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As-vacancies, local moments, and Pauli limiting in LaO_0.9F_0.1FeAs_(1-delta) superconductors

136   0   0.0 ( 0 )
 Added by S. -L. Drechsler
 Publication date 2011
  fields Physics
and research's language is English




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We report magnetization measurements of As-deficient LaO_0.9F_0.1FeAs_1-delta (delta about 0.06) samples with improved superconducting properties as compared with As-stoichiometric optimally doped La-1111 samples. In this As-deficient system with almost homogeneously distributed As-vacancies (AV), as suggested by the (75)As-nuclear quadrupole resonance (NQR) measurements,we observe a strong enhancement of the spin-susceptibility by a factor of 3-7. This observation is attributed to the presence of an electronically localized state around each AV, carrying a magnetic moment of about 3.2 mu_Bohr per AV or 0.8 mu_Bohr/Fe atom. From theoretical considerations we find that the formation of a local moment on neighboring iron sites of an AV sets in when the local Coulomb interaction exceeds a critical value of about 1.0 eV in the dilute limit. Its estimated value amounts to ~ 2.5 eV and implies an upper bound of ~ 2 eV for the Coulomb repulsion at Fe sites beyond the first neighbor-shell of an AV. Electronic correlations are thus moderate/weak in doped La-1111. The strongly enhanced spin susceptibility is responsible for the Pauli limiting behavior of the superconductivity that we observe in As-deficient LaO_0.9F_0.1FeAs_1-delta. In contrast, no Pauli limiting behavior is found for the optimally doped, As-stoichiometric LaO_0.9F_0.1FeAs superconductor in accord with its low spin susceptibility.



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We report upper critical field B_c2(T) data for disordered (arsenic-deficient) LaO_0.9F_0.1FeAs_(1-delta) in a wide temperature and magnetic field range up to 47 T. Because of the large linear slope of Bc2 about -5.4 T/K to -6.6 T/K near Tc = 28.5 K the T-dependence of the in-plane Bc2(T) shows a flattening near 23 K above 30 T which points to Pauli-limited behavior with Bc2(0) about 63-68 T. Our results are discussed in terms of disorder effects within conventional and unconventional superconducting pairings.
In view of the recent experimental facts in the iron-pnictides, we make a proposal that the itinerant electrons and local moments are simultaneously present in such multiband materials. We study a minimal model composed of coupled itinerant electrons and local moments to illustrate how a consistent explanation of the experimental measurements can be obtained in the leading order approximation. In this mean-field approach, the spin-density-wave (SDW) order and superconducting pairing of the itinerant electrons are not directly driven by the Fermi surface nesting, but are mainly induced by their coupling to the local moments. The presence of the local moments as independent degrees of freedom naturally provides strong pairing strength for superconductivity and also explains the normal-state linear-temperature magnetic susceptibility above the SDW transition temperature. We show that this simple model is supported by various anomalous magnetic properties and isotope effect which are in quantitative agreement with experiments.
A direct and element-specific measurement of the local Fe spin moment has been provided by analyzing the Fe 3s core level photoemission spectra in the parent and optimally doped CeFeAsO1-xFx (x = 0, 0.11) and Sr(Fe1 xCox)2As2 (x = 0, 0.10) pnictides. The rapid time scales of the photoemission process allowed the detection of large local spin moments fluctuating on a 10-15 s time scale in the paramagnetic, anti-ferromagnetic and superconducting phases, indicative of the occurrence of ubiquitous strong Hunds magnetic correlations. The magnitude of the spin moment is found to vary significantly among different families, 1.3 muB in CeFeAsO and 2.1 muB in SrFe2As2. Surprisingly, the spin moment is found to decrease considerably in the optimally doped samples, 0.9 muB in CeFeAsO0.89F0.11 and 1.3 muB in Sr(Fe0.9Co0.1)2As2. The strong variation of the spin moment against doping and material type indicates that the spin moments and the motion of itinerant electrons are influenced reciprocally in a self-consistent fashion, reflecting the strong competition between the antiferromagnetic super-exchange interaction among the spin moments and the kinetic energy gain of the itinerant electrons in the presence of a strong Hunds coupling. By describing the evolution of the magnetic correlations concomitant with the appearance of superconductivity, these results constitute a fundamental step toward attaining a correct description of the microscopic mechanisms shaping the electronic properties in the pnictides, including magnetism and high temperature superconductivity.
We report resistivity and upper critical field B_c2(T) data for disordered (As deficient) LaO_0.9F_0.1FeAs_1-delta in a wide temperature and high field range up to 60 T. These samples exhibit a slightly enhanced superconducting transition at T_c = 28.5 K and a significantly enlarged slope dB_c2/dT = -5.4 T/K near T_c which contrasts with a flattening of B_c2(T) starting near 23 K above 30 T. The latter evidences Pauli limiting behaviour (PLB) with B_c2(0) approximately 63 T. We compare our results with B_c2(T)-data from the literature for clean and disordered samples. Whereas clean samples show almost no PLB for fields below 60 to 70 T, the hitherto unexplained pronounced flattening of B_c2(T) for applied fields H II ab observed for several disordered closely related systems is interpreted also as a manifestation of PLB. Consequences are discussed in terms of disorder effects within the frames of (un)conventional superconductivity, respectively.
As-vacancies (V_As) in La-1111-systems, which are nominally non-magnetic defects, are shown to create in their vicinity by symmetry ferromagnetically oriented local magnetic moments due to the strong, covalent bonds with neighboring Fe atoms that they break. From microscopic theory in terms of an appropriately modified Anderson-Wolff model, we find that the moment formation results in a substantially enhanced paramagnetic susceptibility in both the normal and superconducting (SC) state. Despite the V_As act as magnetic scatterers, they do not deteriorate SC properties which can even be improved by V_As by suppressing a competing or coexisting commensurate spin density wave or its remnant fluctuations. Due to the induced local magnetic moments an s_++-scenario in related systems is unlikely.
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