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We study composites of monodisperse ferrimagnetic nanoparticles (NPs) embedded into ferroelectric barium titanate (BTO) films. The BTO films were prepared by pulsed laser deposition. The composite consists of a stack of two BTO films sandwiching one monolayer of iron oxide NPs. We observe a magnetoelectric coupling due to strain and interface charge co-mediation between the BTO and the NPs. This is demonstrated by measurements of the magnetization as function of DC and AC electric fields.

By performing high-pressure single-crystal neutron diffraction measurements, the evolution of structure and magnetic ordering in EuFe2As2 under hydrostatic pressure were investigated. Both the tetragonal-toorthorhombic structural transition and the Fe spin-density-wave (SDW) transition are gradually suppressed and become decoupled with increasing pressure. The antiferromagnetic order of the Eu sublattice is, however, robust against the applied pressure up to 24.7 kbar, without showing any change of the ordering temperature. Under the pressure of 24.7 kbar, the lattice parameters of EuFe2As2 display clear anomalies at 27(3) K, well consistent with the superconducting transition observed in previous high-pressure resistivity measurements. Such an anomalous thermal expansion around Tc strongly suggests the appearance of bulk superconductivity and strong electron-lattice coupling in EuFe2As2 induced by the hydrostatic pressure. The coexistence of long-range ordered Eu-antiferromagnetism and pressure-induced superconductivity is quite rare in the EuFe2As2-based iron pnictides., Comment: 6 pages, 4 figures

The Co2V2O7 is recently reported to exhibit amazing magnetic field-induced magnetization plateaus and ferroelectricity, but its magnetic ground state remains ambiguous due to its structural complexity. Magnetometry measurements, and time-of-flight neutron powder diffraction (NPD) have been employed to study the structural and magnetic properties of Co2V2O7, which consists of two non-equivalent Co sites. Upon cooling below the Ne\'el temperature TN = 6.3 K, we observe magnetic Bragg peaks at 2K in NPD which indicated the formation of long range magnetic order of Co2+ moments. After symmetry analysis and magnetic structure refinement, we demonstrate that Co2V2O7 possesses a complicated non-collinear magnetic ground state with Co moments mainly located in b-c plane and forming a non-collinear spin-chain-like structure along the c-axis. The ab initio calculations demonstrate that the non-collinear magnetic structure is more stable than various ferromagnetic states at low temperature. The non-collinear magnetic structure with canted up-up-down-down spin configuration is considered as the origin of magnetoelectric coupling in Co2V2O7 because the inequivalent exchange striction induced by the spin-exchange interaction between the neighboring spins is the driving force of ferroelectricity. Besides, it is found that the deviation of lattice parameters a and b is opposite below TN, while the lattice parameter c and stay almost constant below TN, evidencing the anisotropic magnetoelastic coupling in Co2V2O7., Comment: 9 pages, 8 figures

The study of universal critical behavior is a crucial issue in a continuous phase transition, which groups various critical phenomena into universality classes for revealing microscopic electronic behaviors. The understanding of the nature of magnetism in Eu-based ferromagnetic superconductors is largely impeded by the infeasibility of performing inelastic neutron scattering measurements to deduce the microscopic magnetic behaviors and the effects on the superconductivity, due to the significant neutron absorption effect of natural $^{152}$Eu and unavailability of large single crystals. However, by systematically combining the neutron diffraction experiment, the first-principles calculations, and the quantum Monte Carlo simulations, we have obtained a perfectly consistent universal critical exponent value of $\beta=0.385(13)$ experimentally and theoretically for Eu(Fe$_{0.75}$Ru$_{0.25}$)$_{2}$As$_{2}$, from which the magnetism in the Eu-based ferromagnetic superconductors is identified as the universal class of a three-dimensional anisotropic quantum Heisenberg model with long-range magnetic exchange coupling. This study not only clarifies the nature of microscopic magnetic behaviors in the Eu-based ferromagnetic superconductors, but also opens a new avenue of systemic methodology for studying the universal critical behaviors associated with magnetic phase transitions in the area of magnetism and the spin fluctuations effects on the unconventional superconductivity., Comment: 6 pages, 4 figures, 1 table

Using complementary polarized and unpolarized single-crystal neutron diffraction, we have investigated the temperature-dependent magnetic structures of Eu$_{0.5}$Ca$_{0.5}$Fe$_{2}$As$_{2}$. Upon 50 \% dilution of the Eu sites with isovalent Ca$^{2+}$, the Eu sublattice is found to be still long-range ordered below $\mathit{T_{Eu}}$ = 10 K, in the A-typed antiferromagnetic (AFM) structure. The moment size of Eu$^{2+}$ spins is estimated to be as large as 6.74(4) $\mu_{B}$ at 2.5 K. The Fe sublattice undergoes a spin-density-wave transition at $\mathit{T_{SDW}}$ = 192(2) K and displays an in-plane AFM structure above $\mathit{T_{Eu}}$. However, at 2.5 K, the Fe$^{2+}$ moments are found to be ordered in a canted AFM structure with a canting angle of 14(4){\deg} out of the $\mathit{ab}$ plane. The spin reorientation of Fe below the AFM ordering temperature of Eu provides a direct evidence of a strong interplay between the two magnetic sublattices in Eu$_{0.5}$Ca$_{0.5}$Fe$_{2}$As$_{2}$., Comment: 6 pages, 5 figures, Accepted by Phys. Rev. B (Rapid Communication)

The ground-state magnetic structure of EuNi$_{2}$As$_{2}$ was investigated by single-crystal neutron diffraction. At base temperature, the Eu$^{2+}$ moments are found to form an incommensurate antiferromagnetic spiral-like structure with a magnetic propagation vector of $\mathit{k}$ = (0, 0, 0.92). They align ferromagnetically in the $\mathit{ab}$ plane with the moment size of 6.75(6) $\mu_{B}$, but rotate spirally by 165.6(1){\deg} around the $\mathit{c}$ axis from layer to layer. The magnetic order parameter in the critical region close to the ordering temperature, $\mathit{T_{N}}$ = 15 K, shows critical behavior with a critical exponent of $\beta_{Eu}$ = 0.34(1), consistent with the three-dimensional Heisenberg model. Moreover, within the experimental uncertainty, our neutron data is consistent with a model in which the Ni sublattice is not magnetically ordered., Comment: 6 pages, 5 figures

We report about the magnetic properties of antiferromagnetic (AF) MnO nanoparticles (NPs) with different sizes (6-19nm). Using a combination of polarized neutron scattering and magnetometry we were able to resolve previously observed peculiarities. Magnetometry, on the one hand, reveals a peak in the zero field cooled (ZFC) magnetization curves at low temperatures (~25K) but no feature around the N\'eel temperature at 118K. On the other hand, polarized neutron scattering shows the expected behavior of the AF order parameter vanishing around 118K. Moreover, hysteresis curves measured at various temperatures reveal an exchange bias effect indicating a coupling of an AF core to a ferromagnetic (FM)-like shell. ZFC data measured at various fields exclude a purely superparamagnetic (SPM) scenario. We conclude that the magnetic behavior of MnO particles can be explained by a superposition of SPM-like thermal fluctuations of the AF-N\'eel vector inside the AF core and a strong magnetic coupling to a ferrimagnetic Mn$_2$O$_3$ or Mn$_3$O$_4$ shell. In addition, we have studied heterodimer ('Janus') particles, where a FM FePt particle is attached to the AF MnO particle. Via the exchange bias effect, the magnetic moment of the FePt subunit is stabilized by the MnO.

The magnetic ground state of the Eu$^{2+}$ moments in a series of Eu(Fe$_{1-x}$Co$_{x}$)$_{2}$As$_{2}$ single crystals grown from the Sn flux has been investigated in detail by neutron diffraction measurements. Combined with the results from the macroscopic properties (resistivity, magnetic susceptibility and specific heat) measurements, a phase diagram describing how the Eu magnetic order evolves with Co doping in Eu(Fe$_{1-x}$Co$_{x}$)$_{2}$As$_{2}$ is established. The ground-state magnetic structure of the Eu$^{2+}$ spins is found to develop from the A-type antiferromagnetic (AFM) order in the parent compound, via the A-type canted AFM structure with some net ferromagnetic (FM) moment component along the crystallographic $\mathit{c}$ direction at intermediate Co doping levels, finally to the pure FM order at relatively high Co doping levels. The ordering temperature of Eu declines linearly at first, reaches the minimum value of 16.5(2) K around $\mathit{x}$ = 0.100(4), and then reverses upwards with further Co doping. The doping-induced modification of the indirect Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction between the Eu$^{2+}$ moments, which is mediated by the conduction $\mathit{d}$ electrons on the (Fe,Co)As layers, as well as the change of the strength of the direct interaction between the Eu$^{2+}$ and Fe$^{2+}$ moments, might be responsible for the change of the magnetic ground state and the ordering temperature of the Eu sublattice. In addition, for Eu(Fe$_{1-x}$Co$_{x}$)$_{2}$As$_{2}$ single crystals with 0.10 $\leqslant$ $\mathit{x}$ $\leqslant$ 0.18, strong ferromagnetism from the Eu sublattice is well developed in the superconducting state, where a spontaneous vortex state is expected to account for the compromise between the two competing phenomena., Comment: 10 pages, 9 figures

We report a comprehensive specific heat and inelastic neutron scattering study to explore the possible origin of multiferroicity in HoCrO$_3$. We have performed specific heat measurements in the temperature range 100 mK - 290 K and inelastic neutron scattering measurements were performed in the temperature range 1.5 - 200 K. From the specific heat data we determined hyperfine splitting at 22.5(2) $\mu$eV and crystal field transitions at 1.379(5) meV, 10.37(4) meV, 15.49(9) meV and 23.44(9) meV, indicating the existence of strong hyperfine and crystal field interactions in HoCrO$_3$. Further, an effective hyperfine field is determined to be 600(3) T. The quasielastic scattering observed in the inelastic scattering data and a large linear term $\gamma=6.3(8)$ mJmol$^{-1}$K$^{-2}$ in the specific heat is attributed to the presence of short range exchange interactions, which is understood to be contributing to the observed ferroelectricity. Further the nuclear and magnetic entropies were computed to be, $\sim$$17.2$ Jmol$^{-1}$K$^{-1}$ and $\sim$34 Jmol$^{-1}$K$^{-1}$, respectively. The entropy values are in excellent agreement with the limiting theoretical values. An anomaly is observed in peak position of the temperature dependent crystal field spectra around 60 K, at the same temperature an anomaly in the pyroelectric current is reported. From this we could elucidate a direct correlation between the crystal electric field excitations of Ho$^{3+}$ and ferroelectricity in HoCrO$_3$. Our present study along with recent reports confirm that HoCrO$_3$, and $R$CrO$_3$ ($R=$ Rare earth) in general, possess more than one driving force for the ferroelectricity and multiferroicity., Comment: 17 pages, 6 figures, published in J. Phys.: Condens. Matter

High resolution inelastic neutron scattering reveals that the elementary magnetic excitations in multiferroic MnWO4 consist of low energy dispersive electromagnons in addition to the well-known spin-wave excitations. The latter can well be modeled by a Heisenberg Hamiltonian with magnetic exchange coupling extending to the 12th nearest neighbor. They exhibit a spin-wave gap of 0.61(1) meV. Two electromagnon branches appear at lower energies of 0.07(1) meV and 0.45(1) meV at the zone center. They reflect the dynamic magnetoelectric coupling and persist in both, the collinear magnetic and paraelectric AF1 phase, and the spin spiral ferroelectric AF2 phase. These excitations are associated with the Dzyaloshinskii-Moriya exchange interaction, which is significant due to the rather large spin-orbit coupling., Comment: 8 pages, 6 figures, accepted for publication in Physical Review B

Using polarized neutron diffraction and x-ray resonant magnetic scattering (XRMS) techniques, multiple phase transitions were revealed in an underdoped, non-superconducting Eu(Fe$_{1-x}$Ir$_{x}$)$_{2}$As$_{2}$ ($\mathit{x}$ = 0.06) single crystal. Compared with the parent compound EuFe$_{2}$As$_{2}$, the tetragonal-to-orthorhombic structural phase transition and the antiferromagnetic order of the Fe$^{2+}$ moments are significantly suppressed to $\mathit{T_{S}}$ = 111 (2) K and $\mathit{T_{N,Fe}}$= 85 (2) K by 6% Ir doping, respectively. In addition, the Eu$^{2+}$ spins order within the $\mathit{ab}$ plane in the A-type antiferromagnetic structure similar to the parent compound. However, the order temperature is evidently suppressed to $\mathit{T_{N,Eu}}$= 16.0 (5) K by Ir doping. Most strikingly, the XRMS measurements at the Ir $\mathit{L_{3}}$ edge demonstrates that the Ir 5$\mathit{d}$ states are also magnetically polarized, with the same propagation vector as the magnetic order of Fe. With $\mathit{T_{N,Ir}}$ = 12.0 (5) K, they feature a much lower onset temperature compared with $\mathit{T_{N,Fe}}$. Our observation suggests that the magnetism of the Eu sublattice has a considerable effect on the magnetic nature of the 5$\mathit{d}$ Ir dopant atoms and there exists a possible interplay between the localized Eu$^{2+}$ moments and the conduction $\mathit{d}$-electrons on the FeAs layers., Comment: 7 pages, 5 figures

The magnetic order of the localized Eu$^{2+}$ spins in optimally-doped Eu(Fe$_{1-x}$Ir$_{x}$)$_{2}$As$_{2}$ ($\mathit{x}$ = 0.12) with superconducting transition temperature $\mathit{T_{SC}}$ = 22 K was investigated by single-crystal neutron diffraction. The Eu$^{2+}$ moments were found to be ferromagnetically aligned along the $\mathit{c}$-direction with an ordered moment of 7.0(1) $\mu_{B}$ well below the magnetic phase transition temperature $\mathit{T_{C}}$ = 17 K. No evidence of the tetragonal-to-orthorhombic structural phase transition was found in this compound within the experimental uncertainty, in which the spin-density-wave (SDW) order of the Fe sublattice is supposed to be completely suppressed and the superconductivity gets fully developed. The ferromagnetic groud state of the Eu$^{2+}$ spins in Eu(Fe$_{0.88}$Ir$_{0.12}$)$_{2}$As$_{2}$ was supported by the first-principles density functional calculation. In addition, comparison of the electronic structure calculations between Eu(Fe$_{0.875}$Ir$_{0.125}$)$_{2}$As$_{2}$ and the parent compound EuFe$_{2}$As$_{2}$ indicates stronger hybridization and more expanded bandwith due to the Ir substitution, which together with the introduction of electrons might work against the Fe-SDW in favor of the superconductivity., Comment: 7 pages, 7 figures, accepted for publication in Physical Review B

The magnetic structure of the Eu2+ moments in the superconducting EuFe2(As1-xPx)2 sample with x = 0.19 has been determined using neutron scattering. We conclude that the Eu2+ moments are aligned along the c direction below T_C = 19.0(1) K with an ordered moment of 6.6(2) mu_B in the superconducting state. An impurity phase similar to the underdoped phase exists within the bulk sample which orders antiferromagnetically below T_N = 17.0(2) K. We found no indication of iron magnetic order, nor any incommensurate magnetic order of the Eu2+ moments in the sample., Comment: Accepted for publication in Phys. Rev. B (regular article)

We re-investigate the magnetically frustrated, {\it diamond-lattice-antiferromagnet} spinels FeAl$_2$O$_4$ and MnAl$_2$O$_4$ using magnetization measurements and diffuse scattering of polarized neutrons. In FeAl$_2$O$_4$, macroscopic measurements evidence a "cusp" in zero field-cooled susceptibility around 13~K. Dynamic magnetic susceptibility and {\it memory effect} experiments provide results that do not conform with a canonical spin-glass scenario in this material. Through polarized neutron scattering studies, absence of long-range magnetic order down to 4~K is confirmed in FeAl$_2$O$_4$. By modeling the powder averaged differential magnetic neutron scattering cross-section, we estimate that the spin-spin correlations in this compound extend up to the third nearest-neighbour shell. The estimated value of the Land\'{e} $g$ factor points towards orbital contributions from Fe$^{2+}$. This is also supported by a Curie-Weiss analysis of the magnetic susceptibility. MnAl$_2$O$_4$, on the contrary, undergoes a magnetic phase transition into a long-range ordered state below $\approx$ 40~K, which is confirmed by macroscopic measurements and polarized neutron diffraction. However, the polarized neutron studies reveal the existence of prominent spin-fluctuations co-existing with long-range antiferromagnetic order. The magnetic diffuse intensity suggests a similar short range order as in FeAl$_2$O$_4$. Results of the present work supports the importance of spin-spin correlations in understanding magnetic response of frustrated magnets like $A$-site spinels which have predominant short-range spin correlations reminiscent of the "spin liquid" state., Comment: 10 pages, 10 figures, double-column, accepted in Phys. Rev. B, 2014

The magnetic structure of the Eu2+ moments in the superconducting EuFe2(As1-xPx)2 sample with x = 0.15 has been determined using element specific x-ray resonant magnetic scattering. Combining magnetic, thermodynamic and scattering measurements, we conclude that the long range ferromagnetic order of the Eu2+ moments aligned primarily along the c axis coexists with the bulk superconductivity at zero field. At an applied magnetic field >= 0.6 T, superconductivity still coexists with the ferromagnetic Eu2+ moments which are polarized along the field direction. We propose a spontaneous vortex state for the coexistence of superconductivity and ferromagnetism in EuFe2(As0.85P0.15)2., Comment: Accepted, Phys. Rev. B

The magnetic structure of superconducting Eu(Fe0.82Co0.18)2As2 is unambiguously determined by single-crystal neutron diffraction. A long-range ferromagnetic order of the Eu2+ moments along the c-direction is revealed below the magnetic phase transition temperature Tc = 17 K. In addition, the antiferromagnetism of the Fe2+ moments still survives and the tetragonal-to-orthorhombic structural phase transition is also observed, although the transition temperatures of the Fe-spin density wave (SDW) order and the structural phase transition are significantly suppressed to Tn = 70 K and Ts = 90 K, respectively, compared to the parent compound EuFe2As2.We present the microscopic evidences for the coexistence of the Eu-ferromagnetism (FM) and the Fe-SDW in the superconducting crystal. The superconductivity (SC) competes with the Fe-SDW in Eu(Fe0.82Co0.18)2As2.Moreover, the comparison between Eu(Fe1-xCox)2As2 and Ba(Fe1-xCox)2As2 indicates a considerable influence of the rare-earth element Eu on the magnetism of the Fe sublattice., Comment: 7 pages, 7 figures, accepted for publication in Physical Review B

We have used polarized and unpolarized neutron diffraction to determine the spatial distribution of the magnetization density induced by a magnetic field of 9 T in the tetragonal phase of K0.8Fe1.6Se2. The maximum entropy reconstruction shows clearly that most of the magnetization is confined to the region around the iron atoms whereas there is no significant magnetization associated with either Se or K atoms. The distribution of magnetization around the Fe atom is slightly nonspherical with a shape which is extended along the [0 0 1] direction in the projection. Multipolar refinement results show that the electrons which give rise to the paramagnetic susceptibility are confined to the Fe atoms and their distribution suggests that they occupy 3d t2g-type orbitals with around 66% in those of xz/yz symmetry. Detail modeling of the magnetic form factor indicates the presence of an orbital moment to the total paramagnetic moment of Fe2+, Comment: 7 pages, accepted for publication in Physical Review B

Inelastic neutron scattering experiments were performed to investigate the crystalline electric field (CEF) excitations of Nd3+ (J = 9/2) in the iron pnictide NdFeAsO. The crystal field level structures for both the high-temperature paramagnetic phase and the low-temperature antiferromagnetic phase of NdFeAsO are constructed. The variation of CEF excitations of Nd3+ reflects not only the change of local symmetry but also the change of magnetic ordered state of the Fe sublattice. By analyzing the crystal field interaction with a crystal field Hamiltonian, the crystal field parameters are obtained. It was found that the sign of the fourth and sixth-order crystal field parameters change upon the magnetic phase transition at 140 K, which may be due to the variation of exchange interactions between the 4f and conduction electrons., Comment: 5 pages, 4 figures

Neutron scattering experiments were performed to investigate magnetic order and magnetic excitations in ternary iron chalcogenide K2Fe4Se5. The formation of a superlattice structure below 580 K together with the decoupling between the Fe-vacancy order-disorder transition and the antiferromagnetic order transition appears to be a common feature in the A2Fe4Se5 family. The study of spin dynamics of K2Fe4Se5 reveals two distinct energy gaps at the magnetic Brillouin zone center, which indicates the presence of magnetic anisotropy and the decrease of local symmetry due to electronic and orbital anisotropy. The low-energy spin wave excitations of K2Fe4Se5 can be properly described by linear spin wave theory within a Heisenberg model. Compared to iron pnictides, K2Fe4Se5 exhibits a more two-dimensional magnetism as characterized by large differences not only between out-of-plane and in-plane spin wave velocities, but also between out-of-plane and in-plane exchange interactions., Comment: 5 pages, 4 figures, Accepted for publication, Physical Review B: Rapid Communications

We report measurements of the temperature dependence of phonon densities of states in K0.8Fe1.6Se2 using inelastic neutron scattering technique. While cooling down to 150 K, a phonon peak splitting around 25 meV is observed and a new peak appears at 31 meV. The measurements support the recent Raman and infra-red measurements indicating a lowering of symmetry of K0.8Fe1.6Se2 upon cooling below 250 K. Ab-initio phonon calculations have been carried out for K0.8Fe1.6Se2 and KFe2Se2. The comparison of the phonon spectra as obtained from the magnetic as well as non magnetic calculations show pronounced differences. We show that in the two calculations the energy range of the vibrational contribution from both Fe and Se are quite different. We conclude that Fe magnetism is correlated to the phonon dynamics and it plays an important role in stabilizing the structure of K0.8Fe1.6Se2 as well as that of KFe2Se2. The calculations highlight the presence of low energy librational modes in K0.8Fe1.6Se2 as compared to KFe2Se2., Comment: 22 pages, 3 Tables, 7 Figures

We have investigated low energy nuclear spin excitations in strongly correlated electron compound HoCrO$_3$. We observe clear inelastic peaks at $E = 22.18 \pm 0.04$ $\mu eV$ in both energy loss and gain sides. The energy of the inelastic peaks remains constant in the temperature range 1.5 - 40 K at which they are observed. The intensity of the inelastic peak increases at first with increasing temperature and then decreases at higher temperatures. The temperature dependence of the energy and intensity of the inelastic peaks is very unusual compared to that observed in other Nd, Co and V compounds. Huge quasielastic scattering appears at higher temperatures presumably due to the fluctuating electronic moments of the Ho ions that get increasingly disordered at higher temperatures.

The magnetic structures adopted by the Fe and Sm sublattices in SmFeAsO have been investigated using element specific x-ray resonant and non-resonant magnetic scattering techniques. Between 110 and 5 K, the Sm and Fe moments are aligned along the c and a directions, respectively according to the same magnetic representation $\Gamma_{5}$ and the same propagation vector (1, 0, 0.5). Below 5 K, magnetic order of both sublattices change to a different magnetic structure and the Sm moments reorder in a magnetic unit cell equal to the chemical unit cell. Modeling of the temperature dependence for the Sm sublattice as well as a change in the magnetic structure below 5 K provide a clear evidence of a surprisingly strong coupling between the two sublattices, and indicate the need to include anisotropic exchange interactions in models of SmFeAsO and related compounds., Comment: 8 pages, 7 figures, accepted for publication in Phys. Rev. B

We report systematic investigation of high pressure crystal structures and structural phase transition upto 46 GPa in CaFeAsF and 40 GPa in SrFeAsF at 40 K using powder synchrotron x-ray diffraction experiments and Rietveld analysis of the diffraction data. We find that CaFeAsF undergoes orthorhombic to monoclinic phase transition at Pc = 13.7 GPa while increasing pressure. SrFeAsF exhibits coexistence of orthorhombic and monoclinic phases over a large pressure range from 9 to 39 GPa. The coexistence of the two phases indicates that the transition is of first order in nature. Unlike in the 122 compounds (BaFe2As2 & CaFe2As2) we do not find any collapse tetragonal transition. The transition to a lower symmetry phase (orthorhombic to monoclinic) in 1111 compounds under pressure is in contrast with the transition to a high symmetry phase (orthorhombic to tetragonal) in 122 type compounds. On heating from 40 K at high pressure, CaFeAsF undergoes monoclinic to tetragonal phase transition around 25 GPa and 200 K. Further, it does not show any post-tetragonal phase transition and remains in the tetragonal phase upto 25 GPa at 300 K. The dPc/dT is found to be positive for the CaFeAsF & CaFe2As2, however the same was not found in case of BaFe2As2. We discuss observations of structural evolution in the context of superconductivity in these and other Fe-based compounds. It appears that the closeness of the Fe-As-Fe bond angle to its ideal tetrahedral value of 109.470 might be associated with occurrence of superconductivity at low temperature., Comment: 23 pages, 11 Figures

KCrF3 represents another prototypical orbital-ordered perovskite, where Cr2+ possesses the same electronic configuration of 3d4 as that of strongly Jahn-Teller distorted Mn3+ in many CMR manganites. The crystal and magnetic structures of KCrF3 compound are investigated by using polarized and unpolarized neutron powder diffraction methods. The results show that the KCrF3 compound crystallizes in tetragonal structure at room temperature and undergoes a monoclinic distortion with the decrease in temperature. The distortion of the crystal structure indicates the presence of cooperative Jahn-Teller distortion which is driven by orbital ordering. With decreasing temperature, four magnetic phase transitions are observed at 79.5, 45.8, 9.5, and 3.2 K, which suggests a rich magnetic phase diagram. Below T_N = 79.5 K, the Cr2+ moment orders in an incommensurate antiferromagnetic arrangement, which can be defined by the magnetic propagation vector (1/2$\pm\,$$\delta\,$, 1/2$\pm\,$$\delta\,$, 0). The incommensurate-commensurate magnetic transition occurs at 45.8 K and the magnetic propagation vector locks into (1/2, 1/2, 0) with the Cr moment of 3.34(5) $\mu_B \,$ aligned ferromagnetically in (220) plane, but antiferromagnetically along [110] direction. Below 9.5 K, the canted antiferromagnetic ordering and weak ferromagnetism arise from the collinear antiferromagnetic structure, while the Dzyaloshinskii-Moriya interaction and tilted character of the single-ion anisotropy might give rise to the complex magnetic behaviors below 9.5 K.

We report high pressure powder synchrotron x-ray diffraction studies on MFe2As2 (M=Ba, Ca) over a range of temperatures and pressures up to about 56 GPa using a membrane diamond anvil cell. A phase transition to a collapsed tetragonal phase is observed in both compounds upon compression. However, at 300 (33) K in the Ba-compound the transition occurs at 26 (29) GPa, which is a much higher pressure than 1.7 (0.3) GPa at 300 (40) K in the Ca-compound, due to its larger volume. It is important to note that the transition in both compounds occurs when they are compressed to almost the same value of the unit cell volume and attain similar ct/at ratios. We also show that the FeAs4 tetrahedra are much less compressible and more distorted in the collapsed tetragonal phase than their nearly regular shape in the ambient pressure phase. We present a detailed analysis of the pressure dependence of the structures as well as equation of states in these important BaFe2As2 and CaFe2As2 compounds., Comment: 26 pages, 12 figures

We have studied a EuFe2As2 single crystal by neutron diffraction under magnetic fields up to 3.5 T and temperatures down to 2 K. A field induced spin reorientation is observed in the presence of a magnetic field along both the a and c axes, respectively. Above critical field, the ground state antiferromagnetic configuration of Eu$^{2+}$ moments transforms into a ferromagnetic structure with moments along the applied field direction. The magnetic phase diagram for Eu magnetic sublattice in EuFe2As2 is presented. A considerable strain ($\sim$0.9%) is induced by the magnetic field, caused by the realignment of the twinning structure. Furthermore, the realignment of the twinning structure is found to be reversible with the rebound of magnetic field, which suggested the existence of magnetic shape-memory effect. The Eu moment ordering exhibits close relationship with the twinning structure. We argue that the Zeeman energy in combined with magnetic anisotropy energy is responsible for the observed spin-lattice coupling., Comment: 5 pages, 4 figures

We present single-crystal neutron-diffuse-scattering measurements with polarization analysis on the spin ice Ho2-xYxTi2O7 (x = 0, 0.3, and 1). At 2 K, the spin flip scattering patterns are typical of a nearest-neighbor spin ice and the effects of Y doping are seen in the width of the pinch points. At low-T, the spin flip patterns are characteristic of a dipolar spin ice and are unaffected by Y doping. In the non-spin flip channel, we observe the signature of strong antiferromagnetic correlations at the same T as the dipolar spin ice correlations appear in the spin flip channel. These experimental observations have been well reproduced by our Monte Carlo simulations., Comment: 13 pages, 3 figures

Soft X-ray resonant scattering studies at the Mn $L_{\texttt{II, III}}$- and the La $M_{\texttt{IV, V}}$- edges of single-crystal LaSr$_2$Mn$_2$O$_7$ are reported. At low temperatures, below $T_\texttt{N} \approx 160$ K, energy scans with a fixed momentum transfer at the \emph{A}-type antiferromagnetic (0 0 1) reflection around the Mn $L_{\texttt{II, III}}$-edges with incident linear $\sigma$ and $\pi$ polarizations show strong resonant enhancements. The splitting of the energy spectra around the Mn $L_{\texttt{II, III}}$-edges may indicate the presence of a mixed valence state, e.g., Mn$^{3+}$/Mn$^{4+}$. The relative intensities of the resonance and the clear shoulder-feature as well as the strong incident $\sigma$ and $\pi$ polarization dependences strongly indicate its complex electronic origin. Unexpected enhancement of the charge Bragg (0 0 2) reflection at the La $M_{\texttt{IV, V}}$-edges with $\sigma$ polarization has been observed up to 300 K, with an anomaly appearing around the orbital-ordering transition temperature, $T_{\texttt{OO}} \approx 220$ K, suggesting a strong coupling (competition) between them., Comment: Accepted by European Physical Journal B

We report detailed measurements of temperature dependence and ab initio lattice dynamical calculations of the phonon density-of-states of two Sr based iron pnictide parent compounds; SrFe2As2 and SrFeAsF. Although both compounds undergo a magnetic as well as a tetragonal-to-orthorhombic structural phase transitions, no drastic change of their phonon spectra is found in the temperature range from 2 to 300 K.. In both the systems the Fe-As stretching modes at 32 meV react to the temperature change and shift towards higher energies with decreasing temperature. Furthermore, we found that in the antiferromagnetic phase of SrFe2As2 at 180 K a peak at 25 meV, due to Fe vibrations, moves slightly to higher energies and become narrower on cooling from 300 K. However we did not find any evidence of softening of low energy phonon modes in both SrFe2As2 and SrFeAsF on decreasing the temperature from 300 K in their paramagnetic phase. This is contrary to our earlier observation of phonon softening in CaFe2As2, Ca0.6Na0.4Fe2As2 and Sr0.6K0.4Fe2As2. For the sake of comparison, the previously studied Ca- and Ba-cases are also presented and the role of the magnetic ordering on the calculated phonon spectra in these two families of pnictides is reported., Comment: Paper has been withdrawn by the author. We have submitted new version at arXiv. The new arXiv Ref is arXiv:1007.1711

The magnetic ordering and crystal structure of iron pnictide SrFeAsF was investigated by using neutron powder diffraction method. With decreasing temperature, the tetragonal to orthorhombic phase transition is found at 180 K, while the paramagnetic to antiferromagnetic phase transition set in at 133 K. Similar to the parent compound of other iron pnictide system, the striped Fe magnetism is confirmed in antiferromagnetic phase and the Fe moment of 0.58(6) uB aligned along long a axis. The thermal expansion of orthorhombic phase of SrFeAsF is also investigated. Based on the Grueneisen approximation and Debye approximation for internal energy, the volume of SrFeAsF can be well fitted with Debye temperature of 347(5) K. The experimental atomic displacement parameters for different crystallographic sites in SrFeAsF are analyzed with Debye model. The results suggested that the expansion of FeAs layers plays an important role in determining the thermal expansion coefficient., Comment: 4 pages, 3 figures

The pressure dependence of a large number of phonon modes in CaFe2As2 with energies covering the full range of the phonon spectrum has been studied using inelastic x-ray and neutron scattering. The observed phonon frequency changes are in general rather small despite the sizable changes of the lattice parameters at the phase transition. This indicates that the bonding properties are not profoundly altered by the phase transition. The transverse acoustic phonons propagating along the c-direction are an exception because they stiffen very significantly in response to the large contraction of the c-axis. The lattice parameters are found to change significantly as a function of pressure before, during and after the first-order phase transition. However, the frequencies change nearly uniformly with the change in the lattice parameters due to pressure, with no regard specifically to the first-order phase transition. Density functional theory describes the frequencies in both the zero pressure and in the collapsed phase in a satisfactory way if based on the respective crystal structures.

Among various parent compounds of iron pnictide superconductors, EuFe2As2 stands out due to the presence of both spin density wave of Fe and antiferromagnetic ordering (AFM) of the localized Eu2+ moment. Single crystal neutron diffraction studies have been carried out to determine the magnetic structure of this compound and to investigate the coupling of two magnetic sublattices. Long range AFM ordering of Fe and Eu spins was observed below 190 K and 19 K, respectively. The ordering of Fe2+ moments is associated with the wave vector k = (1,0,1) and it takes place at the same temperature as the tetragonal to orthorhombic structural phase transition, which indicates the strong coupling between structural and magnetic components. The ordering of Eu moment is associated with the wave vector k = (0,0,1). While both Fe and Eu spins are aligned along the long a axis as experimentally determined, our studies suggest a weak coupling between the Fe and Eu magnetism., Comment: 7 pages, 7 figures

Magnetic resonant X ray scattering experiments have been performed on a single crystal of EuFe_2As_2 at the Eu L_3 absorption edge. This has permitted us to determine for the first time the orientation of Eu magnetic moments in the antiferromagnetic ordered phase below T_N=19 K as parallel to the a-axis. In addition, non-resonant magnetic X ray measurements indicate that Fe magnetic moments align along the same direction in the spin density wave phase (T

We report detailed measurements of composition as well as temperature dependence of the phonon density-of-states in a new series of FeAs compounds with composition CaFe1\_{1-x}Co\_{x}AsF (x = 0, 0.06, 0.12). The composition as well as temperature dependence of phonon spectra for CaFe\_{1-x}Co\_{x}AsF (x = 0, 0.06, 0.12) compounds have been measured using time of flight IN4C and IN6 spectrometers at ILL, France. The comparison of phonon spectra at 300 K in these compounds shows that acoustic phonon modes up to 12 meV harden in the doped compounds in comparison to the parent CaFeAsF. While intermediate energy phonon modes from 15 meV to 25 meV are also found to shift towards high energies only in the 12 % Co doped CaFeAsF compound. The experimental results for CaFe\_{1-x}Co\_{x}AsF (x = 0, 0.06, 0.12) are quite different from our previous phonon studies on parent and superconducting MFe2As2 (M=Ba, Ca, Sr) where low-energy acoustic phonon modes do not react with doping, while the phonon spectra in the intermediate range from 15 to 25 K are found to soften in these compounds. We argue that stronger spin phonon interaction play an important role for the emergence of superconductivity in these compounds. The lattice dynamics of CaFe\_{1-x}Co\_{x}AsF (x = 0, 0.06, 0.12) compounds is also investigated using the ab-initio as well as shell model phonon calculations. We show that the nature of the interaction between the Ca and the Fe-As layers in CaFeAsF compounds is quite different compared with our previous studies on CaFe2As2., Comment: 19 pages, 5 figures

We report the pressure and temperature dependence of the phonon density-of-states in superconducting Ca0.6Na0.4Fe2As2 (Tc=21 K) and the parent compound CaFe2As2, using inelastic neutron scattering. We observe no significant change in the phonon spectrum for Ca0.6Na0.4Fe2As2 at 295 K up to pressures of 5 kbar. The phonon spectrum for CaFe2As2 shows softening of the low-energy modes by about 1 meV when decreasing the temperature from 300 K to 180 K. There is no appreciable change in the phonon density of states across the structural and anti-ferromagnetic phase transition at 172 K. These results, combined with our earlier temperature dependent phonon density of states measurements for Ca0.6Na0.4Fe2As2, indicate that the softening of low-energy phonon modes in these compounds may be due to the interaction of phonons with electron or short-range spin fluctuations in the normal state of the superconducting compound as well as in the parent compound. The phonon spectra are analyzed with ab-initio and empirical model calculations giving partial densities of states and dispersion relations., Comment: 14 pages, 6 figures

Extensive inelastic neutron scattering measurements of phonons on a single crystal of CaFe2As2 allowed us to establish a fairly complete picture of phonon dispersions in the main symmetry directions. The phonon spectra were also calculated by density functional theory (DFT) in the local density approximation (LDA). There are serious discrepancies between calculations done for the optimized structure and experiment, because the optimised structure is not the ambient pressure structure but is very close to the collapsed structure reached at p = 3.5 kbar. However, if the experimental crystal structure is used the calculation gives correct frequencies of most phonons. The most important new result is that linewidths/frequencies of certain modes are larger/softer than predicted by DFT-LDA. We also observed strong temperature dependence of some phonons near the structural phase transition near 173K. This behavior may indicate anomalously strong electron phonon coupling and/or anharmonicity, which may be important to the mechanism of superconductivity., Comment: 12 pages, 3 figues Revised version, Final version, Accepted for publication in Physical Review Letters

A Neutron Powder Diffraction (NPD) experiment has been performed to investigate the structural phase transition and magnetic order in CaFe1-xCoxAsF superconductor compounds (x = 0, 0.06, 0.12). The parent compound CaFeAsF undergoes a tetragonal to orthorhombic phase transition at 134(3) K, while the magnetic order in form of a spin-density wave (SDW) sets in at 114(3) K. The antiferromagnetic structure of the parent compound has been determined with a unique propagation vector k = (1,0,1) and the Fe saturation moment of 0.49(5)uB aligned along the long a-axis. With increasing Co doping, the long range antiferromagnetic order has been observed to coexist with superconductivity in the orthorhombic phase of the underdoped CaFe0.94Co0.06AsF with a reduced Fe moment (0.15(5)uB). Magnetic order is completely suppressed in optimally doped CaFe0.88Co0.12AsF. We argue that the coexistence of SDW and superconductivity might be related to mesoscopic phase separation., Comment: 4pages, 4figures

We report inelastic neutron scattering measurements of the phonon density-of-states in superconducting Sr0.6K0.4Fe2As2 (Tc=30 K) and Ca0.6Na0.4Fe2As2 (Tc=18 K). Compared with the parent compound BaFe2As2 doping affects mainly the lower and intermediate frequency part of the vibrations. Mass effects and lattice contraction cannot explain these changes. A lattice dynamical model has been used to identify the character of the various phonon bands. Softening of phonon modes below 10 meV has been observed in both samples on cooling from 300 K to 140 K. In the Ca doped compound the softening amounts to about 1 meV while for the Sr doped compound the softening is about 0.5 meV. There is no appreciable change in the phonon density of states when crossing Tc., Comment: 5 pages, 4 figures

We report here first extensive measurements of the temperature dependence of phonon density of states of BaFe2As2, the parent compound of the newly discovered FeAs-based superconductors, using inelastic neutron scattering. The experiments were carried out on the thermal time-of-flight neutron spectrometer IN4 at the ILL on a polycrystalline sample. There is no appreciable change in the spectra between T = 10 K and 200 K, although the sample undergoes a magnetic as well as a tetragonal-to-orthorhombic structural phase transition at 140 K. This indicates a rather harmonic phonon system. Shell model lattice dynamical calculations based on interatomic potentials are carried out to characterize the phonon data. The calculations predict a shift of the Ba-phonons to higher energies at 4 GPa. The average energy of the phonons of the Ba-sublattice is also predicted to increase on partial substitution of Ba by K to Ba0.6K0.4. The calculations show good agreement with the experimental phonon spectra, and also with the specific heat data from the literature., Comment: 10 pages, 4 figures

Neutron diffraction experiments have been carried out on a Sn-flux grown BaFe2As2 single crystal, the parent compound of the A-122 family of FeAs-based high-Tc superconductors. A tetragonal to orthorhombic structural phase transition and a three dimensional long-range antiferromagnetic ordering of the iron moment, with a unique magnetic propagation wavevector k = (1, 0, 1), have been found to take place at ~90 K. The magnetic moments of iron are aligned along the long a axis in the low temperature orthorhombic phase (Fmmm with b