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Combined neutron and x-ray diffraction experiments demonstrate the formation of a low-temperature minority tetragonal phase in Ba$_{0.76}$K$_{0.24}$Fe$_2$As$_2$ in addition to the majority magnetic, orthorhombic phase. A coincident enhancement in the magnetic ($\frac{1}{2}$ $\frac{1}{2}$ 1) peaks shows that this minority phase is of the same type that was observed in Ba$_{1-x}$Na$_x$Fe$_2$As$_2$ ($0.24 \leq x \leq 0.28$), in which the magnetic moments reorient along the $c$-axis. This is evidence that the tetragonal magnetic phase is a universal feature of the hole-doped iron-based superconductors., Comment: 6 pages, 7 figures

We present neutron diffraction analysis of BaFe$_2$(As$_{1-x}$P$_x$)$_2$ over a wide temperature (10 to 300 K) and compositional ($0.11 \leq x \leq 0.79$) range, including the normal state, the magnetically ordered state, and the superconducting state. The paramagnetic to spin-density wave and orthorhombic to tetragonal transitions are first order and coincident within the sensitivity of our measurements ($\sim 0.5$ K). Extrapolation of the orthorhombic order parameter down to zero suggests that structural quantum criticality cannot exist at compositions higher than $x = 0.28$, which is much lower than values determined using other methods, but in good agreement with our observations of the actual phase stability range. The onset of spin-density wave order shows a stronger structural anomaly than the charge-doped system in the form of an enhancement of the $c/a$ ratio below the transition., Comment: 10 pages, 7 figures, 2 tables

We report the results of a systematic investigation of the phase diagram of the iron-based superconductor system, Ba1-xNaxFe2As2, from x = 0.1 to x = 1.0 using high resolution neutron and x-ray diffraction and magnetization measurements. We find that the coincident structural and magnetic phase transition to an orthorhombic (O) structure with space group Fmmm and a striped antiferromagnet (AF) with space group F(C)mm'm' in Ba1-xNaxFe2As2 is of first order. A complete suppression of the magnetic phase is observed by x = 0.30, and bulk superconductivity occurs at a critical concentration near 0.15. We compare the new findings to the previously reported results of the hole-doped Ba1-xKxFe2As2 solid solution in order to resolve the differing effects of band filling and A-site cation size on the properties of the magnetic and superconducting ground states. The substantial size difference between Na and K causes various changes in the lattice trends, yet the overarching property phase diagram from the Ba1-xKxFe2As2 phase diagram carries over to the Ba1-xNaxFe2As2 solid solution. We note that the composition dependence of the c axis turns over from positive to negative around x = 0.35, unlike the K-substituted materials. We show that this can be understood by invoking steric effects; primarily the Fe2As2 layer shape is dictated mostly by the electronic filling, which secondarily induces an interlayer spacing adjusted to compensate for the given cation volume. This exemplifies the primacy of even subtle features in the Fe2As2 layer in controlling both the structure and properties in the uncollapsed 122 phases., Comment: 10 pages, 12 figures, 2 tables

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., Comment: Article (6 pages, 3 figures) + Supplementary Information (5 pages, 3 figures)

Superconductivity in iron selenides has experienced a rapid growth, but not without major inconsistencies in the reported properties. For alkali-intercalated iron selenides, even the structure of the superconducting phase is a subject of debate, in part because the onset of superconductivity is affected much more delicately by stoichiometry and preparation than in cuprate or pnictide superconductors. If high-quality, pure, superconducting intercalated iron selenides are ever to be made, the intertwined physics and chemistry must be explained by systematic studies of how these materials form and by and identifying the many coexisting phases. To that end, we prepared pure K_2Fe_4Se_5 powder and superconductors in the K_xFe_{2-y}Se_2 system, and examined differences in their structures by high-resolution synchrotron and single-crystal x-ray diffraction. We found four distinct phases: semiconducting K_2Fe_4Se_5, a metallic superconducting phase K_xFe_2Se_2 with x ranging from 0.38 to 0.58, an insulator KFe_{1.6}Se_2 with no vacancy ordering, and an oxidized phase K_{0.51(5)}Fe_{0.70(2)}Se that forms the PbClF structure upon exposure to moisture. We find that the vacancy-ordered phase K_2Fe_4Se_5 does not become superconducting by doping, but the distinct iron-rich minority phase K_xFe_2Se_2 precipitates from single crystals upon cooling from above the vacancy ordering temperature. This coexistence of metallic and semiconducting phases explains a broad maximum in resistivity around 100 K. Further studies to understand the solubility of excess Fe in the K_xFe_{2-y}Se_2 structure will shed light on the maximum fraction of superconducting K_xFe_2Se_2 that can be obtained by solid state synthesis., Comment: 12 pages, 16 figures, supplemental material

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 samples 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 Fcmm'm'. 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., Comment: Accepted for publication in Physical Review B; 12 pages, 13 figures, 2 tables

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., Comment: 4 pages, 5 figures