Correlated paramagnetism and interplay of magnetic and phononic degrees of freedom in 3d-5d coupled La2CuIrO6.

Conventional paramagnetism-a state with finite magnetic moment per ion sans long range magnetic ordering, but with lowering temperature the moment each ion picks up a particular direction, breaking spin rotational symmetry, and results into long-range magnetic ordering. However, in systems with competing multiple degrees of freedom this conventional notion may easily break and results into short range correlation much above the global magnetic transition temperature. La2CuIrO6 with complex interplay of spins (s = 1/2) on Cu site and pseudo-spin (j  = 1/2) on Ir site owing to strong spin-orbit coupling provides fertile ground to observe such correlated phenomena. By a comprehensive temperature dependent Raman study, we have shown the presence of such a correlated paramagnetic state in La2CuIrO6 much above the long-range magnetic ordering temperature (T N ). Our observation of strong interactions of phonons, associated with Cu/Ir octahedra, with underlying magnetic degrees of freedom mirrored in the observed Fano asymmetry, which remarkably persists as high as ~3.5T N clearly signals the existence of correlated paramagnetism hence broken spin rotational symmetry. Our detailed analysis also reveals anomalous changes in the self-energy parameters of the phonon modes, i.e. mode frequencies and linewidth, below T N , providing a useful gauge for monitoring the strong coupling between phonons and magnetic degrees of freedom.

Direct study of structural phase transformation in single crystalline bulk and thin film BaFe2As2.

The ternary iron arsenide compound BaFe2As2 exhibits a structural phase transition from tetragonal to orthorhombic at a temperature of about 140 K. The twin lamellae arising below this transition temperature were studied in undoped single crystalline bulk and epitaxial thin film samples using electron backscatter diffraction in a scanning electron microscope equipped with a helium cryostat. Applying this technique on bulk single crystals a characteristic twin lamella size in the range of 0.1 µm up to a few µm was observed. In contrast, in epitaxially strained thin films the phase transition is not observed at temperatures above 19 K.

Orbiton-phonon coupling in Ir5+(5d 4) double perovskite Ba2YIrO6.

Ba2YIrO6, a Mott insulator, with four valence electrons in Ir5+ d-shell (5d 4) is supposed to be non-magnetic, with J eff = 0, within the atomic physics picture. However, recent suggestions of non-zero magnetism have raised some fundamental questions about its origin. We focus on the phonon dynamics, probed via Raman scattering, as a function of temperature and different incident photon energies, as an external perturbation. Our studies reveal strong renormalization of the phonon self-energy parameters and integrated intensity for first-order modes, especially redshift of the few first-order modes with decreasing temperature and anomalous softening of modes associated with IrO6 octahedra, as well as high energy Raman bands attributed to the strong anharmonic phonons and coupling with orbital excitations. The distinct renormalization of second-order Raman bands with respect to their first-order counterpart suggest that higher energy Raman bands have significant contribution from orbital excitations. Our observation indicates that strong anharmonic phonons coupled with electronic/orbital degrees of freedom provides a knob for tuning the conventional electronic levels for 5d-orbitals, and this may give rise to non-zero magnetism as postulated in recent theoretical calculations with rich magnetic phases.

Evolution of the magnetic order of Fe and Eu sublattices in Eu1-x Ca x Fe2As2 (0 ⩽ x ⩽ 1) single crystals.

Single crystals of Eu1-x Ca x Fe2As2 ([Formula: see text]) are grown using the high-temperature solution-growth method employing FeAs self-flux. Structural and chemical analysis indicates that these crystals are homogeneous and their lattice parameters exhibit a gradual monotonic decrease with increasing Ca concentration. Detailed magnetic, specific heat and resistivity data were used to construct a phase diagram which depicts the evolution of the structural/spin-density-wave transition at T 0, and of the antiferromagnetic (AFM) ordering temperature of the Eu moments at T N. We found out that while T N decreases monotonically from 19.1 K (for x = 0) to below 2 K (for [Formula: see text]), T 0 remains almost constant up to x = x c and decreases steadily for higher values of x. Annealing at low temperatures for several days leads to enhancement of T N and T 0 by a few kelvin and sharpened the anomalies associated with these transitions. However, annealing did not change the variation of T N and T 0 across the series. The observation that T 0 is almost constant until the long-range AFM ordering of the Eu2+ moments gets destroyed, suggests a subtle interrelationship between the Eu2+ and Fe2+ magnetic sublattices.

Unraveling the Nature of Magnetism of the 5d

We report electron spin resonance (ESR) spectroscopy results on the double perovskite Ba_{2}YIrO_{6}. On general grounds, this material is expected to be nonmagnetic due to the strong coupling of the spin and orbital momenta of Ir^{5+} (5d^{4}) ions. However, controversial experimental reports on either strong antiferromagnetism with static order at low temperatures or just a weakly paramagnetic behavior have triggered a discussion on the breakdown of the generally accepted scenario of the strongly spin-orbit coupled ground states in the 5d^{4} iridates and the emergence of a novel exotic magnetic state. Our data evidence that the magnetism of the studied material is solely due to a few percent of Ir^{4+} and Ir^{6+} magnetic defects while the regular Ir^{5+} sites remain nonmagnetic. Remarkably, the defect Ir^{6+} species manifest magnetic correlations in the ESR spectra at T≲20 K, suggesting a long-range character of superexchange in the double perovskites as proposed by recent theories.

Signatures of a magnetic field-induced unconventional nematic liquid in the frustrated and anisotropic spin-chain cuprate LiCuSbO4.

Modern theories of quantum magnetism predict exotic multipolar states in weakly interacting strongly frustrated spin-1/2 Heisenberg chains with ferromagnetic nearest neighbor (NN) inchain exchange in high magnetic fields. Experimentally these states remained elusive so far. Here we report strong indications of a magnetic field-induced nematic liquid arising above a field of ~13 T in the edge-sharing chain cuprate LiSbCuO4 ≡ LiCuSbO4. This interpretation is based on the observation of a field induced spin-gap in the measurements of the 7Li NMR spin relaxation rate T 1-1 as well as a contrasting field-dependent power-law behavior of T 1-1 vs. T and is further supported by static magnetization and ESR data. An underlying theoretical microscopic approach favoring a nematic scenario is based essentially on the NN XYZ exchange anisotropy within a model for frustrated spin-1/2 chains and is investigated by the DMRG technique. The employed exchange parameters are justified qualitatively by electronic structure calculations for LiCuSbO4.

Two distinct superconducting phases in LiFeAs.

A non-trivial temperature evolution of superconductivity including a temperature-induced phase transition between two superconducting phases or even a time-reversal symmetry breaking order parameter is in principle expected in multiband superconductors such as iron-pnictides. Here we present scanning tunnelling spectroscopy data of LiFeAs which reveal two distinct superconducting phases: at = 18 K a partial superconducting gap opens, evidenced by subtle, yet clear features in the tunnelling spectra, i.e. particle-hole symmetric coherence peak and dip-hump structures. At Tc = 16 K, these features substantiate dramatically and become characteristic of full superconductivity. Remarkably, the distance between the dip-hump structures and the coherence peaks remains practically constant in the whole temperature regimeT ≤ . This rules out the connection of the dip-hump structures to an antiferromagnetic spin resonance.

Weak-coupling superconductivity in a strongly correlated iron pnictide.

Iron-based superconductors have been found to exhibit an intimate interplay of orbital, spin, and lattice degrees of freedom, dramatically affecting their low-energy electronic properties, including superconductivity. Albeit the precise pairing mechanism remains unidentified, several candidate interactions have been suggested to mediate the superconducting pairing, both in the orbital and in the spin channel. Here, we employ optical spectroscopy (OS), angle-resolved photoemission spectroscopy (ARPES), ab initio band-structure, and Eliashberg calculations to show that nearly optimally doped NaFe0.978Co0.022As exhibits some of the strongest orbitally selective electronic correlations in the family of iron pnictides. Unexpectedly, we find that the mass enhancement of itinerant charge carriers in the strongly correlated band is dramatically reduced near the Γ point and attribute this effect to orbital mixing induced by pronounced spin-orbit coupling. Embracing the true band structure allows us to describe all low-energy electronic properties obtained in our experiments with remarkable consistency and demonstrate that superconductivity in this material is rather weak and mediated by spin fluctuations.

Mutual Independence of Critical Temperature and Superfluid Density under Pressure in Optimally Electron-Doped Superconducting LaFeAsO(1-x)F(x).

The superconducting properties of LaFeAsO(1-x)F(x) under conditions of optimal electron doping are investigated upon the application of external pressure up to ∼23 kbar. Measurements of muon-spin spectroscopy and dc magnetometry evidence a clear mutual independence between the critical temperature T(c) and the low-temperature saturation value for the ratio n(s)/m(*) (superfluid density over effective band mass of Cooper pairs). Remarkably, a dramatic increase of ∼30% is reported for n(s)/m(*) at the maximum pressure value while T(c) is substantially unaffected in the whole accessed experimental window. We argue and demonstrate that the explanation for the observed results must take the effect of nonmagnetic impurities on multiband superconductivity into account. In particular, the unique possibility to modify the ratio between intraband and interband scattering rates by acting on structural parameters while keeping the amount of chemical disorder constant is a striking result of our proposed model.

Phonon anomalies, orbital-ordering and electronic raman scattering in iron-pnictide Ca(Fe0.97Co0.03)2As2: temperature-dependent Raman study.

We report inelastic light scattering studies on Ca(Fe0.97Co0.03)2As2 in a wide spectral range of 120-5200 cm( - 1) from 5 to 300 K, covering the tetragonal to orthorhombic structural transition as well as magnetic transition at Tsm ~ 160 K. The mode frequencies of two first-order Raman modes B1g and Eg, both involving the displacement of Fe atoms, show a sharp increase below Tsm. Concomitantly, the linewidths of all the first-order Raman modes show anomalous broadening below Tsm, attributed to strong spin-phonon coupling. The high frequency modes observed between 400 and 1200 cm( - 1) are attributed to electronic Raman scattering involving the crystal field levels of d-orbitals of Fe(2+). The splitting between xz and yz d-orbital levels is shown to be ~25 meV, which increases as temperature decreases below Tsm. A broad Raman band observed at ~3200 cm( - 1) is assigned to two-magnon excitation of the itinerant Fe 3d antiferromagnet.

Flux dynamics and avalanches in the 122 pnictide superconductor Ba0.65Na0.35Fe2As2.

In this work we present the results of the bulk magnetization measurements in a superconducting state of single crystals of Ba0.65Na0.35Fe2As2. The isothermal magnetic field (H âˆ¥ c axis) dependent magnetization (M) loops exhibit a second peak (SP) or 'fishtail effect', as well as remarkable flux jumps at low temperatures. The critical current density Jc obtained from the M(H) loops is rather high, of the order of 10(6) A cm(-2). The analysis of the temperature- and field-dependent Jc implies that high Jc is mainly due to collective (weak) pinning of vortices by dense microscopic point defects with some contribution from a strong pinning mechanism. Pronounced magnetic instabilities in terms of flux jumps depend strongly on temperature as well as on the field sweep rate. The field for the first flux jump as calculated from an adiabatic model, however, is much lower than the experimentally observed values, and this enhanced stability is attributed to a flux creep phenomenon. The analysis of field-dependent magnetic relaxation data additionally supports a collective pinning model. The data further suggest that SP in M(H) is likely related to the crossover in creep dynamics from an elastic to a plastic mechanism. We have constructed the vortex phase diagram on the field-temperature plane.

Evidence for a vortex-glass transition in superconducting Ba(Fe0.9Co0.1)2As2.

Measurements of magneto-resistivity and magnetic susceptibility were performed on single crystals of superconducting Ba(Fe0.9Co0.1)2As2 close to the conditions of optimal doping. The high quality of the investigated samples allows us to reveal dynamic scaling behaviour associated with a vortex-glass phase transition in the limit of a weak degree of quenched disorder. Accordingly, the dissipative component of the ac susceptibility is reproduced well within the framework of Havriliak-Negami relaxation, assuming a critical power-law divergence for the characteristic correlation time τ of the vortex dynamics. Remarkably, the random disorder introduced by the Fe1-xCox chemical substitution is found to act on the vortices as a much weaker quenched disorder than previously reported for cuprate superconductors such as Y1-xPrxBa2Cu3O7-δ.

Local structure and hyperfine interactions of 57Fe in NaFeAs studied by Mössbauer spectroscopy.

Detailed 57Fe Mössbauer spectroscopy measurements on superconducting NaFeAs powder samples have been performed in the temperature range 13 K ≤ T < 300 K. The 57Fe spectra recorded in the paramagnetic range (T > TN ≈ 46 K) are discussed supposing that most of the Fe2+ ions are located in distorted (FeAs4) tetrahedra of NaFeAs phase, while an additional minor (<10%) component of the spectra corresponds to impurity or intergrowth NaFe2As2 phase with a nominal composition near NaFe2As2. Our results reveal that the structural transition (TS ≈ 55 K) has a weak effect on the electronic structure of iron ions, while at T ≤ TN the spectra show a continuous distribution of hyperfine fields HFe. The shape of these spectra is analyzed in terms of two models: (i) an incommensurate spin density wave modulation of iron magnetic structure, (ii) formation of a microdomain structure or phase separation. It is shown that the hyperfine parameters obtained using these two methods have very similar values over the whole temperature range. Analysis of the temperature dependence HFe(T) with the Bean­Rodbell model leads to ζ = 1.16 ± 0.05, suggesting that the magnetic phase transition is first order in nature. A sharp evolution of the VZZ(T) and η(T) parameters of the full Hamiltonian of hyperfine interactions near T ≈ (TN,TS) is interpreted as a manifestation of the anisotropic electron redistribution between the dxz-, dyz- and dxy-orbitals of the iron ions.

Anomalous superconducting state in LiFeAs implied by the 75As Knight shift measurement.

(75)As NMR investigation of a single crystal of superconducting LiFeAs is presented. The Knight shift and the in situ ac susceptibility measurements as a function of temperature and external field are indicative of two superconducting (SC) transition temperatures, each of which is associated with its own upper critical field. Strikingly, the Knight shift maintains its normal state value over a temperature range in the SC state before it drops abruptly, being consistent with spin-singlet pairing. Together with our previous NMR study, the anomalous SC state featuring the constant Knight shift is attributed to the extremely sensitive SC properties of LiFeAs, probably stemming from its proximity to a critical instability.

Probing the role of co substitution in the electronic structure of iron pnictides.

The role of Co substitution in the low-energy electronic structure of Ca(Fe(0.944)Co(0.056))(2)As(2) is investigated by resonant photoemission spectroscopy and density-functional theory. The Co 3d state center of mass is observed at 250 meV higher binding energy than that of Fe, indicating that Co possesses one extra valence electron and that Fe and Co are in the same oxidation state. Yet, significant Co character is detected for the Bloch wave functions at the chemical potential, revealing that the Co 3d electrons are part of the Fermi sea determining the Fermi surface. This establishes the complex role of Co substitution in CaFe(2)As(2) and the inadequacy of a rigid-band shift description.

Inelastic neutron-scattering measurements of incommensurate magnetic excitations on superconducting LiFeAs single crystals.

Magnetic correlations in superconducting LiFeAs were studied by elastic and by inelastic neutron-scattering experiments. There is no indication for static magnetic ordering, but inelastic correlations appear at the incommensurate wave vector (0.5±Î´,0.5-/+δ,0) with δ~0.07 slightly shifted from the commensurate ordering observed in other FeAs-based compounds. The incommensurate magnetic excitations respond to the opening of the superconducting gap by a transfer of spectral weight.

Weak superconducting pairing and a single isotropic energy gap in stoichiometric LiFeAs.

We report superconducting (SC) properties of stoichiometric LiFeAs (T(c)=17 K) studied by small-angle neutron scattering (SANS) and angle-resolved photoemission (ARPES). Although the vortex lattice exhibits no long-range order, well-defined SANS rocking curves indicate better ordering than in chemically doped 122 compounds. The London penetration depth lambda(ab)(0)=210+/-20 nm, determined from the magnetic field dependence of the form factor, is compared to that calculated from the ARPES band structure with no adjustable parameters. The temperature dependence of lambda(ab) is best described by a single isotropic SC gap Delta(0)=3.0+/-0.2 meV, which agrees with the ARPES value of Delta(0)(ARPES)=3.1+/-0.3 meV and corresponds to the ratio 2Delta/k(B)T(c)=4.1+/-0.3, approaching the weak-coupling limit predicted by the BCS theory. This classifies LiFeAs as a weakly coupled single-gap superconductor.