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 temperatures. This observation is very well in line with the existing theories of field-induced CDW transitions.
The effect of pressure on the B--T phase diagram of $α$-(BEDT-TTF)$_2$KHg(SCN)$_4$ is studied. The measured phase lines can be well described by a recent model of a charge-density wave system with varying nesting conditions. A remarkable increase of the transition temperature with magnetic field is found in a certain pressure and field range. We associate this result with a dramatic enhancement of the orbital effect of magnetic field due to a deterioration of the nesting conditions by pressure. Furthermore, we present data which can be interpreted as a first sign of field-induced charge-densit…
We have used a low-frequency magneto-thermopower (MTEP) method to probe the high magnetic field ground state behavior of $α$-(BEDT-TTF)$_2$KHg(SCN)$_4$ along all three principal crystallographic axes at low temperatures. The thermopower tensor coefficients ($S_{xx}, S_{yx}$ and $S_{zz}$) have been measured to 30 T, beyond the anomalous low temperature, field-induced transition at 22.5 T. We find a significant anisotropy in the MTEP signal, and also observe large quantum oscillations associated with the de Haas - van Alphen effect. The anisotropy indicates that the ground state properties are c…
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.
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.
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.
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.
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…
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…
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…
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…
The temperature-dependent infrared properties of $θ$-(BEDT-TTF)$_2$RbZn(SCN)$_4$ were investigated. In the temperatures above the metal-insulator (M-I) transition, the optical conductivity remains finite in the low energy region, but shows no conventional Drude feature typical of metals. Below the M-I transition temperature, the low-energy spectral weight is significantly reduced. An opening of optical gap at about 300 cm$^{-1}$ is observed clearly in the polarization parallel to the donor-stacking direction. Analysis of both the electronic and vibronic spectra suggests a redistribution of cha…
We explore the nature of the metal-insulator transition in $β^{\prime\prime}$-(BEDT-TTF)$_{2}$Hg(SCN)$_{2}$Cl by x-ray, electrical transport, ESR, Raman and infrared investigations. Magnetic and vibrational spectroscopy concurrently reveal a gradual dimerization along the stacking direction $a$, setting in already at the crossover temperature of 150K from the metallic to the insulating state. A spin gap $Δ_σ= 47$meV is extracted. From the activated resistivity behavior below 55K a charge gap $Δ_ρ=60$meV is derived. At $T_{\rm CO} = 72$K the C=C vibrational modes reveal the development of a cha…
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 present an X-ray diffraction study of the quasi-2D conductors a-(BEDTTTF)2MHg(SCN), with M=K and Rb. They exhibit a phase transition of the density wave type at TDW=8-10K and 12-13K respectively, evidenced by magnetoresistivity, specific heat, NMR and Hall constant measurements. The structural study shows the presence of satellite reflections already at ambient temperature. The related modulation is incommensurate with multiple harmonics. For some of the compounds studied, the intensity of the satellite reflections strongly increases below TDW. According to Fermi surface (FS) calculations, …
The infrared spectra of the quasi-two-dimensional organic conductors $α$-(BEDT-TTF)$_2$$M$Hg(SCN)$_4$ ($M$ = NH$_4$, Rb, Tl) were measured in the range from 50 to 7000 \cm down to low temperatures in order to explore the influence of electronic correlations in quarter-filled metals. The interpretation of electronic spectra was confirmed by measurements of pressure dependant reflectance of $α$-(BEDT-TTF)$_2$KHg(SCN)$_4$ at T=300 K. The signatures of charge order fluctuations become more pronounced when going from the NH$_4$ salt to Rb and further to Tl compounds. On reducing the temperature, th…
We report that the sample miniaturization of first-order-phase-transition bulk systems causes a greater degree of supercooling. From a theoretical perspective, the size effects can be rationalized by considering two mechanisms: (i) the nucleation is a rare and stochastic event, and thus, its rate is correlated with the volume and/or surface area of a given sample; (ii) when the sample size decreases, the dominant heterogeneous nucleation sites that play a primary role for relatively large samples are annealed out. We experimentally verified the size effects on the supercooling phenomena for tw…
We perform magnetic susceptibility and magnetic torque measurements on the organic $κ$-(BEDT-TTF)$_2$Hg(SCN)$_2$Br, which is recently suggested to host an exotic quantum dipole-liquid in its low-temperature insulating phase. Below the metal-insulator transition temperature, the magnetic susceptibility follows a Curie-Weiss law with a positive Curie-Weiss temperature, and a particular $M\propto \sqrt{H}$ curve is observed. The emergent ferromagnetically interacting spins amount to about 1/6 of the full spin moment of localized charges. Taking account of the possible inhomogeneous quasi-charge-o…
The dielectric constant and ac conductivity have been measured for the layered organic conductor theta-(BEDT-TTF)_2CsZn(SCN)_4 along the out-of-plane direction, which show a relaxation behavior similar to those in the charge-density-wave conductor. Most unexpectedly, they exhibit a large bias dependence with a hysteresis, and changes in magnitude by 100-1000 times at a threshold. These findings are very similar to the collective excitation of the charge density wave. theta-$(BEDT-TTF)_2CsZn(SCN)_4 has collective excitations associated with charge ordering, though it shows no clear indication o…
We find a characteristic low-energy peak structure located in the range of 100-300 cm$^{-1}$ in the optical conductivity spectra of a quasi-two-dimensional organic compound with a triangular lattice, $θ$-$\mbox{(BEDT-TTF)}_2\mbox{CsZn(SCN)}_4$, in which two different types of short-range charge orderings (COs) coexist. Upon lowering the temperature, the low-energy peak becomes significant and shifts to much lower frequencies only for the polarization of ${E \parallel a}$, in contrast to the other broad electronic bands in the mid-infrared region. On introducing disorder, the low-energy peak is…
α-(BEDT-TTF)2KHg(SCN)4 is considered to be in the charge-density-wave (CDW) state below 8 K. We present new magnetoresistance data suggesting that the material undergoes a series of field-induced CDW (FICDW) transitions at pressures slightly exceeding the critical pressure Pc at which the zero-field CDW state is destroyed. Further, we argue that a novel kind of FICDW transitions, entirely determined by a superposition of the strong Pauli and quantizing orbital effects of magnetic field on the CDW wavevector, arises when the field is strongly tilted towards the conducting layers. These new tran…
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…
We combine first principles density functional calculations with empirical relationships for the Coulomb interactions in the `monomer' model of $κ$-(BEDT-TTF)$_2X$. This enables us to calculate the parameters for the model of coupled dipolar and spin degrees of freedom proposed by Hotta [Phys. Rev. B $\textbf{82}$, 241104 (2010)], and Naka and Ishihara [J. Phys. Soc. Japan $\textbf{79}$, 063707 (2010)]. In all materials studied, retaining only the largest interactions leads to a transverse field Ising model of the dipoles. This quantifies, justifies and confirms recent claims that the dipoles …
The low-temperature charge-density-wave (CDW) state in the layered organic metals $α$-(BEDT-TTF)$_2$MHg(SCN)$_4$ has been studied by means of the Shubnikov -- de Haas and de Haas -- van Alphen effects. In addition to the dominant alpha-frequency, which is also observed in the normal state, both the magnetoresistance and magnetic torque possess a slowly oscillating component. These slow oscillations provide a firm evidence for the CDW-induced reconstruction of the original cylindrical Fermi surface. The alpha-oscillations of the interlayer magnetoresistance exhibit an anomalous phase inversion …
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 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.
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…
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…
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…
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 report detailed angle-dependent studies of the microwave (f=50 to 90 GHz) interlayer magneto-electrodynamics of a single crystal sample of the organic charge-density-wave (CDW) conductor alpha-(BEDT-TTF)2KHg(SCN)4. Recently developed instrumentation enables both magnetic field (B) sweeps for a fixed sample orientation and, for the first time, angle sweeps at fixed f/B. We observe series' of resonant absorptions which we attribute to periodic orbit resonances (POR) - a phenomenon closely related to cyclotron resonance. The angle dependence of the POR indicate that they are associated with th…
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…
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(…
We present high-resolution measurements of the relative length change as a function of temperature of the organic charge-transfer salt $κ$-(BEDT-TTF)$_2$Hg(SCN)$_2$Cl. We identify anomalous features at $T_g \approx\,63$ K which can be assigned to a kinetic glass-like ordering transition. By determining the activation energy $E_A$, this glass-like transition can be related to conformational degrees of freedom of the ethylene endgroups of the organic building block BEDT-TTF. As opposed to other $κ$-(BEDT-TTF)$_2X$ salts, we identify a peculiar ethylene endgroup ordering in the present material i…
Single crystals of the organic charge-transfer salts $α$-(BEDT-TTF)$_2M$Hg(SCN)$_4$ have been studied using Hall-potential measurements ($M=$K) and magnetization experiments ($M$ = K, Rb). The data show that two types of screening currents occur within the high-field, low-temperature CDW$_x$ phases of these salts in response to time-dependent magnetic fields. The first, which gives rise to the induced Hall potential, is a free current (${\bf j}_{\rm free}$), present at the surface of the sample. The time constant for the decay of these currents is much longer than that expected from the sample…
We report the results of a detailed study of the field orientation-dependence of the de Haas-van Alphen waveform in $α$-(BEDT-TTF)$_2$KHg(SCN)$_4$. By considering the field orientation-dependence of the sign and phase of the fundamental $α$ frequency, at fields both well above and below the kink transition field, it is found that a single value for the product of the effective mass with the electron {\it g}-factor can explain the experimental data deep within both the high magnetic field and low magnetic field phases. This implies that spin-splitting does not occur within the low magnetic fiel…
Recently we have shown that the striking angular dependent magnetoresistance in the low temperature phase (LTP) of alpha-(BEDT-TTF)_2KHg(SCN)_4 is consistently described in terms of unconventional charge density wave (UCDW). Here we investigate theoretically the thermoelectric power and the Nernst effect in UDW. The present results account consistently for the recent data of magnetothermopower in alpha-(BEDT-TTF)_2KHg(SCN)_4 obtained by Choi et al. (Phys. Rev. B, 65, 205119 (2002)). This confirms further our identification of LTP in this salt as UCDW. We propose also that the Nernst effect pro…
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…
To elucidate different photoinduced melting dynamics of charge orders observed in quasi-two-dimensional organic conductors $ θ$-(BEDT-TTF)$_2$RbZn(SCN)$_4$ and $ α$-(BEDT-TTF)$_2$I$_3$ [BEDT-TTF=bis(ethylenedithio)tetrathiafulvalene], we theoretically study photoinduced time evolution of charge and spin correlation functions on the basis of exact many-electron wave functions coupled with classical phonons in extended Peierls-Hubbard models on anisotropic triangular lattices. In both salts, the so-called horizontal-stripe charge order is stabilized by nearest-neighbor repulsive interactions and…
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 …
Charge ordering with structural distortion in quasi-two-dimensional organic conductors θ-(ET)2RbZn(SCN)4 (ET=BEDT-TTF) and α-(ET)2I3 is investigated theoretically. By using the Hartree-Fock approximation for an extended Hubbard model which includes both on-site and intersite Coulomb interactions together with Peierls-type electron-lattice couplings, we examine the role of lattice degrees of freedom on charge order. It is found that the experimentally observed, horizontal charge order is stabilized by lattice distortion in both compounds. In particular, the lattice effect is crucial to the real…
Superconductivity or metallic state may coexist with density wave ordering at imperfect nesting of the Fermi surface. In addition to the macroscopic spatial phase separation, there are, at least, two possible microscopic structures of such coexistence: (i) the soliton-wall phase and (ii) the ungapped Fermi-surface pockets. We show that the conductivity anisotropy allows to distinguish between these two microscopic density-wave structures. The results obtained may help to analyze the experimental observations in layered organic metals (TMTSF)$_{2}$PF$_{6}$, (TMTSF)$_{2}$ClO$_{4}$, $α$-(BEDT-TTF…
We present the results of magnetotransport and magnetic torque measurements on the alpha-(BEDT-TTF)2KHg(SCN)4 charge-transfer salt within the high magnetic field phase, in magnetic fields extending to 33 T and temperatures as low as 27 mK. While the high magnetic field phase (at fields greater than ~ 23 T) is expected, on theoretical grounds, to be either a modulated charge-density wave phase or a charge/spin-density wave hybrid, the resistivity undergoes a dramatic drop below ~ 3 K within the high magnetic field phase, falling in an approximately exponential fashion at low temperatures, while…
Raman signatures of the strong intra- and inter-molecular charge oscillations in bis(ethylenedithio)-tetrathiafulvalene (BEDT-TTF) \k{appa}-phase salts
A superposition of the Pauli and orbital coupling of a high magnetic field to charge carriers in a charge-density-wave (CDW) system is proposed to give rise to transitions between subphases with quantized values of the CDW wavevector. By contrast to the purely orbital field-induced density-wave effects which require a strongly imperfect nesting of the Fermi surface, the new transitions can occur even if the Fermi surface is well nested at zero field. We suggest that such transitions are observed in the organic metal $α$-(BEDT-TTF)$_2$KHg(SCN)$_4$ under a strongly tilted magnetic field.
We suggest a theory of the Field-Induced Charge-Density-Wave (FICDW) phases, generated by high magnetic fields in quasi-low-dimensional conductors. We demonstrate that, in layered quasi-one-dimensional conductors, the corresponding critical magnetic fields ratios are universal and do not depend on any fitting parameter. In particular, we find that $H_1/H_0 = 0.73, \ H_2/H_0 = 0.59, H_3/H_0 = 0.49, H_4/H_0 = 0.42$, where $H_n$ is a critical field of a phase transition between the FICDW phases with numbers $n$ and $n+1$. The suggested theory is in very good qualitative and quantitative agreement…
We scrutinize the magnetic properties of $κ$-(BEDT-TTF)$_2$Hg(SCN)$_2$Cl through its first-order metal-insulator transition at $T_{\rm CO}=30$ K by means of $^1$H nuclear magnetic resonance (NMR). While in the metal we find Fermi-liquid behavior with temperature-independent $(T_1T)^{-1}$, the relaxation rate exhibits a pronounced enhancement when charge order sets in. The NMR spectra remain unchanged through the transition and no magnetic order stabilizes down to 25 mK. Similar to the isostructural spin-liquid candidates $κ$-(BEDT-TTF)$_2$Cu$_2$(CN)$_3$ and $κ$-(BEDT-TTF)$_2$Ag$_2$(CN)$_3$, $T…
The origin of the charge ordering in organic compounds $θ$-(BEDT-TTF)$_2 X$ ($X=MM'$(SCN)$_4$, $M=$Tl,Rb,Co, $M'=$Cs,Zn) is studied using an extended Hubbard model. Calculating the charge susceptibility within random phase approximation (RPA), we find that the $(3\times 3)\sim (3\times 4)$ charge ordering observed at relatively high temperatures can be considered as a consequence of a cooperation between the Fermi surface nesting, controlled by the hopping integral in the $c$ direction, and the electron-electron interactions, where the distant (next nearest neighbor) interactions that have not…
To get insight into the nature of the electronic fluid in the frustration-driven charge glasses, we investigate in-plane and out-of-plane charge transport for several quasi-triangular-lattice organic systems, $θ$-(BEDT-TTF)$_2$X [X=RbZn(SCN)$_4$, CsZn(SCN)$_4$ and I$_3$]. These compounds host a charge order, charge glass and Fermi liquid, depending on the strength of charge frustration. We find that the resistivity exhibits extremely two-dimensional (2D) anisotropy and contrasting temperature dependence between in the in-plane and out-of-plane directions in the charge glass phase, qualitativel…
We present a combined study of thermal expansion and resistance fluctuation spectroscopy measurements exploring the static and dynamic aspects of the charge-glass formation in the quasi-two-dimensional organic conductors $θ$-(BEDT-TTF)$_2$$MM^\prime$(SCN)$_4$ with $M$ = Cs and $M^\prime$ = Co,Zn. In these materials, the emergence of a novel charge-glass state so far has been interpreted in purely electronic terms by considering the strong frustration of the Coulomb interactions on a triangular lattice. Contrary to this view, we provide comprehensive evidence for the involvement of a \textit{st…
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…
Many experiments suggest that the unidentified low temperature phase (LTP) of alpha-(BEDT-TTF)_2KHg(SCN)_4 is most likely unconventional charge density wave (UCDW). To further this identification we present our theoretical study of the threshold electric field of UCDW in a magnetic field. The magnetic field-temperature phase diagram is very similar to those in a d-wave superconductor. We find a rather strong field dependence of the threshold electric field, which should be readily accessible experimentally.
We consider the effect of imperfect nesting in quasi-one dimensional unconventional density waves. The phase diagram is very close to those in a conventional DW. The linear and non-linear aspects of the electric conductivity are discussed. At T=0 the frequency dependent electric conductivity develops a small dip at low frequencies. The threshold electric field depends strongly on the imperfect nesting parameter, allowing us to describe the measured threshold electric field in the low temperature phase of the quasi-two dimensional organic conductor, alpha-(BEDT-TTF)_2KHg(SCN)_4 very well.
As it is well known most of charge density wave (CDW) and spin density wave (SDW) exhibit the nonlinear transport with well defined threshold electric field E_T. Here we study theoretically the threshold electric field of unconventional density waves. We find that the threshold field increases monotonically with temperature without divergent behaviour at T_c, unlike the one in conventional CDW. The present result in the 3D weak pinning limit appears to describe rather well the threshold electric field observed recently in the low-temperature phase (LTP) of alpha-(BEDT-TTF)_2KHg(SCN)_4.
The polarized reflectivity of $β^{\prime\prime}$-(BEDO-TTF)$_5$[CsHg(SCN)$_4$]$_2$ is studied in the infrared range between 60 cm-1 and 6000 cm-1 from room temperature down to 10 K. Already at T=300 K a pseudogap in the optical conductivity is present of about 300 cm-1; the corresponding maximum in the spectrum shifts to lower frequencies as the temperature decreases. In contrast to quarter-filled BEDT-TTF-based conductors of the $β^{\prime\prime}$-phase a robust Drude component in the conductivity spectra is observed which we ascribe to the larger fraction of charge carriers associated with t…
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.
Recently many people discuss unconventional density waves (i.e. unconventional charge density waves (UCDW) and unconventional spin density waves (USDW)). Unlike in conventional density waves, the quasiparticle spectrum in these systems is gapless. Also these systems remain metallic. Indeed it appears that there are many candidates for UDW. The low temperature phase of alpha-(BEDT-TTF)_2KHg(SCN)_4, the antiferromagnetic phase in URu_2Si_2, the CDW in transition metal dichalcogenite NbSe_2, the pseudogap phase in high T_c cuprate superconductors, the glassy phase in organic superconductor kappa-…
Non-Fermi liquid behavior is shown to occur in two-dimensional metals which are close to a charge ordering transition driven by the Coulomb repulsion. A linear temperature dependence of the scattering rate together with an increase of the electron effective mass occur above T*, a temperature scale much smaller than the Fermi temperature. It is shown that the anomalous temperature dependence of the optical conductivity of the quasi-two-dimensional organic metal alpha-(BEDT-TTF)2MHg(SCN)4, with M=NH4 and Rb, above T*=50-100 K, agrees qualitatively with our predictions for the electronic properti…
