Elucidating the nature of the magnetic ground state of iron-based superconductors is of paramount importance in unveiling the mechanism behind their high temperature superconductivity. Until recently, it was thought that superconductivity emerges onl
y from an orthorhombic antiferromagnetic stripe phase, which can in principle be described in terms of either localized or itinerant spins. However, we recently reported that tetragonal symmetry is restored inside the magnetically ordered state of a hole-doped BaFe2As2. This observation was interpreted as indirect evidence of a new double-Q magnetic structure, but alternative models of orbital order could not be ruled out. Here, we present Mossbauer data that show unambiguously that half of the iron sites in this tetragonal phase are non-magnetic, establishing conclusively the existence of a novel magnetic ground state with a non-uniform magnetization that is inconsistent with localized spins. We show that this state is naturally explained as the interference between two spin-density waves, demonstrating the itinerant character of the magnetism of these materials and the primary role played by magnetic over orbital degrees of freedom.
A theory of superconductivity in the iron-based materials requires an understanding of the phase diagram of the normal state. In these compounds, superconductivity emerges when stripe spin density wave (SDW) order is suppressed by doping, pressure or
atomic disorder. This magnetic order is often pre-empted by nematic order, whose origin is yet to be resolved. One scenario is that nematic order is driven by orbital ordering of the iron 3d-electrons that triggers stripe SDW order. Another is that magnetic interactions produce a spin-nematic phase, which then induces orbital order. In this article, we report the observation by neutron powder diffraction of an additional four- fold-symmetric phase in Ba1-xNaxFe2As2 close to the suppression of SDW order, which is consistent with the predictions of magnetically-driven models of nematic order.
We report the results of a systematic investigation of the phase diagram of the iron-based superconductor, Ba1-xKxFe2As2, from x = 0 to x = 1.0 using high resolution neutron and x-ray diffraction and magnetization measurements. The polycrystalline sa
mples were prepared with an estimated compositional variation of Deltax <~ 0.01, allowing a more precise estimate of the phase boundaries than reported so far. At room temperature, Ba1-xKxFe2As2 crystallizes in a tetragonal structure with the space group symmetry of I4/mmm, but at low doping, the samples undergo a coincident first-order structural and magnetic phase transition to an orthorhombic (O) structure with space group Fmmm and a striped antiferromagnet (AF) with space group Fcmmm. The transition temperature falls from a maximum of 139K in the undoped compound to 0K at x = 0.252, with a critical exponent as a function of doping of 0.25(2) and 0.12(1) for the structural and magnetic order parameters, respectively. The onset of superconductivity occurs at a critical concentration of x = 0.130(3) and the superconducting transition temperature grows linearly with x until it crosses the AF/O phase boundary. Below this concentration, there is microscopic phase coexistence of the AF/O and superconducting order parameters, although a slight suppression of the AF/O order is evidence that the phases are competing. At higher doping, superconductivity has a maximum Tc of 38 K at x = 0.4 falling to 3 K at x = 1.0. We discuss reasons for the suppression of the spin-density-wave order and the electron-hole asymmetry in the phase diagram.
We report inelastic neutron scattering measurements of the resonant spin excitations in Ba1-xKxFe2As2 over a broad range of electron band filling. The fall in the superconducting transi- tion temperature with hole doping coincides with the magnetic e
xcitations splitting into two incom- mensurate peaks because of the growing mismatch in the hole and electron Fermi surface volumes, as confirmed by a tight-binding model with s+- symmetry pairing. The reduction in Fermi surface nesting is accompanied by a collapse of the resonance binding energy and its spectral weight caused by the weakening of electron-electron correlations.
We report inelastic neutron scattering measurements of crystal field transitions in PrFeAsO, PrFeAsO0.87F0.13, and NdFeAsO0.85F0.15. Doping with fluorine produces additional crystal field excitations, providing evidence that there are two distinct ch
arge environments around the rare earth ions, with probabilities that are consistent with a random distribution of dopants on the oxygen sites. The 4f electrons of the Pr3+ and Nd3+ ions have non-magnetic and magnetic ground states, respectively, indicating that the enhancement of Tc compared to LaFeAsO1-xFx is not due to rare earth magnetism.
We report a high resolution neutron diffraction investigation of the coupling of structural and magnetic transitions in Ba1xKxFe2As2. The tetragonal-orthorhombic and antiferromagnetic transitions are suppressed with potassium-doping, falling to zero
at x <~ 0.3. However, unlike Ba(Fe1xCox)2As2, the two transitions are first-order and coincident over the entire phase diagram, with a biquadratic coupling of the two order parameters. The phase diagram is refined showing that the onset of superconductivity is at x = 0.133 with all three phases coexisting until x >~ 0.24.
We present a neutron scattering investigation of Ce1-xYxAl3 as a function of chemical pressure, which induces a transition from heavy-fermion behavior in CeAl3 (TK=5 K) to a mixed-valence state at x=0.5 (TK=150 K). The crossover can be modeled accura
tely on an absolute intensity scale by an increase in the k-f hybridization, Vkf, within the Anderson impurity model. Surprisingly, the principal effect of the increasing Vkf is not to broaden the low-energy components of the dynamic magnetic susceptibility but to transfer spectral weight to high energy.
Neutrons have played an important role in advancing our understanding of the pairing mechanism and the symmetry of the superconducting energy gap in the iron arsenide compounds. Neutron measurements of the phonon density-of-state are in good agreemen
t with ab initio calculations, provided the magnetism of the iron atoms is taken into account. However, the predicted superconducting transition temperatures are less than 1 K, making a conventional phononic mechanism for superconductivity highly unlikely. Measurements of the spin dynamics within the spin density wave phase of the parent compounds show evidence of strongly dispersive spin waves with exchange interactions consistent with the observed magnetic order. Antiferromagnetic fluctuations persist in the normal phase of the superconducting compounds, but they are more diffuse. Below Tc, there is evidence compounds that these fluctuations condense into a resonant spin excitation at the antiferromagnetic wavevector with an energy that scales with Tc, consistent with unconventional superconductivity of extended-s+/- wave symmetry.
The recent observations of superconductivity at temperatures up to 55K in compounds containing layers of iron arsenide have revealed a new class of high temperature superconductors that show striking similarities to the more familiar cuprates. In bot
h series of compounds, the onset of superconductivity is associated with the suppression of magnetic order by doping holes and/or electrons into the band leading to theories in which magnetic fluctuations are either responsible for or strongly coupled to the superconducting order parameter. In the cuprates, theories of magnetic pairing have been invoked to explain the observation of a resonant magnetic excitation that scales in energy with the superconducting energy gap and is suppressed above the superconducting transition temperature, Tc. Such resonant excitations have been shown by inelastic neutron scattering to be a universal feature of the cuprate superconductors, and have even been observed in heavy fermion superconductors with much lower transition temperatures. In this paper, we show neutron scattering evidence of a resonant excitation in Ba0.6K0.4Fe2As2, which is a superconductor below 38K, at the momentum transfer associated with magnetic order in the undoped compound, BaFe2As2, and at an energy transfer that is consistent with scaling in other strongly correlated electron superconductors. As in the cuprates, the peak disappears at Tc providing the first experimental confirmation of a strong coupling of the magnetic fluctuation spectrum to the superconducting order parameter in the new iron arsenide superconductors.
