Strong coupling between magnetic and structural order parameters in SrFe2As2
A. Jesche, N. Caroca-Canales, H. Rosner, H. Borrmann, A. Ormeci, D. Kasinathan, K. Kaneko, H. H. Klauss, H. Luetkens, R. Khasanov, A. Amato, A. Hoser, C. Krellner, C. Geibel
X-ray and Neutron diffraction as well as muon spin relaxation and Mössbauer experiments performed on SrFe$_2$As$_2$ polycrystalls confirm a sharp first order transition at $T_0 = 205$,K corresponding to an orthorhombic phase distortion and to a columnar antiferromagnetic Fe ordering with a propagation vector (1,0,1), and a larger distortion and larger size of the ordered moment than reported for BaFe$_2$As$_2$. The structural and the magnetic order parameters present an remarkable similarity in their temperature dependence from $T_0$ down to low temperatures, showing that both phenomena are intimately connected. Accordingly, the size of the ordered Fe moments scale with the lattice distortion when going from SrFe$_2$As$_2$ to BaFe$_2$As$_2$. Full-potential band structure calculations confirm that the columnar magnetic order and the orthorhombic lattice distortion are intrinsically tied to each other.
We constructed, by the first-principles calculations, a magnetic phase diagram of Sr$_{2}$RuO$_4$ in the space spanned by structural distortions. Our phase diagram can qualitatively explain the experimental one for Ca$_{2-x}$Sr$_x$RuO$_4$. We found that the rotation and the tilting of RuO$_6$ octahedron are responsible for the ferro- and antiferro-magnetism, respectively, while the flattening of RuO$_6$ is the key factor to stabilize those magnetic ground states. Our results imply that the magnetic and the structural instabilities in Sr$_2$RuO$_4$ are closely correlated cooperatively rather th…
The extensive ab initio total energy calculations using the VASP-PAW method with the generalized gradient approximation (GGA) for the exchange-correlation potential are applied to systematic investigation of structural, electronic and magnetic properties in quaternary oxybismuthides LaOMBi (where M = Sc, Ti...Ni, Cu). The energy spectrum features similar to lanthanum-iron oxyarsenide LaOFeAs and non-magnetic ground state are indicative of superconductivity possible in lanthanum-nickel oxybismuthide LaONiBi.
We discuss the role of striction in the intertwined magnetic and structural phase transitions in the underdoped iron-pnictides. The magneto-elastic coupling to acoustic modes is then derived and estimated in framework of the multiband spectrum for itinerant electrons with nesting features. We argue that the 1-st order character of the magneto-elastic phase transition originates from the lattice instabilities near the onset of spin-density wave order introducing, thus, a shear acoustic mode as a new order parameter. Taking non-harmonic termis in the lattice energy into account may explain the s…
The antiferromagnetic order and structural distortion in the LaFe(As1-xSbx)O system have been investigated by powder neutron diffraction and physical properties measurements. Polycrystalline samples of LaFe(As1-xSbx)O (x<0.5) were prepared using solid state synthesis at ambient and high pressure. We find that the isoelectronic substitution of Sb for As decreases the structural and magnetic transition temperatures but, contrary to the effects of phosphorus substitution, superconductivity is not induced. Instead a slight increase in the Fe magnetic moment is observed.
Resistivity, specific heat and magnetic susceptibility measurements performed on SrFe2As2 samples evidence a behavior very similar to that observed in LaFeAsO and BaFe2As2 with the difference that the formation of the SDW and the lattice deformation occur in a pronounced first order transition at T_0=205K. Comparing further data evidences that the Fe-magnetism is stronger in SrFe2As2 and in EuFe2As2 than in the other layered FeAs systems investigated up to now. Full potential LDA band structure calculations confirm the large similarity between the compounds, especially for the relevant low ene…
We report measurements of structural phase transition of four parent compounds $R$FeAsO ($R$ = La, Sm, Gd, and Tb) by means of low-temperature X-ray diffraction (XRD). Magnetic transition temperatures associated with Fe ions ($T_{N1}$) are also determined from the temperature dependence of resistivity. As $R$ is changed from La, through Sm and Gd, to Tb, both the c-axis and a-axis lattice constants decrease significantly. Meanwhile both the structural phase transition temperature ($T_S$) and $T_{N1}$ decrease monotonously. It is also found that the temperature gap between $T_S$ and $T_{N1}$ be…
We have performed extensive ab initio calculations to investigate phonon dynamics and their possible role in superconductivity in BaFe2As2 and related systems. The calculations are compared to inelastic neutron scattering data that offer improved resolution over published data [Mittal et al., PRB 78 104514 (2008)], in particular at low frequencies. Effects of structural phase transition and full/partial structural relaxation, with and without magnetic ordering, on the calculated vibrational density of states are reported. Phonons are best reproduced using either the relaxed magnetic structures…
NaFeAs belongs to a class of Fe-based superconductors which parent compounds show separated structural and magnetic transitions. Effects of the structural transition on spin dynamics therefore can be investigated separately from the magnetic transition. A plateau in dynamic spin response is observed in a critical region around the structural transition temperature T_S. It is interpreted as due to the stiffening of spin fluctuations along the in-plane magnetic hard axis due to the dxz and dyz orbital ordering. The appearance of anisotropic spin dynamics in the critical region above the T_S at T…
In the present paper, we report a comparison study of SrFe$_2$As$_2$ and SrFeAsF using Mössbauer spectroscopy. The temperature dependence of the magnetic hyperfine field is fitted with a modified Bean-Rodbell model. The results give much smaller magnetic moment and magneto-structural coupling effect for SrFeAsF, which may be understood as due to different inter-layer properties of the two compounds.
The physical properties and structural evolution of the MX$_2$-type solid solution Au$_{1-x}$Pd$_x$Te$_2$ are reported. The end member AuTe$_2$ is a normal metal with a monoclinic distorted CdI$_2$-type structure with preformed Te-Te dimers. A monoclinic--trigonal structural phase transition at a finite temperature occurs upon Pd substitution and is suppressed to zero temperature near $x$ = 0.55, and a superconducting phase with a maximum $T_{\rm c}$ = 4.65 K emerges. A clear indication of strong coupling superconductivity is observed near the composition of the structural instability. The com…
A phase diagram of superconducting Sr(Fe$_{1-x}$Co$_x$)$_2$As$_2$ as a function of doping (x) is determined by a series of thermodynamic and transport measurements on single crystals. On comparison with a similar phase diagram for Ba(Fe$_{1-x}$Co$_x$)$_2$As$_2$ (Co-doped Ba122), we find that the increased dimensionality of Co-doped Sr122 results in a single first-order-like transition where the magnetic and structural transitions coincide, unlike the case of Co-doped Ba122 that exhibits split quasicontinuous magnetic and structural transitions. We relate this dimensionally-tuned splitting in t…
The phase diagram of Ca$_{2-x}$Sr$_x$RuO$_4$ has been studied by neutron diffraction on powder and single-crystalline samples. The experiments reveal antiferromagnetic order and structural distortions characterized by tilts and rotations of the RuO$_6$-octahedra. There is strong evidence that the structural details of the isovalent samples tune the magnetic as well as the electronic behavior. In particular we observe for low Sr-concentration a metal insulator transition associated with a structural change and magnetic ordering.
In this paper we present detailed Mössbauer spectroscopy study of structural and magnetic properties of the undoped parent compound CaFe$_2$As$_2$ single crystal. By fitting the temperature dependence of the hyperfine magnetic field we show that the magneto-structural phase transition is clearly first-order in nature and we also deduced the compressibility of our sample to be $1.67\times10^{-2}\,GPa^{-1}$. Within the Landau's theory of phase transition, we further argue that the observed phase transition may stem from the strong magneto-structural coupling effect. Temperature dependence of the…
We present a systematic investigation of the antiferromagnetic ordering and structural distortion for the series of Ba(Fe{1-x}Ru{x})2As2 compounds (0 <= x <= 0.246). Neutron and x-ray diffraction measurements demonstrate that, unlike for the electron-doped compounds, the structural and magnetic transitions remain coincident in temperature. Both the magnetic and structural transitions are gradually suppressed with increased Ru concentration and coexist with superconductivity. For samples that are superconducting, we find strong competition between superconductivity, the antiferromagnetic orderi…
Neutron diffraction and muon spin relaxation measurements are used to obtain a detailed phase diagram of Pr(Fe,Ru)AsO. The isoelectronic substitution of Ru for Fe acts effectively as spin dilution, suppressing both the structural and magnetic phase transitions. The temperature of the tetragonal-orthorhombic structural phase transition decreases gradually as a function of x. Slightly below the transition temperature coherent precessions of the muon spin are observed corresponding to static magnetism, possibly reflecting a significant magneto-elastic coupling in the FeAs layers. Short range orde…
Commonalities among the order parameters of the ubiquitous antiferromagnetism present in the parent compounds of the iron arsenide high temperature superconductors are explored. Additionally, comparison is made between the well established two-dimensional Heisenberg-Ising magnet, K$_2$NiF$_4$ and iron arsenide systems residing at a critical point whose structural and magnetic phase transitions coincide. In particular, analysis is presented regarding two distinct classes of phase transition behavior reflected in the development of antiferromagnetic and structural order in the three main classes…
We report the structural and magnetic phase transitions of triclinic Ca10(FeAs)10(Pt3As8). High-resolution X-ray powder diffraction reveals splitting of the in-plane (a,b) lattice parameters at Ts ~ 120 K. Platinum-doping weakens the distortion and shifts the transition temperature to 80 K in Ca10(Fe1-xPt_xAs)10(Pt3As8) with x = 0.03. muSR experiments show the onset of magnetic order near Ts and a broad magnetic phase transition. No symmetry breaking is associated to the structural transition in Ca10(FeAs)10(Pt3As8) in contrast to the other parent compounds of iron arsenide superconductors.
The electronic structure of NaFeAs is studied with angle resolved photoemission spectroscopy on high quality single crystals. Large portions of the band structure start to shift around the structural transition temperature, and smoothly evolve as the temperature lowers through the spin density wave transition. Moreover, band folding due to magnetic order emerges around structural transition. Our observation provides direct evidence that the structural and magnetic transitions share the same origin, and are both driven by the electronic structure reconstruction in Fe-based superconductors, inst…
We present here high resolution magnetization measurements on high-quality BaFe$_{2(1-x)}$Co$_{2x}$As$_{2}$, 0$\leq$x$\leq$0.046 as-grown single crystals. The results confirm the existence of a magnetic tricritical point in the ($x$,$T$) plane at x$^{m}_{tr}$$\approx$0.022 and reveal the emergence of the heat capacity anomaly associated with the onset of the structural transition at x$^{s}$$\approx$0.0064. We show that the samples with doping near x$^{m}_{tr}$ do not show superconductivity, but rather superconductivity emerges at a slightly higher cobalt doping, x$\approx$0.0315
In addition to higher Tc compared with the ubiquitous cuprates for a material composed of a single electronically active layer, the newly discovered LnFeAsO superconductors offer additional compositional variation. In a similar fashion to the CuO2 layers in cuprates, the FeAs layers now dominate the electronic states that produce superconductivity. Cuprate superconductors distinguish themselves structurally by adopting different stacking of the Cu-O and electronically inactive "spacer" layers. Using the same structural philosophy, materials with the formula (A,K)Fe2As2,A=Ba or Sr have been rep…
Single crystals of Fe(1+x)Te(1-y)Se(y) have been grown with a controlled Fe excess and Se doping, and the crystal structure has been refined for various compositions. The systematic investigation of magnetic and superconducting properties as a function of the structural parameters shows how the material can be driven into various ground states, depending on doping and the structural modifications. Our results prove that the occupation of the additional Fe site, Fe2, enhances the spin localization. By reducing the excess Fe, the antiferromagnetic ordering is weakened, and the superconducting gr…
Study and comparison of over 30 examples of electron doped BaFe2As2 for transition metal (TM) = Co, Ni, Cu, and (Co/Cu mixtures) have lead to an understanding that the suppression of the structural/antiferromagnetic phase transition to low enough temperature in these compounds is a necessary condition for superconductivity, but not a sufficient one. Whereas the structural/antiferromagnetic transitions are suppressed by the number of TM dopant ions (or changes in the c-axis) the superconducting dome exists over a limited range of values of the number of electrons added by doping (or values of t…
Specific heat, resistivity, magnetic susceptibility, linear thermal expansion (LTE), and high-resolution synchrotron X-ray powder diffraction investigations of single crystals Fe1+yTe (0.06 < y < 0.15) reveal a splitting of a single, first-order transition for y < 0.11 into two transitions for y > 0.12. Most strikingly, all measurements on identical samples Fe1.13Te consistently indicate that, upon cooling, the magnetic transition at T_N precedes the first-order structural transition at a lower temperature T_s. The structural transition in turn coincides with a change in the character of the m…
We report time-of-flight neutron powder diffraction results on stoichiometric BaFe2As2. Pair distribution function analysis shows that the orthorhombic distortion in the a-b plane at short distances are significantly different from the average lattice distortion, indicating local variations in the lattice at the short-range. We propose that this local variation reflects a high density of nano-twins, short-ranged structures which locally affect the magnetic alignment. This results suggests that the discrepancies between the observed and calculated magnetic moments in BaFe2As2 arise partly from …
The interplay between the structural and magnetic phase transitions occurring in the Fe-based pnictide superconductors is studied within a Ginzburg-Landau approach. We show that the magnetoelastic coupling between the corresponding order parameters is behind the salient features observed in the phase diagram of these systems. This naturally explains the coincidence of transition temperatures observed in some cases as well as the character (first or second-order) of the transitions. We also show that magnetoelastic coupling is the key ingredient determining the collinearity of the magnetic orde…
We present the results of an investigation of both the magnetic and structural phase transitions in a high quality single crystalline sample of the undoped, iron pnictide compound BaFe$_2$As$_2$. Both phase transitions are characterized via neutron diffraction measurements which reveal simultaneous, continuous magnetic and structural orderings with no evidence of hysteresis, consistent with a single second order phase transition. The onset of long-range antiferromagnetic order can be described by a simple power law dependence $ϕ(T)^2\propto(1-\frac{T}{T_N})^{2β}$ with $β=0.103\pm0.018$; a valu…
We report neutron scattering experiments probing the influence of uniaxial strain on both the magnetic and structural order parameters in the parent iron pnictide compound, BaFe$_2$As$_2$. Our data show that modest strain fields along the in-plane orthorhombic b-axis can affect significant changes in phase behavior simultaneous to the removal of structural twinning effects. As a result, we demonstrate in BaFe$_2$As$_2$ samples detwinned via uniaxial strain that the in-plane C$_4$ symmetry is broken by \textit{both} the structural lattice distortion \textit{and} long-range spin ordering at temp…
We show that the strong hybridization between the iron 3d and the arsenic 4p orbitals, in the newly discovered iron-based high-T$_{c}$ superconductors, leads to an explanation of certain experimental observations that are presently not well understood. The existence of a lattice distortion, the smallness of the Fe magnetic moment in the undoped systems, and the suppression of both the lattice distortion and the magnetic order upon doping with fluorine, are all shown to result from this hybridization.
A neutron scattering study of nonsuperconducting La$_{2-x}$Sr$_x$CaCu$_2$O$_6$ (x=0 and 0.2), a bilayer copper oxide without CuO chains, has revealed an unexpected tetragonal-to-orthorhombic transition with a doping dependent transition temperature. The predominant structural modification below the transition is an in-plane shift of the apical oxygen. In the doped sample, the orthorhombic superstructure is strongly disordered, and a glassy state involving both magnetic and structural degrees of freedom develops at low temperature. The spin correlations are commensurate.
Using an adapted Sn-flux growth technique we obtained comparatively large CeFeAsO single crystals of better quality than previously reported polycrystals or single crystals, as evidenced by much sharper anomalies at the structural and magnetic phase transitions as well as a much higher residual resistivity ratio of 12. In the magnetically ordered phase we observe a very pronounced metallic behavior of the in-plane resistivity, which excludes a Mott insulator regime at low temperature. The separation Delta_T = T_0 - T_N between structural and magnetic ordering temperatures decreases with increa…
We report a clear anomaly in the rf response of a tunnel-diode resonator measured in borocarbide crystals in dc fields along the $c-$axis. We associate the anomaly in the dynamic magnetic susceptibility, $χ$, with a structural transition in the vortex lattice. $χ$ is sensitive to the Campbell penetration depth $λ_{C}$ of the rf perturbation into the mixed state. $λ_{C}$ depends on the vortex lattice elastic moduli, which in turn depend on the vortex lattice structure. The high-field transition line is clearly mapped and shown to behave in agreement with theory.
We present calculations of structural and magnetic properties of the iron-pnictide superconductor LaFeAsO including electron-electron correlations. For this purpose we apply a fully charge self-consistent combination of Density-Functional Theory with the Dynamical Mean-Field theory, allowing for the calculation of total energies. We find that the inclusion of correlation effects gives a good agreement of the Arsenic z position with experimental data even in the paramagnetic (high-temperature) phase. Going to low temperatures, we study the formation of the ordered moment in the striped spin-den…
The family of the superconducting quasi-skutterudites (Ca$_x$Sr$_{1-x}$)$_3$Rh$_4$Sn$_{13}$ features a structural quantum critical point at $x_c=0.9$, around which a dome-shaped variation of the superconducting transition temperature $T_c$ is found. Using specific heat, we probe the normal and the superconducting states of the entire series straddling the quantum critical point. Our analysis indicates a significant lowering of the effective Debye temperature on approaching $x_c$, which we interpret as a result of phonon softening accompanying the structural instability. Furthermore, a remarkab…
The mechanism of electron pairing in high-temperature superconductors is still the subject of intense debate. Here, we provide direct evidence of the role of structural dynamics, with selective atomic motions (buckling of copper-oxygen planes), in the anisotropic electronlattice coupling. The transient structures were determined using time-resolved electron diffraction, following carrier excitation with polarized femtosecond heating pulses, and examined for different dopings and temperatures. The deformation amplitude reaches 0.5 % of the c-axis value of 30 A when the light polarization is in …
