L. Harnagea

Leibniz Institute for Solid State and Materials Research Dresden, Dresden, Saxony, Germany

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Publications (35)91.93 Total impact

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    ABSTRACT: Using two experimental techniques, we studied single crystals of the 122-FeAs family with almost the same critical temperature, Tc. We investigated the temperature dependence of the lower critical field of a single crystal under static magnetic fields parallel to the axis. The temperature dependence of the London penetration depth can be described equally well either by a single anisotropic -wave-like gap or by a two-gap model, while a d-wave approach cannot be used to fit the London penetration depth data. Intrinsic multiple Andreev reflection effect spectroscopy was used to detect bulk gap values in single crystals of the intimate compound, with the same Tc. We estimated the range of the large gap value 6-8 meV (depending on small variation of and its a space anisotropy of about 30%, and the small gap 1.7 meV. This clearly indicates that the gap structure of our investigated systems more likely corresponds to a nodeless s-wave two gaps.
    08/2014;
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    ABSTRACT: We present an inelastic neutron scattering study on single-crystalline LiFeAs devoted to the characterization of the incommensurate antiferromagnetic fluctuations at $\mathbf{Q}=(0.5\pm\delta, 0.5\mp\delta, q_l)$. Time-of-flight measurements show the presence of these magnetic fluctuations up to an energy transfer of 60 meV, while polarized neutrons in combination with longitudinal polarization analysis on a triple-axis spectrometer prove the pure magnetic origin of this signal. The normalization of the magnetic scattering to an absolute scale yields that magnetic fluctuations in LiFeAs are by a factor eight weaker than the resonance signal in nearly optimally Co-doped BaFe$_2$As$_2$, although a factor two is recovered due to the split peaks owing to the incommensurability. The longitudinal polarization analysis indicates weak spin space anisotropy with slightly stronger out-of-plane component between 6 and 12 meV. Furthermore, our data suggest a fine structure of the magnetic signal most likely arising from superposing nesting vectors.
    07/2014;
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    ABSTRACT: We report inelastic light scattering studies on Ca(Fe0.97Co0.03)2As2 in a wide spectral range of 120-5200 cm-1 from 5K to 300K, covering the tetragonal to orthorhombic structural transition as well as magnetic transition at Tsm ~ 160K. The mode frequencies of two first-order Raman modes B1g and Eg, both involving displacement of Fe atoms, show 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 400-1200 cm-1 are attributed to the electronic Raman scattering involving the crystal field levels of d-orbitals of Fe2+. 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.
    Journal of Physics Condensed Matter 06/2014; 26(30). · 2.22 Impact Factor
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    ABSTRACT: The electronic structure of the iron chalcogenide superconductor FeSe 1−x was investigated by high-resolution angle-resolved photoemission spectroscopy (ARPES). The results were compared to DFT calculations showing some significant differences between the experimental electronic structure of FeSe 1−x , DFT calculations, and existing data on FeSe x Te 1−x . The bands undergo a pronounced orbital-dependent renormalization, different from what was observed for FeSe x Te 1−x and any other pnictides.
    Physical Review B 06/2014; 89:220506. · 3.66 Impact Factor
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    ABSTRACT: We present femtosecond time-resolved pump-probe spectroscopic studies of a pseudogap (PG) along with the superconducting (SC) gap in an overdoped iron pnictide Ca(Fe0.927Co0.073)2As2. It is seen that the temperature evolution of the photoexcited quasiparticle (QP) relaxation dynamics, coherently excited A1g-symmetric optical phonon and two acoustic phonon dynamics behave anomalously in the vicinity of the superconducting transition temperature Tc. A continuous change in the sign of the experimentally measured transient differential reflectivity Delta_R/R signal at the zero time-delay between the pump and probe pulses at a temperature of ~200 K is inferred as an evidence of the emergence of the PG phase around that temperature. This behavior is independent of the pump photon energy and occurs for crystals without the spin density wave phase transition.
    EPL (Europhysics Letters) 01/2014; · 2.26 Impact Factor
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    ABSTRACT: The local spin susceptibility in superconducting LiFeAs was studied by polarized neutron diffraction as a function of temperature. In the superconducting phase the spin susceptibility is clearly suppressed and it can be well described by the Yosida function suggesting a singlet pairing to occur at low temperature. The spin susceptibility in the normal state and its suppression in the superconducting phase are fully comparable to observations in Co-doped BaFe2As2.
    12/2013; 89(4).
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    ABSTRACT: We report a low-temperature specific heat study of high-quality single crystals of the heavily hole doped superconductor Ca$_{0.32}$Na$_{0.68}$Fe$_2$As$_2$. This compound exhibits bulk superconductivity with a transition temperature $T_c \approx 34$\,K, which is evident from the magnetization, transport, and specific heat measurements. The zero field data manifests a significant electronic specific heat in the normal state with a Sommerfeld coefficient $\gamma \approx 53$ mJ/mol K$^{2}$. Using a multi-band Eliashberg analysis, we demonstrate that the dependence of the zero field specific heat in the superconducting state is well described by a three-band model with an unconventional s$_\pm$ pairing symmetry and gap magnitudes $\Delta_i$ of approximately 2.35, 7.48, and -7.50 meV. Our analysis indicates a non-negligible attractive intraband coupling,which contributes significantly to the relatively high value of $T_c$. The Fermi surface averaged repulsive and attractive coupling strengths are of comparable size and outside the strong coupling limit frequently adopted for describing high-$T_c$ iron pnictide superconductors. We further infer a total mass renormalization of the order of five, including the effects of correlations and electron-boson interactions.
    11/2013; 89(13).
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    ABSTRACT: (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.
    Journal of Physics Condensed Matter 04/2013; 25(16):162204. · 2.22 Impact Factor
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    ABSTRACT: Nonequilibrium quasiparticle relaxation dynamics is reported in superconducting Ca(Fe0.944Co0.056)2As2 single crystals by measuring transient reflectivity changes using femtosecond time-resolved pump-probe spectroscopy. Large changes in the temperature-dependent differential reflectivity values in the vicinity of the spin density wave (TSDW) and superconducting (TSC) transition temperatures of the sample have been inferred to have charge gap opening at those temperatures. We have estimated the zero-temperature charge gap value in the superconducting state to be ∼1.8kBTSC and an electron–phonon coupling constant λ of ∼0.1 in the normal state that signifies the weak coupling in iron pnictides. From the peculiar temperature-dependence of the quasiparticle dynamics in the intermediate temperature region between TSC and TSDW we infer a temperature scale where the charge gap associated with the spin ordered phase is maximum and closes on either side while approaching the two phase transition temperatures.
    Solid State Communications 04/2013; 160:8–12. · 1.53 Impact Factor
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    ABSTRACT: Electronic structure of newly synthesized single crystals of calcium iron arsenide doped with sodium with Tc ranging from 33 to 14 K has been determined by angle-resolved photoemission spectroscopy (ARPES). The measured band dispersion is in general agreement with theoretical calculations, nonetheless implies absence of Fermi surface nesting at antiferromagnetic vector. A clearly developing below Tc strongly band-dependant superconducting gap has been revealed for samples with various doping levels. BCS ratio for optimal doping, $2\Delta/k_{\rm B}T_{\rm c}=5.5$, is substantially smaller than the numbers reported for related compounds, implying a non-trivial relation between electronic dispersion and superconducting gap in iron arsenides.
    Physical Review B 03/2013; 87:094501. · 3.66 Impact Factor
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    ABSTRACT: Several angle-resolved photoemission spectroscopy (ARPES) studies reveal a poorly nested Fermi surface of LiFeAs, far away from a spin density wave instability, and clear-cut superconducting gap anisotropies. On the other hand a very different, more nested Fermi surface and dissimilar gap anisotropies have been obtained from quasiparticle interference (QPI) data, which were interpreted as arising from intraband scattering within holelike bands. Here we show that this ARPES-QPI paradox is completely resolved by interband scattering between the holelike bands. The resolution follows from an excellent agreement between experimental quasiparticle scattering data and T-matrix QPI calculations (based on experimental band structure data), which allows disentangling interband and intraband scattering processes.
    Physical Review Letters 01/2013; 110(1):017006. · 7.73 Impact Factor
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    ABSTRACT: We report ultrafast quasiparticle (QP) dynamics and coherent acoustic phonons in undoped CaFe_2As_2 iron pnictide single crystals exhibiting spin-density wave (SDW) and concurrent structural phase transition at temperature TSDW ~ 165 K using femtosecond time-resolved pump-probe spectroscopy. The contributions in transient differential reflectivity arising from exponentially decaying QP relaxation and oscillatory coherent acoustic phonon mode show large variations in the vicinity of T_SDW. From the temperature-dependence of the QP recombination dynamics in the SDW phase, we evaluate a BCS-like temperature dependent charge gap with its zero-temperature value of ~(1.6+/-0.2)k_BT_SDW, whereas, much above T_SDW, an electron-phonon coupling constant of ~0.13 has been estimated from the linear temperature-dependence of the QP relaxation time. The long-wavelength coherent acoustic phonons with typical time-period of ~100 ps have been analyzed in the light of propagating strain pulse model providing important results for the optical constants, sounds velocity and the elastic modulus of the crystal in the whole temperature range of 3 K to 300 K.
    Journal of the Physical Society of Japan 01/2013; 82(4):044715. · 2.09 Impact Factor
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    ABSTRACT: We report temperature evolution of coherently excited acoustic and optical phonon dynamics in superconducting iron pnictide single crystal Ca(Fe_0.944Co_0.056)_2As_2 across the spin density wave transition at T_SDW ~ 85 K and superconducting transition at T_SC ~20 K. Strain pulse propagation model applied to the generation of the acoustic phonons yields the temperature dependence of the optical constants, and longitudinal and transverse sound velocities in the temperature range of 3.1 K to 300 K. The frequency and dephasing times of the phonons show anomalous temperature dependence below T_SC indicating a coupling of these low energy excitations with the Cooper-pair quasiparticles. A maximum in the amplitude of the acoustic modes at T ~ 170 is seen, attributed to spin fluctuations and strong spin-lattice coupling before T_SDW.
    EPL (Europhysics Letters) 12/2012; 100(5):57007. · 2.26 Impact Factor
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    ABSTRACT: $^{75}$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 reveal 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 in the SC state at high temperatures, whereas it drops abruptly entering the other state at low temperatures indicating the occurrence of spin-singlet pairing. We discuss that the anomalous SC state at high temperatures emerges due to the extreme sensitivity of the system.
    11/2012;
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    ABSTRACT: We report a combined valence band photoemission and Auger spectroscopy study of single crystalline Ca(Fe,Co)2As2 and Ba(Fe,TM)2As2 with TM=Ni or Cu. The valence band photoemission data show directly that the TM-states move to higher binding energies with increasing atomic number, contributing less and less to the states close to the Fermi level. Furthermore, the 3d8 final state of the LVV Auger decay, which is observed for Ni and Cu, unambiguously reveals the accumulation of charge at these impurities. We also show that the onsite Coulomb interaction on the impurity strongly increases when moving from Co over Ni to Cu. Our results quantify the impurity potentials and imply that the superconducting state is robust against impurity scattering.
    Physical review. B, Condensed matter 10/2012; 87(13). · 3.77 Impact Factor
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    ABSTRACT: Ca(Fe1−xCox)2As2 single crystals with concentration x=0.032, 0.051, and 0.063 were investigated by means of neutron diffraction under hydrostatic pressure. The region of existence of the high-temperature tetragonal, low-temperature orthorhombic, and pressure-induced collapsed tetragonal phases have been determined and the corresponding p-T phase diagrams for the three compositions have been constructed. Structural details of the tetragonal phases at various conditions have been determined. The anomaly marking the orthorhombic-to-tetragonal structural phase transition temperature TS decreases with increasing Co substitution. Similarly to that, the critical pressure of the tetragonal (or orthorhombic)-to-collapsed-tetragonal transition also decreases with increasing Co doping level. The behavior is highly hysteretic and the differences in critical pressures with increasing and decreasing branches eventually makes the collapsed tetragonal phase stable down to ambient pressure and enables structural studies under identical conditions. Within the error bars on the fourth digit, no modification of the As structural positional parameter is found. Such a result suggests that the change of the As-As bond is caused solely by the reduction of the c-axis lattice parameter.
    Physical review. B, Condensed matter 03/2012; 85(10). · 3.77 Impact Factor
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    ABSTRACT: 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 Fe's, indicating that Co posses one extra valence electron, and that Fe and Co are in the same 2+ oxidation state. Yet, significant Co character is detected for the Bloch wavefunctions 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 CaFe2As2, and the inadequacy of a rigid-band shift description.
    Physical Review Letters 03/2012; 109(7). · 7.73 Impact Factor
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    ABSTRACT: A crucial step in revealing the nature of unconventional superconductivity is to investigate the symmetry of the superconducting order parameter. Scanning tunneling spectroscopy has proven a powerful technique to probe this symmetry by measuring the quasiparticle interference (QPI) which sensitively depends on the superconducting pairing mechanism. A particularly well-suited material to apply this technique is the stoichiometric superconductor LiFeAs as it features clean, charge neutral cleaved surfaces without surface states and a relatively high T(c)∼18  K. Our data reveal that in LiFeAs the quasiparticle scattering is governed by a van Hove singularity at the center of the Brillouin zone which is in stark contrast to other pnictide superconductors where nesting is crucial for both scattering and s(±) superconductivity. Indeed, within a minimal model and using the most elementary order parameters, calculations of the QPI suggest a dominating role of the holelike bands for the quasiparticle scattering. Our theoretical findings do not support the elementary singlet pairing symmetries s(++), s(±), and d wave. This brings to mind that the superconducting pairing mechanism in LiFeAs is based on an unusual pairing symmetry such as an elementary p wave (which provides optimal agreement between the experimental data and QPI simulations) or a more complex order parameter (e.g., s+id wave symmetry).
    Physical Review Letters 03/2012; 108(12):127001. · 7.73 Impact Factor
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    ABSTRACT: 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±δ,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.
    Physical Review Letters 03/2012; 108(11):117001. · 7.73 Impact Factor
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    ABSTRACT: The anisotropy of the magnetic excitations in BaFe2As2 was studied by polarization analysis. We find the in-plane polarized transverse magnon to lie at higher energy than the out-of-plane polarized one indicating very strong in-plane single-ion anisotropy. Superconducting LiFeAs exhibits the suppression of local susceptibility expected for spin-singlet pairing. Inelastic correlations appear in LiFeAs at the incommensurate wave vectors, they respond to the opening of the superconducting gap by a transfer of spectral weight.
    02/2012;