Shubnikov-de Haas oscillations spectrum of the strongly correlated quasi-2D organic metal (ET)8[Hg4Cl12(C6H5Br)2] under pressure

Pressure dependence of the Shubnikov-de Haas (SdH) oscillations spectra of the quasi-two dimensional organic metal (ET)₈[ Hg₄Cl₁₂(C₆H₅Br)₂] have been studied up to 1.1 GPa in pulsed magnetic fields of up to 54 T. According to band structure calculations, its Fermi surface can be regarded as a network of compensated orbits. The SdH spectra exhibit many Fourier components typical of such a network, most of them being forbidden in the framework of the semiclassical model. Their amplitude remains large in all the pressure range studied which likely rules out chemical potential oscillation as a dominant contribution to their origin, in agreement with recent calculations relevant to compensated Fermi liquids. In addition to a strong decrease of the magnetic breakdown field and effective masses, the latter being likely due to a reduction of the strength of electron correlations, a sizeable increase of the scattering rate is observed as the applied pressure increases. This latter point, which is at variance with data of most charge transfer salts is discussed in connection with pressure-induced features of the temperature dependence of the zero-field interlayer resistance.     

Magnetic oscillations in the 2D network of compensated coupled orbits of the organic metal (BEDT-TTF) 8 Hg 4 Cl 12 (C 6 H 5 Br) 2

Interlayer magnetoresistance and magnetisation of the quasi-two dimensional organic metal (BEDT-TTF)₈Hg₄Cl₁₂(C₆H₅Br)₂ have been investigated in pulsed magnetic fields extending up to 60 T and 33 T, respectively. About fifteen fundamental frequencies, composed of linear combinations of only three basic frequencies, are observed in the oscillatory spectra of the magnetoresistance. The dependencies of the oscillation amplitude on the temperature and on the magnitude and orientation of the magnetic field are analyzed in the framework of the conventional two-dimensional Lifshitz-Kosevitch (LK) model. This model is implemented by damping factors which accounts for the magnetic breakthrough occurring between electron and hole orbits yielding conventional Shubnikov-de Haas closed orbits (model of Falicov and Stachowiak) and quantum interferometers. In particular, a quantum interferometer enclosing an area equal to the first Brillouin zone area is evidenced. The LK model consistently accounts for the temperature and magnetic field dependence of the oscillation amplitude of this interferometer. On the contrary, although this model formally accounts for almost all of the observed oscillatory components, it fails to give consistent quantitative data in most other cases. Received 4 September 2002 / Received in final form 14 November 2002 Published online 27 January 2003 RID="a" ID="a"e-mail: audouard@insa-tlse.fr RID="b" ID="b"UMR 5830: Unité Mixte de Recherche CNRS - Université Paul Sabatier - INSA de Toulouse RID="c" ID="c"UMS 5642: Unité Mixte de Service CNRS - Université Paul Sabatier - INSA de Toulouse     

Frequency combinations in the magnetoresistance oscillations spectrum of a linear chain of coupled orbits with a high scattering rate

The oscillatory magnetoresistance spectrum of the organic metal (BEDO)₅Ni(CN)₄. 3C₂H₄(OH)₂ has been studied up to 50 T, in the temperature range from 1.5 K to 4.2 K. In high magnetic field, its Fermi surface corresponds to a linear chain of quasi-two-dimensional orbits coupled by magnetic breakdown (MB). The scattering rate consistently deduced from the data relevant to the basic α and the MB-induced β orbits is very large which points to a significant reduction of the chemical potential oscillation. Despite of this feature, the oscillations spectrum exhibits many frequency combinations. Their effective masses and (or) Dingle temperature are not in agreement with either the predictions of the quantum interference model or the semiclassical model of Falicov and Stachowiak.     

On the stoichiometry of the organic metal bis(ethylenedioxy)-tetrathiafulvalene chloride

We report on Shubnikov-de Haas and de Haas-van Alphen measurements of an organic metal based on the molecular donor bis(ethylenedioxy)-tetrathiavulvalene (= BEDO-TTF) and the anion Cl^- with H₂O molecules. The observed single oscillation frequency perfectly follows the two-dimensional dependence with T. The Fermi-surface area of of the first Brillouin zone proves a quarter-filled band, i.e., a 2:1 stoichiometry of the BEDO-TTF donor with respect to the anion. The apparent discrepancy to X-ray data which give a 1:1 ratio between BEDO-TTF and Cl^- is understood by replacement of H₂O molecules with (H₃O)⁺ ions. The proposed stoichiometry therefore is (BEDO-TTF)₂ ⁺(H₅O₂)⁺(Cl^-)₂. The cyclotron effective mass is when deduced from the temperature dependence of the fundamental oscillation amplitude, but strongly reduced when extracted from higher harmonics. This and the strong harmonic content of the oscillations signals an influence of the two-dimensional electronic structure and can be qualitatively understood by applying the concept of magnetic interaction to the effect of the oscillatory chemical potential. Received: 16 April 1998 / Revised: 7 July 1998 / Accepted: 9 July 1998     

Unconventional field and angle dependences of the Shubnikov-de Haas oscillations spectra in the quasi two-dimensional organic superconductor (BEDO-TTF) 2ReO 4H 2O

We report on the inter-layer oscillatory conductance of the two-dimensional organic superconductor (BEDO-TTF)₂ReO₄H₂O measured in static and pulsed magnetic fields of up to 15 and 52 T, respectively. In agreement with previous in-plane studies, two Shubnikov-de Haas oscillation series linked to the two electron and the hole orbits are observed. The influence of the magnitude and orientation of the magnetic field with respect to the conducting plane is studied in the framework of the conventional two- and three-dimensional Lifshits-Kosevich (LK) model. Deviations of the data from this model are observed in low fields strongly tilted with respect to the normal to the conducting plane. In this latter case, the observed behaviour is consistent with an unexplained lowering of the cyclotron effective mass. At high magnetic field, the oscillatory data could have been compatible with the occurrence of a magnetic breakdown orbit built from the hole and electron orbits. However, the increase of the cyclotron effective mass, linked to the electron orbits, as the magnetic field increases above ∼12 T is consistent with a field-induced phase transition. In the lower field range, where the conventional LK model holds, the analysis of the angle dependence of the oscillations amplitude suggests significant renormalisation of the effective Landé factor. Received 22 August 2000 and Received in final form 20 December 2000     

Characterization of the Fermi surface of the organic superconductor - by measurements of Shubnikov-de Haas and angle-dependent magnetoresistance oscillations and by electronic band-structure calculations

The electronic structure of the quasi two-dimensional (2D) organic superconductor -(ET)₂SF₅CH₂CF₂SO₃ was examined by measuring Shubnikov-de Haas (SdH) and angle-dependent magnetoresistance (AMRO) oscillations and by comparing with electronic band-structure calculations. The SdH oscillation frequencies follow the angular dependence expected for a 2D Fermi surface (FS), and the observed fundamental frequency shows that the 2D FS is 5% of the first Brillouin zone in size. The AMRO data indicate that the shape of the 2D FS is significantly non-circular. The calculated electronic structure has a 2D FS in general agreement with experiment. From the temperature and angular dependence of the SdH amplitude, the cyclotron and band effective masses were estimated to be and ,where g is the conduction electron g factor and the free electron mass. The band effective mass is estimated to be from the calculated electronic band structure. Received: 3 March 1997 / Revised: 5 May 1997 / Received in final form: 5 November 1997 / Accepted: 10 November 1997     

de Haas-van Alphen effect and the Fermi surface of PrNi5

The Fermi surface of PrNi₅ has been studied by the measurements of the de Haas-van Alphen (dHvA) effect at temperatures between 0.3 and in magnetic fields up to 12 T. Two dHvA frequencies have been obtained. The electronic structure of PrNi₅ was calculated using the full potential linearized augmented plane wave method. Five sheets of the Fermi surface and the multiple extremal cross sections were determined. First and second sheet have a hole-like structure. The agreement between theory and experiment is obtained by a small downward shift ( 0.1 eV) of the Fermi energy which is probably due to an underestimation of the role of 4 f electrons. Received 9 May 2000 and Received in final form 20 September 2000     

Phenomenological theory of the s-wave state in superconductors without an inversion center

In materials without an inversion center of symmetry the spin degeneracy of the conducting band is lifted by an antisymmetric spin orbit coupling (ASOC). Under such circumstances, spin and parity cannot be separately used to classify the Cooper pairing states. Consequently, the superconducting order parameter is generally a mixture of spin singlet and triplet pairing states. In this paper we investigate the structure of the order parameter and its response to disorder for the most symmetric pairing state (A₁). Using the example of the heavy Fermion superconductor CePt₃Si, we determine characteristic properties of the superconducting instability. Depending on the type of the pairing interaction, the gap function is characterized by the presence of line nodes. We show that this line nodes move in general upon temperature. Such nodes would be essential to explain recent low-temperature data of thermodynamic quantities such as the NMR-T₁ ^-1, London penetration depth, and heat conductance. Moreover, we study the effect of (non-magnetic) impurity on the superconducting state.     

Hall effect plateaus and giant Shubnikov-de Haas oscillations in (BiSb)Telayered single crystals near the quantum limit

On bulk layered single crystals (Bi_0.25Sb_0.75)₂Te₃ with a hole concentration cm^-3 and a mobility cm²/Vs magnetoresistance and Hall effect investigations were performed in the temperature range T = 1.4 K ... 20 K in magnetic fields up to 18 T. For the magnetic field perpendicular to the layered structure giant Shubnikov-de Haas oscillations are measured; the positions of the maxima are triplets in the reciprocally scaled magnetic field. From the damping of the amplitudes with increasing temperature the cyclotron mass m _c = 0.12m ₀ is evaluated. Correlated with the SdH oscillations doublets of Hall effect plateaus (or kinks in low fields) are found. The weak well known Shubnikov-de Haas oscillations from the generally accepted multivallied highest valence band can be detected as a modulation on the giant oscillation. The high anisotropy of the SdH oscillations and their triplet structure in connection with the layered crystal structure lead us to suggest that the effects are caused by hole carrier pairing (mediated by the bipolaron mechanism) in quasi 2D sheets parallel to the crystal layer stacks. The measured Hall plateau resistances coincide with the quantum Hall effect values considering the number of layer stacks and the valley degeneracy of the 3D hole carrier reservoir. The ratio of spin splitting to Landau (cyclotron) splitting is observed to be . Received: 12 September 1997 / Revised: 8 January 1998 / Accepted: 22 January 1998     

Coulomb correlations do not fill the e<Superscript>′</Superscript><Subscript>g</Subscript> hole pockets in Na<Subscript>0.3</Subscript>CoO<Subscript>2</Subscript>

There exists presently considerable debate over the question whether local Coulomb interactions can explain the absence of the small e^′ _g Fermi surface hole pockets in photoemission studies of Na_0.3CoO₂. By comparing dynamical mean field results for different single particle Hamiltonians and exact diagonalization as well as quantum Monte Carlo treatments, we show that, for realistic values of the Coulomb energy U and Hund exchange J, the e^′ _g pockets can be slightly enhanced or reduced compared to band structure predictions, but they do not disappear.     

Doping-dependent electronic structure of cuprates studied using angle-scanned photoemission

Full k -maps of the electronic structure near the Fermi level of differently doped cuprates measured with angle-scanned photoelectron spectroscopy are presented. The valence band maximum of the antiferromagnetic insulator Sr₂CuO₂Cl₂, which is taken as a representative of an undoped cuprate, and the Fermi surfaces of overdoped, optimally doped and underdoped Bi₂Sr₂CaCu₂O_8+δ high-temperature superconductors are mapped in the normal state. The results confirm the existence of large Luttinger Fermi surfaces at high doping with a Fermi surface volume proportional to (1+x), where x is the hole concentration. At very low doping, however, we find that this assumption based on Luttinger's theorem is not fulfilled. This implies a change in the topology of the Fermi surface. Furthermore the intensity of the shadow bands observed on the Fermi surface of Bi₂Sr₂CaCu₂O_8+δ as a function of the doping is discussed. Received 12 October 1999 and Received in final form 12 April 2000     

First-principles study of the optical properties of PbFX (X = Cl,Br, I) compounds in its matlockite-type structure

We present the results of the ab initio theoretical study of the optical properties for PbFX (X = Cl, Br, I) compounds in its matlockite-type structure using the full potential linearized augmented plane wave (FP-LAPW) method as implemented in the WIEN2K code. We employed generalized gradient approximation (GGA), which is based on exchange-correlation energy optimization to calculate the total energy. Also we have used the Engel-Vosko GGA formalism, which optimizes the corresponding potential for band structure calculations. Our calculations show that the valence band maximum (VBM) and conduction band minimum (CBM) are located at Z resulting in a direct energy gap. We present calculations of the frequency-dependent complex dielectric function ε( ω) and its zero-frequency limit ε₁ ( 0 ). We find that the values of ε₁ ( 0 ) increases with decreasing the energy gap. The reflectivity spectra and absorption coefficient has been calculated and compared with the available experimental data. The optical properties are analyzed and the origin of some of the peaks in the spectra is discussed in terms of the calculated electronic structure.     

Experimental study of electron-phonon properties in ZrB 2

High quality samples and absence of superconductivity down to 40 mK make of ZrB₂ the best normal state reference system for the superconducting isostructural MgB₂. Actually, the question of pairing has to be focused on the electron-phonon interaction in the normal state. After presenting the resistivity measurements of ZrB₂, we explain the details of the Bloch-Grüneisen and Einstein models used to deduce the first results. We then compare experimental de Haas-van Alphen effect data with theoretical Fermi surfaces to present additional results on electron quasi-particle renormalization. The estimations reveal an isotropic and negligible coupling constant of in average 0.145. The contribution of the coupling to the optical phonon modes is 0.082, in contrast to the known larger coupling of 0.283 [3] to the E_2g phonon mode in MgB₂.     

Doping-dependent evolution of low-energy excitations and quantum phase transitions within an effective model for high-T<Subscript>c</Subscript> copper oxides

In this paper a mean-field theory for the spin-liquid paramagnetic non-superconducting phase of the p- and n-type high-T_c cuprates is developed. This theory applied to the effective t-t'-t′′-J^* model with the ab initio calculated parameters and with the three-site correlated hoppings. The static spin-spin and kinematic correlation functions beyond Hubbard-I approximation are calculated self-consistently. The evolution of the Fermi surface and band dispersion is obtained for the wide range of doping concentrations x. For p-type systems the three different types of behavior are found and the transitions between these types are accompanied by the changes in the Fermi surface topology. Thus a quantum phase transitions take place at x = 0.15 and at x = 0.23.Due to the different Fermi surface topology we found for n-type cuprates only one quantum critical concentration, x = 0.2. The calculated doping dependence of the nodal Fermi velocity and the effective mass are in good agreement with the experimental data.     

Electronic structure and magnetism of YbRhSn

The electronic band structure of YbRhSn has been calculated using the self-consistent full potential nonorthogonal local orbital minimum basis scheme based on the density functional theory. We investigated the electronic structure with the spin-orbit interaction and on-site Coulomb potential for the Yb-derived 4f orbitals to obtain the correct ground state of YbRhSn. The exchange interaction between local f electrons and conduction electrons play an important role in the heavy fermion characters of them. The fully relativistic band structure scheme shows that spin-orbit coupling splits the 4f states into two manifolds, the 4f_7/2 and the 4f_5/2 multiplet.     

Electron and hole effective masses in self-assembled quantum dots

Electron and hole effective masses in self-assembled InAs/GaAs quantum dots are determined by fitting the energy levels calculated by a single-band model to those obtained by a more sophisticated tight-binding method. For the dots of various shapes and dimensions, the electron effective-mass is found to be much larger than that in the bulk and become anisotropic in the dots of large aspect ratio while the hole effective-mass becomes almost isotropic in the dots of small aspect ratio. For flat InAs/GaAs quantum dots, the most appropriate value for the electron and hole effective-mass is believed to be the electron effective-mass in bulk GaAs and the vertical heavy-hole effective-mass in bulk InAs, respectively.     

Violation of the Luttinger sum rule within the Hubbard model on a triangular lattice

The frequency-moment expansion method is developed to analyze the validity of the Luttinger sum rule within the Mott-Hubbard insulator, as represented by the generalized Hubbard model at half filling and large U. For the particular case of the Hubbard model with nearest-neighbor hopping on a triangular lattice lacking the particle-hole symmetry results reveal substantial violation of the sum rule.     

Localization of conduction electrons and the magnetic properties of the molecular metals β″-(BEDT-TTF)4NH4[M(C2O4)3] · DMF (M = Cr3+, Fe3+)

Quasi-two-dimensional organic metals β″-(BEDT-TTF)₄NH₄[M(C₂O₄)₃] · DMF containing the oxalate complexes of Cr³⁺ or Fe³⁺ ions between the conducting organic layers of the BEDT-TTF molecules are studied by EPR spectroscopy, and the contributions of these metallic complexes, conduction electrons, and non-equilibrium lattice defects to the magnetic susceptibility are determined. An analysis of the temperature dependence of the magnetic susceptibility and the EPR line shape has revealed partial localization of conduction electrons at T < 20 K in the crystals with Cr³⁺ ions. The size of the localization region is close to the size of an individual BEDT-TTF molecule. The localization effect weakens as nonequilibrium defects disappear during long-term storage at room temperature. The localization of conduction electrons is found to be accompanied by the appearance of weak antiferromagnetic interaction between the Cr³⁺ ions at T < 20 K, which disappears when Fe³⁺ ions substitute for Cr³⁺ ions.