mode in Raman spectra, the magnitude of the resonance enhancement in Raman spectra, and linewidths of some phonon peaks both in Raman and infrared spectra depend on the cooling rate. These observations were explained by disorder-rela…
We investigate the superconductivity in the deuterated BEDT-TTF molecular substitution system $κ$-[(h8-BEDT-TTF)$_{1-x}$(d8-BEDT-TTF)$_x$]$_2$Cu[N(CN)$_2$]Br, where h8 and d8 denote fully hydrogenated and deuterated molecules, respectively. Systematic and wide range ($x$ = 0 -- 1) substitution can control chemical pressure finely near the Mott boundary, which results in the modification of the superconductivity. After cooling slowly, the increase of $T_{\textrm{c}}$ observed up to $x \sim$ 0.1 is evidently caused by the chemical pressure effect. Neither reduction of $T_{\textrm{c}}$ nor suppre…
Electronic phase separation consisting of the metallic and insulating domains with 50 -- 100 $μ$m in diameter is found in the organic Mott system $κ$-[($h$8-BEDT-TTF)$_{1-x}$($d$8-BEDT-TTF)$_{x}$]$_{2}$Cu[N(CN)$_{2}$]Br by means of scanning micro-region infrared spectroscopy using the synchrotron radiation. The phase separation appears below the critical end temperature 35 -- 40 K of the first order Mott transition. The observation of the macroscopic size of the domains indicates a different class of the intrinsic electronic inhomogeneity from the nano-scale one reported in the inorganic Mott …
In the most studied family of organic superconductors kappa-(BEDT-TTF)_2X, the BEDT-TTF molecules that make up the conducting planes are coupled as dimers. For some anions X, an antiferromagnetic insulator is found at low temperatures adjacent to superconductivity. With an average of one hole carrier per dimer, the BEDT-TTF band is effectively 1/2-filled. Numerous theories have suggested that fluctuations of the magnetic order can drive superconducting pairing in these models, even as direct calculations of superconducting pairing in monomer 1/2-filled band models find no superconductivity. He…
Infrared reflection measurements of the half-filled two-dimensional organic conductors $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_{2}$]Br$_{x}$Cl$_{1-x}$ were performed as a function of temperature ($5 {\rm K}<T<300$ K) and Br-substitution ($x=0%$, 40%, 73%, 85%, and 90%) in order to study the metal-insulator transition. We can distinguish absorption processes due to itinerant and localized charge carriers. The broad mid-infrared absorption has two contributions: transitions between the two Hubbard bands and intradimer excitations from the charges localized on the (BEDT-TTF)$_2$ dimer. Since the latter coupl…
The polarized optical reflectance spectra of the quasi two dimensional organic correlated electron system $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]$Y$, $Y =$ Br and Cl are measured in the infrared region. The former shows the superconductivity at $T_{\rm c} \simeq$ 11.6 K and the latter does the antiferromagnetic insulator transition at $T_{\rm N} \simeq$ 28 K. Both the specific molecular vibration mode $ν_{3}(a_{g})$ of the BEDT-TTF molecule and the optical conductivity hump in the mid-infrared region change correlatively at $T^{*} \simeq$ 38 K of $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Br, although no …
The far-infrared in-plane reflectivity of the organic superconductor $α_t$-(BEDT-TTF)$_{2}$I$_{3}$ is measured down to frequencies of 10 cm$^{-1}$; the optical conductivity is obtained by a Kramers-Kronig procedure. In the superconducting state an energy gap opens at 25 cm$^{-1}$ which corresponds to $2Δ/k_BT_c = 4.4$ in agreement with moderate coupling. Even well below $T_c=8$ K a considerable absorption remains for $\hbarω<2Δ$. We discuss different posibilities to explain this behaviour.
The effect of disorder on the electronic properties near the Mott transition is studied in an organic superconductor $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Br, which is systematically irradiated by X-ray. We observe that X-ray irradiation causes Anderson-type electron localization due to molecular disorder. The resistivity at low temperatures demonstrates variable range hopping conduction with Coulomb interaction. The experimental results show clearly that the electron localization by disorder is enhanced by the Coulomb interaction near the Mott transition.
The density of states of the organic superconductor $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Br, measured by scanning tunneling spectroscopy on \textit{in-situ} cleaved surfaces, reveals a logarithmic suppression near the Fermi edge persisting above the critical temperature $T_\mathrm{c}$. A soft Hubbard gap as predicted by the Anderson-Hubbard model for systems with disorder exactly describes the experimentally observed suppression. The electronic disorder also explains the diminished coherence peaks of the quasiparticle density of states below $T_\mathrm{c}$.
We present direct evidence of a superconducting state existing in the title compound below 300 mK under quasi-hydrostatic pressure. The superconducing transition is observed in the whole pressure range studied, 0 < P < 4 kbar. However, the character of the transition drastically changes with suppressing the charge-density wave state.
The specific heat of the layered organic superconductor $κ$-% (BEDT-TTF)$_2$Cu(NCS)$_2$, where BEDT-TTF is bisethylenedithio-% tetrathiafulvalene, has been studied in magnetic fields up to 28 T applied perpendicular and parallel to the superconducting layers. In parallel fields above 21 T, the superconducting transition becomes first order, which signals that the Pauli-limiting field is reached. Instead of saturating at this field value, the upper critical field increases sharply and a second first-order transition line appears within the superconducting phase. Our results give strong evidence…
The vortex state in a single crystal of the layered organic superconductor κ-(BEDT-TTF2Cu(NCS)2, where BEDT-TTF (or ET) is bis(ethylenedithio)tetrathiafulvalene, was studied by 1H-NMR. Under a low field region around 0.75 T, the vortex glass-liquid transition was demonstrated by a diverging of the longitudinal nuclear spin relaxation rate and peak-broadening in spectra. Under a high field region near the upper critical field Hc2(0)~7 T, the curvature of nuclear spin relaxation curves showed a drastic change at the temperature where the emergence of the quantum vortex slush state was reported. …
We present a theoretical study on the superconductivity of $β'$-(BEDT-TTF)$_2$ICl$_2$ at $T_{\rm c}=$14.2 K under a high hydrostatic pressure recently found, which is the highest among organic superconductors. In the present work, we study an effective model using the fluctuation-exchange (FLEX) approximation based on the results of first-principles calculation. In the obtained phase diagram, the superconductivity with $d_{xy}$-like symmetry is realized next to the antiferromagnetic phase, as a result of the one-dimensional to two-dimensional crossover driven by the pressure.
We propose a mew picture for superconductivity in $κ-(BEDT-TTF)_2X$ salts arguing that small-{\bf q} electron-phonon scattering dominates the pairing. We reproduce the distinct X-shaped d-wave gap reported recently by magnetooptic measurements and we argue that the softness of the momentum structure of the gap and the near degeneracy of s- and d-wave gap states may be at the origin of the experimental controversy about the gap symmetry. We show that a magnetic field applied parallel to the planes may induce extended gapless-regions on the FS accounting for the experimental signatures of a Fuld…
The nature of the low-temperature phase of the quasi-two-dimensional conductors $α-(BEDT-TTF)_2{M}Hg(SCN)_4$[{M}=K,Rb,Tl] is considered. It is argued that the magnetic field dependence of the phase diagram is more consistent with a charge-density wave, rather than a spin-density wave ground state. The phase diagram of a charge-density wave in a magnetic field is discussed using a Ginzburg-Landau free energy derived from microscopic theory. New experiments are proposed to test the charge-density-wave hypothesis and detect an additional high field phase.
The thermal conductivity of organic superconductor kappa-(BEDT-TTF)2Cu(NCS)2 (Tc =10.4 K) has been studied in a magnetic field rotating within the 2D superconducting planes with high alignment precision. At low temperatures (T < 0.5 K), a clear fourfold symmetry in the angular variation, which is characteristic of a d-wave superconducting gap with nodes along the directions rotated 45 degrees relative to the b and c axes of the crystal, was resolved. The determined nodal structure is inconsistent with recent theoretical predictions of superconductivity induced by the antiferromagnetic spin flu…
We propose that the superconducting pairing symmetry of organic superconductors $κ$-(BEDT-TTF)$_{2}$X can be determined by measuring the position in momentum space of the incommensurate peaks of the spin susceptibility. We show that the positions of these peaks are uniquely determined by the symmetry of the superconducting state and the geometry of Fermi surface. Based on the effective Hubbard model on an anisotropic triangular lattice, we demonstrate the different incommensurate patters of spin responses for $d_{x^{2}-y^{2}}$- and $d_{xy}$-like pairing states. In addition, we predict the none…
While the optical properties of the superconducting salt $α$-(BEDT-TTF)$_2$NH$_4$Hg(SCN)$_4$ remain metallic down to 2 K, in the non-superconducting K-analog a pseudogap develops at frequencies of about 200 cm$^{-1}$ for temperatures T < 200 K. Based on exact diagonalisation calculations on an extended Hubbard model at quarter-filling we argue that fluctuations associated with short range charge ordering are responsible for the observed low-frequency feature. The different ground states, including superconductivity, are a consequence of the proximity of these compounds to a quantum phase charg…
We determine the pressure dependence of the electron-phonon coupling constant in $κ$-(BEDT-TTF)$_{2}$Cu(SCN)$_{2}$ by comparison of high pressure Raman scattering and high pressure infrared reflectivity (IR) measurements. We use comparison of the IR reflection spectrum from deuterated and protonated samples to aid the deconvolution of several overlapping phonon modes. These coupled modes are modelled with a Green's function to extract the linear pressure dependence of the individual modes. The Raman active molecular vibrations of the BEDT-TTF dimers stiffen by 0.1-1 %GPa$^{-1}$. In contrast, t…
We report high-field magnetotransport measurements on β''-(BEDT-TTF)_4[(H_3O)M(C_2O_4)_3]Y, where M=Ga, Cr and Fe and Y=C_5H_5N. We observe similar Shubnikov-de Haas oscillations in all compounds, attributable to four quasi-two-dimensional Fermi-surface pockets, the largest of which corresponds to a cross-sectional area ~8.5\% of the Brillouin zone. The cross-sectional areas of the pockets are in agreement with the expectations for a compensated semimetal, and the corresponding effective masses are ~m_e, rather small compared to those of other BEDT-TTF salts. Apart from the case of the smalles…
We present magnetic-torque experiments on the organic superconductor k-(BEDT-TTF)2Cu(NCS)2 for magnetic fields applied parallel to the 2D superconducting layers. The experiments show a crossover from a second-order to a first-order transition when the upper critical field reaches 21 T. Beyond this field, which we interpret as the Pauli limit for superconductivity, the upper critical field line shows a pro-nounced upturn and a phase transition line separates the superconducting state into a low- and a high-field phase. We interpret the data in the framework of a Fulde-Ferrell-Larkin-Ovchinnikov…
The conducting properties of the pressure-induced, layered organic superconductor (BEDT-TTF)_3Cl_2.2H_20 have been studied at 13.5 and 14.0 kbar using low temperatures, high magnetic fields and two-axis rotation. An upper critical field that is significantly larger than that expected from the Pauli paramagnetic limit is observed when the field is applied parallel to the conducting layers. The angle dependent magnetoresistance suggests incoherent transport between the conducting layers at both pressures and the observed negative magnetoresistance at 13.5 kbar can be explained by considering And…
We performed $^{13}$C-NMR experiment and measured spin-lattice relaxation rate divided by temperature $1/T_{1}T$ near the superconducting (SC) transition temperature $T_{c}$ in $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Br ($κ$-Br salt), and $κ$-(BEDT-TTF)$_{2}$Cu(NCS)$_{2}$ ($κ$-NCS salt). We observed the reduction of $1/T_{1}T$ starting at the temperature higher than $T_c$ in $κ$-Br salt. Microscopic observation of quasi-particle density of states in the fluctuating SC state revealed the effects of short-range Cooper pairs induced in the normal state to the quasi-particle density of states. We also …
We show that the anisotropy of the effective spin model for the dimer Mott insulator phase of $κ$-(BEDT-TTF)$_2X$ salts is dramatically different from that of the underlying tight-binding model. Intra-dimer quantum interference results in a model of coupled spin chains, where frustrated interchain interactions suppress long-range magnetic order. Thus, we argue, the "spin liquid" phase observed in some of these materials is a remnant of the Tomonaga-Luttinger physics of a single chain. This is consistent with previous experiments and resolves some outstanding puzzles. An erratum [Phys. Rev. Let…
The superconducting transition in the layered organic compound α-(BEDT-TTF)_2KHg(SCN)_4 has been studied in the two hydrostatic pressure regimes where a charge-density wave is either present or completely suppressed. Within the charge-density-wave state the experimental results reveal a network of weakly coupled superconducting regions. This is especially seen in a strong enhancement of the measured critical field and the corresponding positive curvature of its temperature dependence. Further, it is shown that on lowering the pressure into the density-wave state traces of a superconducting pha…
The electron paramagnetic resonance study for an organic superconductor $β''$-(BEDT-TTF)$_{4}$[(H$_3$O)Ga(C$_2$O$_4$)$_3$]$\cdot$C$_6$H$_5$NO$_2$ reveals that superconductivity coexists uniformly with the charge ordered state in one material. In the charge ordered state, the interplane spin exchange is gapped, while the in-plane conductivity is not significantly modified. This anisotropic behavior is explained by the exotic charge ordered state, in which molecular-site selective carrier localization coexists with conducting carriers on other molecules. Relationship between superconductivity an…
We have studied the interlayer resistivity of the prototypical quasi-two-dimensional organic superconductor $κ$-(BEDT-TTF)$_2$Cu(NCS)$_2$ as a function of temperature, current and magnetic field, within the superconducting state. We find a region of non-zero resistivity whose properties are strongly dependent on magnetic field and current density. There is a crossover to non-Ohmic conduction below a temperature that coincides with the 2D vortex solid -- vortex liquid transition. We interpret the behaviour in terms of a model of current- and thermally-driven phase slips caused by the diffusive …
Cyclotron resonance, along with its second and third harmonics, has been observed in the quasi-two-dimensional organic superconductor $β^{\prime\prime}$-(BEDT-TTF)$_2$SF$_5$CH$_2$CF$_2$SO$_3$. The harmonic content is richly angle-dependent, and is interpreted in terms of the interlayer warping of the Fermi surface giving rise to the cyclotron resonance. In a departure from Kohn's theorem, but in agreement with recent theoretical predictions, the effective mass deduced from the cyclotron resonance measurements is greater than that determined from magnetic quantum oscillations.
The Mott-insulator κ-(BEDT-TTF)_2Cu_2(CN)_3 is the prime candidate of a quantum spin liquid with puzzling magnetic properties. Our THz and infrared investigations reveal that also the charge dynamics does not follow the expectations for a Mott insulator. The frequency-dependent conductivity exhibits a power-law behavior $σ_1(ω)\propto ω^n$ that grows stronger as the temperature decreases and extends all the way through the far-infrared. With $n\approx 0.8$ to 1.5 we obtain a significantly smaller exponent than predicted by Ng and Lee [Phys. Rev. Lett. {\bf 99}, 156402 (2007)]. We suggest fluct…
The suppression of superconductivity by nonmagnetic disorder is investigated systematically in the organic superconductor $κ$-(BEDT-TTF)$_2$Cu(NCS)$_2$. We introduce a nonmagnetic disorder arising from molecule substitution in part with deuterated BEDT-TTF or BMDT-TTF for BEDT-TTF molecules and molecular defects introduced by X-ray irradiation. A quantitative evaluation of the scattering time $τ_{\rm dHvA}$ is carried out by de Haas-van Alphen (dHvA) effect measurement. A large reduction in $T_{\rm c}$ with a linear dependence on $1/τ_{\rm dHvA}$ is found in the small-disorder region below $1/…
Fluctuation spectroscopy is used to investigate the organic bandwidth-controlled Mott system $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Cl. We find evidence for percolative-type superconductivity in the spatially inhomogeneous coexistence region of antiferromagnetic insulating and superconducting states which develops under pressure at low temperatures. When the superconducting transition is driven by a magnetic field, percolation seems to be dominated by unstable superconducting clusters upon approaching $T_c (B)$ from above, before a "classical" type of percolation is resumed at low fields, dominated by…
In the organic superconducting κ-(BEDT-TTF) compounds, various transport phenomena exhibit striking non-Fermi liquid behaviors, which should be the important clues to understanding the electronic state of this system. Especially, the Hall coefficient ($R_H$) shows Curie-Weiss type temperature dependence, which is similar to that of high-Tc cuprates. In this paper, we study a Hubbard model on an anisotropic triangular lattice at half filling, which is an effective model of κ-(BEDT-TTF) compounds. Based on the fluctuation-exchange (FLEX) approximation, we calculate the resistivity ($ρ$) and $R_H…
Interplay between the Mott transition and the multicritical phenomenon of d-wave superconductivity (SC) and antiferromagnetism (AF) is studied theoretically. We describe the Mott transition, which is analogous to a liquid-gas phase transition, in terms of an Ising-type order parameter $η$. We reveal possible mean-field phase diagrams produced by this interplay. Renormalization group analysis up to one-loop order gives flows of coupling constants, which in most cases lead to fluctuation-induced first-order phase transitions even when the SO(5) symmetry exists betwen the SC and AF. Behaviors of …
We investigated the infrared optical spectra of an organic dimer Mott insulator $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Cl, which was irradiated with X-rays. We observed that the irradiation caused a large spectral weight transfer from the mid-infrared region, where interband transitions in the dimer and Mott-Hubbard bands take place, to a Drude part in a low-energy region; this caused the Mott gap to collapse. The increase of the Drude part indicates a carrier doping into the Mott insulator due to irradiation defects. The strong redistribution of the spectral weight demonstrates that the organic M…
Discontinuities in elastic constants are detected at the superconducting transition of layered organic conductors κ-(BEDT-TTF)_{2}X by longitudinal and transverse ultrasonic velocity measurements. Symmetry arguments show that discontinuities in shear elastic constants can be explained in the orthorhombic compound only if the superconducting order parameter has a mixed character that can be of two types, either A_{1g}+B_{1g} or B_{2g}+B_{3g} in the classification of irreducible representations of the orthorhombic point group D_{2h}. Consistency with other measurements suggests that the A_{1g}+B…
We compare magnetotransport measurements under pressure on the organic superconductor $κ$-(BEDT-TTF)$_{2}$Cu(SCN)$_{2}$ with different pressure-media and discover that the results are pressure media dependent. This pressure-medium dependence is thought to originate from the difference in thermal contraction between the very soft and highly anisotropic sample and the isotropically contracting, but solid pressure medium, thus resulting in non-hydrostatic pressure on the sample. However, comparison of pressure measurements with different media reveals a pressure-medium independent correlation bet…
We investigate the influence of disorders in terminal ethylene groups of BEDT-TTF molecules (ethylene-disorders) on the vortex pinning of the organic superconductor $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Br. Magnetization measurements are performed under different cooling-processes. The second peak in the magnetization hysteresis curve is observed for all samples studied, and the hysteresis width of the magnetization becomes narrower by cooling faster. In contradiction to the simple pinning effect of disorder, this result shows the suppression of the vortex pinning force by introducing more ethylene-d…
We theoretically study the competition among different electronic phases in molecular conductors $κ$-(BEDT-TTF)$_2$X. The ground-state properties of a 3/4-filled extended Hubbard model with the $κ$-type geometry are investigated by a variational Monte Carlo method. We find various competing phases: dimer-Mott insulator, polar charge-ordered insulator, 3-fold charge-ordered metal, and superconductivity, whose pairing symmetry is an "extended-$s$+$d_{x^2-y^2}$"-wave type. Our results show that the superconducting phase is stabilized not on the verge of the Mott metal-insulator transition but nea…
Incommensurate lattice fluctuations are present in the beta_L phase (T_c = 1.5 K) of ET_2I_3 (where ET is BEDT-TTF - bis(ethylenedithio)tetrathiafulvalene) but are absent in the beta_H phase (T_c = 7 K). We propose that the disorder in the conformational degrees of freedom of the terminal ethylene groups of the ET molecules, which is required to stabilise the lattice fluctuations, increases the quasiparticle scattering rate and that this leads to the observed difference in the superconducting critical temperatures, T_c, of the two phases. We calculate the dependence of T_c on the interlayer re…
A Hubbard model at half-filling on an anisotropic triangular lattice has been proposed as the minimal model to describe conducting layers of $κ-(BEDT-TTF)_2X$ organic materials. The model interpolates between the square lattice and decoupled chains. The $κ-(BEDT-TTF)_2X$ materials present many similarities with cuprates, such as the presence of unconventional metallic properties and the close proximity of superconducting and antiferromagnetic phases. As in the cuprates, spin fluctuations are expected to play a crucial role in the onset of superconductivity. We perform a weak-coupling renormali…
Details of the Fermi-surface topology of deuterated $κ$-(BEDT-TTF)$_2$Cu(NCS)$_2$ ~have been measured as a function of pressure, and compared with equivalent measurements of the undeuterated salt. We find that the superconducting transition temperature is much more dramatically suppressed by increasing pressure in the deuterated salt. It is suggested that this is linked to pressure-induced changes in the Fermi-surface topology, which occur more rapidly in the deuterated salt than in the undeuterated salt as the pressure is raised. Our data suggest that the negative isotope effect observed on d…
We report the in-plane microwave surface impedance of a high quality single crystal of κ-(BEDT-TTF)2Cu[N(CN)2]Br. In the superconducting state, we find three independent signatures of d-wave pairing: i) a strong, linear temperature dependence of superfluid density; ii) deep in the superconducting state the quasiparticle scattering rate Γ~ T^3; and iii) no BCS coherence peak is observed in the quasiparticle conductivity. Above T_c, the Kadowaki-Woods ratio and the temperature dependence of the in-plane conductivity show that the normal state is a Fermi liquid below ~ 23 K, yet resilient quasipa…
We calculate the effective Coulomb repulsion between electrons/holes, U, and site energy for an isolated BEDT-TTF [bis(ethylenedithio)tetrathiafulvalene] molecule in vacuo. U=4.2 \pm 0.1 eV for 44 experimental geometries taken from a broad range of conformations, polymorphs, anions, temperatures, and pressures (the quoted `error' is one standard deviation). Hence we conclude that U is essentially the same for all of the compounds studied. This shows that the strong (hydrostatic and chemical) pressure dependence observed in the phase diagrams of the BEDT-TTF salts is not due to U. Therefore, if…
We calculate the effective Coulomb interactions between holes in dimers of the organic molecule BEDT-TTF in vacuo. We use density functional theory (DFT) to parameterise Hubbard models for beta and kappa phase organic charge transfer salts. We focus on the intra-dimer Coulomb repulsion, U_d, and the inter-monomer Coulomb repulsion, V_m. We find that U_d = 3.22 \pm 0.09 eV and V_m = 2.71 \pm 0.10 eV for 23 experimental geometries taken from a range of materials in both polymorphs. The quoted error is one standard deviation over the set of conformations studied. We conclude that U_d and V_m are …
The C=C stretching modes in resonance Raman spectra and infrared reflectivity were measured at temperatures between 15 K and 300 K using various polarizations in k-(BEDT-TTF)_2Cu[N(CN)_2]Br, its fully and partially deuterated analogues, and ^{13}C-substituted analogue. The infrared- and Raman-active bands were re-assigned based on the factor group analysis. We found a Raman-active EMV-coupled ν_3 mode near 1420 cm_{-1}, which shows a large downshift and broadening through the inter-dimer EMV interaction. The mixing of the bridge and ring C=C stretching vibrations depends upon the symmetry of t…
We present the results of precise correlated-electron calculations on the monomer lattices of the organic charge-transfer solids $κ$-(BEDT-TTF)$_2$X for 32 and 64 molecular sites. Our calculations are for band parameters corresponding to X = Cu[N(CN)$_2$]Cl and Cu$_2$(CN)$_3$, which are semiconducting antiferromagnetic and quantum spin liquid, respectively, at ambient pressure. We have performed our calculations for variable electron densities $ρ$ per BEDT-TTF molecule, with $ρ$ ranging from 1 to 2. We find that $d$-wave superconducting pair-pair correlations are enhanced by electron-electron …
Unconventional density waves (UDW) are one of the ground states in metallic crystalline solids and have been speculated already in 1968. However, more focused studies on UDW started only recently, perhaps after the identification of the low temperature phase in alpha-(BEDT-TTF)_2KHg(SCN)_4 as unconventional charge density wave (UCDW) in 2002. More recently, the metallic phase of Bechgaard salts (TMTSF)_2X with X=PF_6 and ReO_4 under both pressure and magnetic field appears to be unconventional spin density wave (USDW). The pseudogap regime of high T_c superconductors LSCO, YBCO, Bi2212 and the…
Static susceptibility of kappa-[(BEDT-TTF)1-x(BEDSe-TTF)x]2Cu[N(CN)2]Br alloys with the BEDSe-TTF content near the border-line of ambient pressure superconductivity (x~0.3) has been measured as a function of temperature, magnetic field, and pressure. A non-monotonic pressure dependence is observed for both the superconducting critical temperature and superconducting volume fraction, with both quantities showing growth under pressure in the initial pressure range P < 0.3 kbar. The results are discussed in comparison with the data on the related kappa-phase BEDT-TTF superconductors in which not …
We present a first-principles density-functional calculation for the Raman spectra of a neutral BEDT-TTF molecule. Our results are in excellent agreement with experimental results. We show that a planar structure is not a stable state of a neutral BEDT-TTF molecule. We consider three possible conformations and discuss their relation to disorder in these systems.
Half-filled two-leg Hubbard ladders have spin-gapped short-range antiferromagnetic correlations while three-leg ladders have power law antoferromagnetic correlations, and both systems have d_{x^2-y^2}-power law pairing correlations when they are doped. Thus these ladders exhibit some of the phenomenology seen in the layered cuprates. Here we report results for half-filled frustrated Hubbard ladders, based upon ladder segments taken from a tight-binding model of kappa-BEDT-TTF. Although these ladders are half-filled, varying the degree of frustration can drive them across an insulator-metal tra…
High-resolution specific-heat measurements of the organic superconductor kappa-(BEDT-TTF)_2Cu[N(CN)_2]Br in the superconducting (B = 0) and normal (B = 14 T) state show a clearly resolvable anomaly at Tc = 11.5 K and an electronic contribution, Ces, which can be reasonably well described by strong-coupling BCS theory. Most importantly, Ces vanishes exponentially in the superconducting state which gives evidence for a fully gapped order parameter.
The first study of thermal conductivity, $κ$, in a quasi-two-dimensional organic superconductor of the $κ$-(BEDT-TTF)$_2$X family reveals features analogous to those already observed in the cuprates. The onset of superconductivity is associated with a sudden increase in $κ$ which can be suppressed by the application of a moderate magnetic field. At low temperatures, a finite linear term - due to a residual electronic contribution- was resolved. The magnitude of this term is close to what is predicted by the theory of transport in unconventional superconductors.
We present magnetic-torque measurements of the organic superconductor k-(BEDT-TTF)2Cu(NCS)2 for in-plane magnetic fields up to 32 T. In this layered two-dimensional compound the superconductivity can persist even in fields above the Pauli limit of about 21 T. There, a pronounced upturn of the upper-critical-field line occurs and the superconducting phase-transition line splits and forms an additional high magnetic field phase. k-(BEDT-TTF)2Cu(NCS)2 is a spin-singlet superconductor, therefore, such a superconducting high-field phase beyond the Pauli limit can originate only from Cooper pairing …
Single crystals of the layered organic type II superconductor, $κ$-(BEDT-TTF)$_{2}$Cu(NCS)$_{2}$, have been studied in magnetic fields of up to 33 T and at temperatures between 0.5 K and 11 K using a compact differential susceptometer. When the magnetic field lies precisely in the quasi-two-dimensional planes of the material, there is strong evidence for a phase transition from the superconducting mixed state into a Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) state, manisfested as a change in the rigidity of the vortex system. The behaviour of the transition as a function of temperature is in good…
We calculate the lattice phonons and the electron-phonon coupling of the organic superconductor κ-(BEDT-TTF)_2 I_3, reproducing all available experimental data connected to phonon dynamics. Low-frequency intra-molecular vibrations are strongly mixed to lattice phonons. Both acoustic and optical phonons are appreciably coupled to electrons through the modulation of the hopping integrals (e-LP coupling). By comparing the results relevant to superconducting κ- and β-(BEDT-TTF)_2 I_3, we show that electron-phonon coupling is fundamental to the pairing mechanism. Both e-LP and electron-molecular vi…
