Aperiodic quantum oscillations of particle-hole asymmetric Dirac cones

We report experimental measurements and theoretical analysis of Shubnikov-de Haas (SdH) oscillations in a Dirac cone system: the a-(BEDT-TTF)2I3 organic metal under hydrostatic pressure. The measured SdH oscillations reveal anomalies at high magnetic fields B where the 1/B oscillations periodicity is lost above 7 T. We interpret these unusual results within a theoretical model that takes into account intrinsic distortions of the a-(BEDT-TTF)2I3 Dirac cones such as a parabolic particle-hole asymmetric correction. Others possible causes, such as a cone tilting or a Zeeman effect, are carefully ruled out. The observations are consistent among a-(BEDT-TTF)2I3 samples with different Fermi levels

Charge-transfer processes in radical ion molecular conductors κ-(BEDT-TTF)2Cu[N(CN)2]Br x Cl1 − x : The superconductor (x = 0.9) and the conductor with the metal-insulator transition (x = 0)

Optical spectral investigations of low-dimensional organic molecular conductors κ-(BEDT-TTF)2Cu[N(CN)2]Br x Cl1 − x with x = 0.9 (the superconductor with T c = 11.3 K) and x = 0 (the metal with the metal-insulator transition at T < 50 K) are performed in the range 50–6000 cm−1 (6 meV–0.74 eV) at temperatures from 300 to 20 K. The optical conductivity spectra are quantitatively analyzed in terms of the proposed model, according to which the charge transfer involves two types of charge carriers, i.e., electrons (holes) localized on clusters (dimers and tetramers formed by BEDT-TTF molecules) and quasi-free charge carriers, with the use of the tetramer “cluster“ model based on the Hubbard Hamiltonian for correlated electrons and the Drude model for quasi-free charge carriers. Physical parameters of the model, such as the energy of Coulomb repulsion between two electrons (holes) in one molecule, the transfer integrals between molecules inside the dimer and between dimers, and the electron-molecular vibration coupling constants, are determined. The anisotropy of the spectra in the conducting plane is explained. The inference is made that only electrons localized on clusters couple with intramolecular vibrations

Bandwidth-controlled Mott transition in κ−(BEDT−TTF)2Cu[N(CN)2]BrxCl1−x\kappa-(BEDT-TTF)_2 Cu [N(CN)_2] Br_x Cl_{1-x} I. Optical studies of localized charge excitations

Infrared reflection measurements of the half-filled two-dimensional organic conductors $\kappa$-(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 couple to intramolecular vibrations of BEDT-TTF, the analysis of both electronic and vibrational features provides a tool to disentangle these contributions and to follow their temperature and electronic-correlations dependence. Calculations based on the cluster model support our interpretation.Comment: 12 pages, 12 figure

Inhomogeneous superconductivity in organic conductors: role of disorder and magnetic field

Several experimental studies have shown the presence of spatially inhomogeneous phase coexistence of superconducting and non superconducting domains in low dimensional organic superconductors. The superconducting properties of these systems are found to be strongly dependent on the amount of disorder introduced in the sample regardless of its origin. The suppression of the superconducting transition temperature $T_c$ shows clear discrepancy with the result expected from the Abrikosov-Gor'kov law giving the behavior of $T_c$ with impurities. Based on the time dependent Ginzburg-Landau theory, we derive a model to account for the striking feature of $T_c$ in organic superconductors for different types of disorder by considering the segregated texture of the system. We show that the calculated $T_c$ quantitatively agrees with experiments. We also focus on the role of superconducting fluctuations on the upper critical fields $H_{c2}$ of layered superconductors showing slab structure where superconducting domains are sandwiched by non-superconducting regions. We found that $H_{c2}$ may be strongly enhanced by such fluctuations.Comment: to appear in Journal of Physics: Condensed Matte

Crystalline Arrays of Pairs of Molecular Rotors: Correlated Motion, Rotational Barriers, and Space-Inversion Symmetry Breaking Due to Conformational Mutations

The rod-like molecule bis 4-(4-pyridyl)ethynyl)bicyclo[2.2.2]oct-1-yl)buta-1,3-diyne, 1, contains two 1,4-bis(ethynyl)bicyclo[2.2.2]octane (ethynyl) chiral rotators linked by a diyne fragment and self assembles in a one-dimensional, monoclinic C2/c centrosymmetric structure where two equilibrium positions with large occupancy imbalance (88% versus 12%) are identified on a single rotor site Combining variable temperature (70-300 K) proton spin-lattice relaxation, H-1 T-1(-1), at two different H-1 Larmor frequencies (55 and 210 MHz) and DFT calculations of rotational barriers, we were able to assign two types of Brownian rotators with different activation energies, 1.85 and 6.1 kcal mol(-1), to the two H-1 spin-lattice relaxation processes on the single rotor site. On the basis of DFT calculations, the low-energy process has been assigned to adjacent rotors in a well-correlated synchronous motion, whereas the high-energy process is the manifestation of an abrupt change in their kinematics once two blades of adjacent rotors are seen to rub together. Although crystals of 1 should be second harmonic inactive, a large second-order optical response is recorded when the electric field oscillates in a direction parallel to the unique rotor axle director. We conclude that conformational mutations by torsional interconversion of the three blades of the BCO units break space-inversion symmetry in sequences of mutamers in dynamic equilibrium in the crystal in domains at a rnesoscopic scale comparable with the wavelength of light used A control experiment was performed with a crystalline film of a similar tetrayne molecule, 1,4-bis(3-((trimethylsilyl)ethynyl)bicyclo-[1.1.1]pent-1-yObuta-1,3-diyne, whose bic-ydopentane units can rotate but are achiral and produce no second-order optical response

Optical studies of κ\kappa-(ET)2_{2}Cu[ N(CN)2_{2}] Br0.85_{0.85}Cl0.15_{0.15}

The low-temperature ground states of the quasi two-dimensional layered organic charge transfer salts $\kappa$-(ET)$_{2}$Cu[ N(CN)$_{2}$] Br$_{1-x}$Cl$_{x}$ are known to be strongly dependent on the Br/Cl content of the anions. At low temperatures, pure Cl compounds undergo a phase transition into an antiferromagnetic ground state while the pure Br compound is a organic superconductor. Here we present polarized infrared reflectivity measurements on the compound with 85% bromine and 15% chlorine. Our measurements were performed within the highly conducting a-c plane. From room temperature down to 90 K, we observe the typical signatures of a semiconductor in our spectra. When the sample is cooled down further, a significant amount of spectral weight is shifted towards lower frequencies. At 6 K, a Drude-like optical conductivity is observed in the far infrared Key words. charge-transfer salts – organic superconductors – optical properties

Relaxation dynamics in the one-dimensional organic charge-transfer salt δ−(EDT−TTF−CONMe2)2Br

A detailed investigation of the charge-ordered charge-transfer salt \delta-(EDT-TTF-CONMe$_{2}$)$_{2}$Br by thermal-expansion measurements and dielectric spectroscopy reveals three dynamic processes of relaxational character. The slowest one exhibits the characteristics of glassy freezing and is ascribed to the conformational dynamics of terminal ethylene groups of the organic molecules. Such a process was previously found for related charge-transfer salts where, however, the anions form polymerlike chains, in contrast to the spherical anions of the present material. Dielectric spectroscopy reveals two additional relaxational processes. The characteristics of the faster one are consistent with excitations of a one-dimensional Wigner lattice as recently observed in this material by infrared spectroscopy, which are also accompanied by conformational changes of the molecules. However, at low temperature the ethylene-group relaxation exhibits the cooperativity-induced dramatic slowing down that is typical for glassy freezing, while the defect-related Wigner-lattice excitation follows thermally activated behavior as expected for single-dipole relaxations.Comment: 9 pages, 4 figure