75As NMR and susceptiblity were measured in a Ba(Fe1-xCox)2As2 single crystal for x=6% for various field H values and orientations. The sharpness of the superconducting and magnetic transitions demonstrates a homogeneity of the Co doping x better than +-0.25%. On the nanometer scale, the paramagnetic part of the NMR spectra is found very anisotropic and very narrow for H//ab which allows to rule out the interpretation of Ref.[6] in terms of strong Co induced electronic inhomogeneities. We propose that a distribution of hyperfine couplings and chemical shifts due to the Co effect on its nearest As explains the observed linewidths and relaxations. All these measurements show that Co substitution induces a very homogeneous electronic doping in BaFe2As2, from nano to micrometer lengthscales, on the contrary to the K doping.
In this supplementary material, we investigate further the impurity-induced freezing mechanism in a doped system of 3D weakly coupled ladders resembling Bi(Cu$_{1-x}$Zn$_x$)$_2$ZnPO$_6$ using large scale Quantum Monte Carlo simulations.
75As NMR and susceptiblity were measured in a Ba(Fe1-xCox)2As2 single crystal for x=6%. Nuclear Magnetic Resonance (NMR) spectra and relaxation rates allow to show that all Fe sites experience an incommensurate magnetic ordering below T=31K. Comparison with undoped compound allows to estimate a typical moment of 0.05 muB. Anisotropy of the NMR widths can be interpreted using a model of incommensurability with a wavevector (1/2-eps,0,l) with eps of the order of 0.04. Below TC=21.8K, a full volume superconductivity develops as shown by susceptibility and relaxation rate, and magnetic order remains unaffected, demonstrating coexistence of both states on each Fe site.
Using 23Na NMR measurements on sodium cobaltates at intermediate dopings (0.44<=x<=0.62), we establish the qualitative change of behavior of the local magnetic susceptibility at x*=0.63-0.65, from a low x Pauli-like regime to the high x Curie-Weiss regime. For 0.5<=x<=0.62, the presence of a maximum T* in the temperature dependence of the susceptibility shows the existence of an x-dependent energy scale. T_1 relaxation measurements establish the predominantly antiferromagnetic character of spin correlations for x<x*. This contradicts the commonly assumed uncorrelated Pauli behavior in this x range and is at odds with the observed ferromagnetic correlations for x>x*. It is suggested that at a given x the ferromagnetic correlations might dominate the antiferromagnetic ones above T*. From 59Co NMR data, it is shown that moving towards higher x away from x=0.5 results in the progressive appearance of nonmagnetic Co3+ sites, breaking the homogeneity of Co states encountered for x<=0.5. The main features of the NMR-detected 59Co quadrupolar effects, together with indications from the powder x-ray diffraction data, lead us to sketch a possible structural origin for the Co3+ sites. In light of this ensemble of new experimental observations, a new phase diagram is proposed, taking into account the systematic presence of correlations and their x-dependence.
We present a comparative study of CoO2 layers in the Bi-misfit and NaxCoO2 cobaltates. Co NMR measures the intrinsic susceptibility of the Co layers and is not affected by spurious contributions. At low dopings where room-temperature thermopower (TEP) is large, Curie-Weiss susceptibilities are observed in both materials. But NMR and muSR experiments find neither charge nor spin order down to low temperatures in Bi-misfit, in contrast to the case of NaxCoO2. This demonstrates that metallicity, charge and magnetic orders are specific of the Na layers in NaxCoO2 whereas strong correlations are generic of the cobaltates physics and could explain the large TEP.
