Neutron diffraction measurements have been performed on a powder sample of BaMn2As2 over the temperature T range from 10 K to 675 K. These measurements demonstrate that this compound exhibits collinear antiferromagnetic ordering below the Neel temper
ature T_N = 625(1) K. The ordered moment mu = 3.88(4) mu_B/Mn at T = 10 K is oriented along the c axis and the magnetic structure is G-type, with all nearest-neighbor Mn moments antiferromagnetically aligned. The value of the ordered moment indicates that the oxidation state of Mn is Mn^{2+} with a high spin S = 5/2. The T dependence of mu suggests that the magnetic transition is second-order in nature. In contrast to the closely related AFe2As2 (A = Ca, Sr, Ba, Eu) compounds, no structural distortion is observed in the magnetically ordered state of BaMn2As2.
Neutron powder diffraction studies of the crystal and magnetic structures of the magnetocaloric compound Mn1.1Fe0.9(P0.8Ge0.2) have been carried out as a function of temperature, applied magnetic field, and pressure. The data reveal that there is onl
y one transition observed over the entire range of variables explored, which is a combined magnetic and structural transformation between the paramagnetic to ferromagnetic phases (Tc~255 K for this composition). The structural part of the transition is associated with an expansion of the hexagonal unit cell in the direction of the a- and b-axes and a contraction of the c-axis as the FM phase is formed, which originates from an increase in the intra-layer metal-metal bond distance. The application of pressure is found to have an adverse effect on the formation of the FM phase since pressure opposes the expansion of the lattice and hence decreases Tc. The application of a magnetic field, on the other hand, has the expected effect of enhancing the FM phase and increasing Tc. We find that the substantial range of temperature/field/pressure coexistence of the PM and FM phases observed is due to compositional variations in the sample. In-situ high temperature diffraction measurements were carried out to explore this issue, and reveal a coexisting liquid phase at high temperatures that is the origin of this variation. We show that this range of coexisting phases can be substantially reduced by appropriate heat treatment to improve the sample homogeneity.
We use bulk magnetic susceptibility, electronic specific heat, and neutron scattering to study structural and magnetic phase transitions in Fe$_{1+y}$Se% $_x$Te$_{1-x}$. Fe$_{1.068}$Te exhibits a first order phase transition near 67 K with a tetragon
al to monoclinic structural transition and simultaneously develops a collinear antiferromagnetic (AF) order responsible for the entropy change across the transition. Systematic studies of FeSe$%_{1-x}$Te$_x$ system reveal that the AF structure and lattice distortion in these materials are different from those of FeAs-based pnictides. These results call into question the conclusions of present density functional calculations, where FeSe$_{1-x}$Te$_x$ and FeAs-based pnictides are expected to have similar Fermi surfaces and therefore the same spin-density-wave AF order.
We use neutron scattering to study the structural distortion and antiferromagnetic (AFM) order in LaFeAsO$_{1-x}$F$_{x}$ as the system is doped with fluorine (F) to induce superconductivity. In the undoped state, LaFeAsO exhibits a structural distort
ion, changing the symmetry from tetragonal (space group $P4/nmm$) to orthorhombic (space group $Cmma$) at 155 K, and then followed by an AFM order at 137 K. Doping the system with F gradually decreases the structural distortion temperature, but suppresses the long range AFM order before the emergence of superconductivity. Therefore, while superconductivity in these Fe oxypnictides can survive in either the tetragonal or the orthorhombic crystal structure, it competes directly with static AFM order.
We report the anisotropic magnetic properties of Ho2Ge2O7 determined from dc and ac magnetization, specific heat and powder neutron diffraction experiments. The magnetic lanthanide sublattice, seen in our refinement of the tetragonal pyrogermanate cr
ystal structure, is a right-handed spiral of edge-sharing and corner-sharing triangles; the local Ho-O coordination indicates that the crystal field is anisotropic. Susceptibility and magnetization data indeed show that the magnetism is highly anisotropic, and the magnetic structure has the Ho moments confined to the plane perpendicular to the structural spiral. The ordered moment of Ho3+, as determined from refinement of the neutron diffraction data, is 9.0 mu_B. Magnetic ordering occurs around 1.6 K. Temperature and field dependent ac susceptibility measurements show that this compound displays spin relaxation phenomena analogous to what is seen in the spin ice pyrochlore system Ho2Ti2O7.
Magnetic spin fluctuations is one candidate to produce the bosonic modes that mediate the superconductivity in the ferrous superconductors. Up until now, all of the LaOFeAs and BaFe2As2 structure types have simple commensurate magnetic ground states,
as result of nesting Fermi surfaces. This type of spin-density-wave (SDW) magnetic order is known to be vulnerable to shifts in the Fermi surface when electronic densities are altered at the superconducting compositions. Superconductivity has more recently been discovered in alpha-Fe(Te,Se), whose electronically active antifluorite planes are isostructural to the FeAs layers found in the previous ferrous superconductors and share with them the same quasi-two-dimensional electronic structure. Here we report neutron scattering studies that reveal a unique complex incommensurate antiferromagnetic order in the parent compound alpha-FeTe. When the long-range magnetic order is suppressed by the isovalent substitution of Te with Se, short-range correlations survive in the superconducting phase.
We use powder neutron diffraction to study the spin and lattice structures of polycrystalline samples of nonsuperconducting PrFeAsO and superconducting PrFeAsO0.85F0.15 and PrFeAsO0.85. We find that PrFeAsO exhibits an abrupt structural phase transit
ions at 153 K, followed by static long range antiferromagnetic order at 127 K. Both the structural distortion and magnetic order are identical to other rare-earth oxypnictides. Electron-doping the system with either Fluorine or oxygen deficiency suppresses the structural distortion and static long range antiferromagnetic order, therefore placing these materials into the same class of FeAs-based superconductors.
The transition temperature Tc~26 K of the recently discovered superconductor LaFeAs(O,F) has been demonstrated to be extremely sensitive to the lanthanide ion, reaching 55 K for the Sm containing oxypnictides. Therefore, it is important to determine
how the moment on the lanthanide affects the overall magnetism in these systems. Here we report a neutron diffraction study of the Nd oxypnictides. Long ranged antiferromagnetic order is apparent in NdFeAsO below 1.96 K. Rietveld refinement shows that both Fe and Nd magnetic ordering are required to describe the observed data with the staggered moment 1.55(4) Bohr magneton per Nd and 0.9(1) Bohr magneton per Fe at 0.3 K. The other structural properties such as the tetragonal-orthorhombic distortion are found to be very similar to those in LaFeAsO. Neither the magnetic ordering nor the structural distortion occur in the superconducting sample NdFeAsO0.80F0.20 at any temperatures down to 1.5 K.
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 la
yers 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 reported and possess a Tc~38 K. Here, we report the neutron diffraction studies of BaFe2As2 that shows, in contrast to previous studies on the LnFeAsO materials, an antiferromagnetic transition which concurs with first-order structural transition. Although the magnetic and structural transitions occur differently in the AFe2As2 and LnFeAsO-type materials, this work clearly demonstrates that the complete evolution to a low symmetry structure is a pre-requirement for the magnetic order.
We use neutron scattering to study the structural and magnetic phase transitions in the iron pnictides CeFeAsO1-xFx as the system is tuned from a semimetal to a high-transition-temperature (high-Tc) superconductor through Fluorine (F) doping x. In th
e undoped state, CeFeAsO develops a structural lattice distortion followed by a stripe like commensurate antiferromagnetic order with decreasing temperature. With increasing Fluorine doping, the structural phase transition decreases gradually while the antiferromagnetic order is suppressed before the appearance of superconductivity, resulting an electronic phase diagram remarkably similar to that of the high-Tc copper oxides. Comparison of the structural evolution of CeFeAsO1-xFx with other Fe-based superconductors reveals that the effective electronic band width decreases systematically for materials with higher Tc. The results suggest that electron correlation effects are important for the mechanism of high-Tc superconductivity in these Fe pnictides.
