Soft X-ray resonant powder diffraction has been performed at the Mn L2,3 edges of A-site ordered SmBaMn2O6. The energy and polarization dependence of the (1/2 1/2 0) reflection provide direct evidence for a (x2-z2)/(y2-z2) type orbital ordering in contrast to the single layer manganite. The temperature dependence of the reflection indicates an orbital reorientation transition at 210 K, below which the charge and orbital ordered MnO2 sheets show AAAA type of stacking. The concurring reduction of the ferromagnetic super exchange correlations leads to further charge localization.
We present a combined neutron and synchrotron powder diffraction study of the crystal and magnetic structure of VOCl. The occurrence of antiferromagnetic order in VOCl is accompanied by a monoclinic distortion. The high sensitivity of the magnetic interaction parameters on V-O-V bond angles and V-V distances yields strong magnetoelastic coupling which implies the structural distortion below T$_N$ as well as anomalous structural effects in the paramagnetic phase.
Rb2SnCu3F12 has been studied using synchrotron powder X-ray diffraction, powder neutron diffraction and single crystal X-ray diffraction at a range of temperatures (100 to 500 K). A broad but clear phase transition, possibly of re-entrant character, is found to occur in the powder form, whereas the corresponding transition is not seen in the single crystal.
Insulating 5d3 La3OsO7 and hole doped La2.8Ca0.2OsO7 materials featuring well separated pseudo-one-dimensional zig-zag chains of corner-sharing OsO6 octahedra have been synthesized and their magnetic and electrical transport properties characterized. Long range magnetic order between the antiferromagnetic chains is determined with a propagation vector k = 1/2, 1/2, 0 and TN = 45 and 53 K for the parent and doped materials. An Os5+ moment of 1.7(1) μB for La3OsO7 and 1.2(2) μB for La2.8Ca0.2OsO7 is refined. The long range magnetic structure is compared to the few currently known for isostructur…
We carried out detailed studies of the magnetic structure, magnetoelastic coupling, and thermal properties of EuCrO$_3$ nano-powders from room temperature to liquid helium temperature. Our neutron powder diffraction and X-ray powder diffraction measurements provide precise atomic positions of all atoms in the cell, especially for the light oxygen atoms. The low-temperature neutron powder diffraction data revealed extra Bragg peaks of magnetic origin which can be attributed to a $G_x$ antiferromagnetic structure with an ordered moment of $\sim$ 2.4 $μ_{\rm B}$ consistent with the $3d^3$ electro…
We present the low-temperature magnetic structures of SrGd$_2$O$_4$ combining neutron diffraction methods on polycrystalline and single-crystal samples containing the $^{160}$Gd isotope. In contrast to other members of the Sr$Ln_2$O$_4$ family ($Ln$ = lanthanide) this system reveals two long-range ordered magnetic phases, which our diffraction data unambiguously identify. Below $T_{\rm N1}$ = 2.73~K, a $\mathbf{q}_1$ = (0 0 0) magnetic structure is stabilized where ferromagnetic chains along the $c$~axis (space group $Pnam$) are coupled antiferromagnetically with neighboring chains. On cooling…
The magnetic ground state of polycrystalline Néel skyrmion hosting material GaV$_4$S$_8$ has been investigated using ac susceptibility and powder neutron diffraction. In the absence of an applied magnetic field GaV$_4$S$_8$ undergoes a transition from a paramagnetic to a cycloidal state below 13~K and then to a ferromagnetic-like state below 6~K. With evidence from ac susceptibility and powder neutron diffraction, we have identified the commensurate magnetic structure at 1.5 K, with ordered magnetic moments of $0.23(2)~μ_{\mathrm{B}}$ on the V1 sites and $0.22(1)~μ_{\mathrm{B}}$ on the V2 site…
The crystal and magnetic structure of (La0.70Ca0.30)(CryMn1-y)O3 for y = 0.70, 0.50 and 0.15 has been investigated using neutron powder diffraction. The three samples crystallize in the Pnma space group at both 290 K and 5 K and exhibit different magnetic structures at low temperature. In (La0.70Ca0.30)(Cr0.70Mn0.30)O3, antiferromagnetic order with a propagation vector k = 0 sets in. The magnetic structure is Gx, i.e. of the G-type with spins parallel to the a-axis. On the basis of our Rietveld refinement and the available magnetisation data, we speculate that only Cr3+ spins order, whereas Mn…
The discovery of superconductivity in the 122 iron selenide materials above 30 K necessitates an understanding of the underlying magnetic interactions. We present a combined experimental and theoretical investigation of magnetic and semiconducting Ce$_{2}$O$_{2}$FeSe$_{2}$ composed of chains of edge-linked iron selenide tetrahedra. The combined neutron diffraction and inelastic scattering study and density functional calculations confirm the ferromagnetic nature of nearest-neighbour Fe -- Se -- Fe interactions in the ZrCuSiAs-related iron oxyselenide Ce$_{2}$O$_{2}$FeSe$_{2}$. Inelastic measur…
Double perovskite iridates $A_2$ZnIrO$_6$ ($A$ = alkaline or lanthanide) show complex magnetic behaviors ranging from weak ferromagnetism to successive antiferromagnetic transitions. Here we report the static ($dc$) and dynamic ($ac$) magnetic susceptibility, and neutron powder diffraction measurements for $A$ = La and Nd compounds to elucidate the magnetic ground state. Below 10~K, the $A$ = La compound is best described as canted iridium moments in an antiferromagnet arrangement with a propagation vector \textbf{k} = 0 and a net ferromagnetic component along the $c$-axis. On the other hand, …
The magnetic ground state of two isostructural coordination polymers (i) the quasi two-dimensional S = 1/2 square-lattice antiferromagnet [Cu(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$; and (ii) a new compound [Co(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$, were examined with neutron powder diffraction measurements. We find the ordered moments of the Heisenberg S = 1/2 Cu(II) ions in [Cu(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$ are 0.6(1)$μ_{B}$, whilst the ordered moments for the Co(II) ions in [Co(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$ are 3.02(6)$μ_{B}$. For Cu(II), this reduced moment indicates the presence of …
Machine learning magnetic interactions from neutron powder diffraction data
School of Physics, Georgia Institute of Technology（佐治亚理工学院物理学院）；Neutron Scattering Division, Oak Ridge National Laboratory（橡树岭国家实验室中子散射部）；Materials Science and Technology Division, Oak Ridge National Laboratory（橡树岭国家实验室材料科学与技术部）
We have studied the temperature dependence of crystal and magnetic structures of the Jahn-Teller distorted transition metal difluorides CrF$_2$ and CuF$_2$ by neutron powder diffraction in the temperature range 2-280 K. The lattice parameters and the unit cell volume show magnetoelastic effects below the Néel temperature. The lattice strain due to the magnetostriction effect couples with the square of the order parameter of the antiferromagnetic phase transition. We also investigated the temperature dependence of the Jahn-Teller distortion which does not show any significant effect at the anti…
The crystal and magnetic structures of the spinel compounds ZnCr$_2$S$_4$ and ZnCr$_2$Se$_4$ were investigated by high resolution powder synchrotron and neutron diffraction. ZnCr$_2$Se$_4$ exhibits a first order phase transition at $T_N=21$ K into an incommensurate helical magnetic structure. Magnetic fluctuations above $T_N$ are coupled to the crystal lattice as manifested by negative thermal expansion. Both, the complex magnetic structure and the anomalous structural behavior can be related to magnetic frustration. Application of an external magnetic field shifts the ordering temperature and…
FeXMn1-XS (0 <x< 0.3) synthesized on the basis of α-MnS are the novel Mott-type substances with the rock salt structure. Neutron diffraction study shows that the shift of the Neel temperature of these materials from 150 (x = 0) to 200 K (x = 0.29) under the action of chemical pressure (x) is accompanied by a decrease in the cubic NaCl lattice parameters. The structural transition with a change in crystal symmetry and a decrease in resistance before the magnetic transition at x = 0.25 is found. Therefore, FeXMn1-XS are interesting materials for both fundamental study of the interrelation betwee…
We report neutron diffraction and transport results on the newly discovered superconducting nitride ThFeAsN with $T_c=$ 30 K. No magnetic transition, but a weak structural distortion around 160 K, is observed cooling from 300 K to 6 K. Analysis on the resistivity, Hall transport and crystal structure suggests this material behaves as an electron optimally doped pnictide superconductors due to extra electrons from nitrogen deficiency or oxygen occupancy at the nitrogen site, which together with the low arsenic height may enhance the electron itinerancy and reduce the electron correlations, thus…
Through powder x-ray diffraction we have investigated the structural behavior of SmVO3, in which orbital and magnetic degrees of freedom are believed to be closely coupled to the crystal lattice. We have found, contrary to previous reports, that SmVO3 exists in a single, monoclinic, phase below 200 K. The associated crystallographic distortion is then stabilized through the magnetostriction that occurs below 134 K. The crystal structure has been refined using synchrotron x-ray powder diffraction data measured throughout the structural phase diagram, showing a substantial Jahn-Teller distortion…
We have measured the specific heat of the S = 1/2 alternating Heisenberg antiferromagnetic chain compound pentafluorophenyl nitronyl nitroxide in magnetic fields using a single crystal and powder. A sharp peak due to field-induced magnetic ordering (FIMO) is observed in both samples. The H-T phase boundary of the FIMO of the single crystal is symmetric with respect to the central field of the gapless field region HC1 < H < HC2, whereas it is distorted for the powder whose ordering temperatures are lower. An analysis employing calculations based on the finite temperature density matrix renormal…
We use neutron powder diffraction to study on the non-superconducting phases of ThFeAsN$_{1-x}$O$_x$ with $x=0.15, 0.6$. In our previous results on the superconducting phase ThFeAsN with $T_c=$ 30 K, no magnetic transition is observed by cooling down to 6 K, and possible oxygen occupancy at the nitrogen site is shown in the refinement(H. C. Mao \emph{et al.}, EPL, 117, 57005 (2017)). Here, in the oxygen doped system ThFeAsN$_{1-x}$O$_x$, two superconducting region ($0\leqslant x \leqslant 0.1$ and $0.25\leqslant x \leqslant 0.55$) have been identified by transport experiments (B. Z. Li \emph{e…
The melting process of the orbital order in Pr0.5Ca0.5MnO3 single crystal has been studied in detail as a function of temperature by neutron diffraction. It is demonstrated that a commensurate-incommensurate (C-IC) transition of the orbital ordering takes place in a bulk sample, being consistent with the electron diffraction studies. The lattice structure and the transport properties go through drastic changes in the IC orbital ordering phase below the charge/orbital ordering temperature Tco/oo, indicating that the anomalies are intimately related to the partial disordering of the orbital orde…
Magnetic diffractive scattering of coherent metastable helium atomic beams from CoO(001) surfaces reveal the presence of an anomalous enhancement in the intensity of the half-order antiferromagnetic diffraction peak over the temperature range of 250-320K. Electronic cluster calculations based on Hartree-Fock states with configuration interactions, together with mean-field and Monte Carlo studies of this system suggest that this behavior is associated with low-lying surface spin excited states.
Here we show that the low temperature phase of magnetite is associated with an effective, although fractional, ordering of the charge. Evidence and a quantitative evaluation of the atomic charges are achieved by using resonant x-ray diffraction (RXD) experiments whose results are further analyzed with the help of ab initio calculations of the scattering factors involved. By confirming the results obtained from X-ray crystallography we have shown that RXD is able to probe quantitatively the electronic structure in very complex oxides, whose importance covers a wide domain of applications.
Resonant x-ray diffraction performed at the $\rm L_{II}$ and $\rm L_{III}$ absorption edges of Ru has been used to investigate the magnetic and orbital ordering in Ca$_2$RuO$_4$ single crystals. A large resonant enhancement due to electric dipole $2p\to 4d$ transitions is observed at the wave-vector characteristic of antiferromagnetic ordering. Besides the previously known antiferromagnetic phase transition at $\rm T_{N}=110$ K, an additional phase transition, between two paramagnetic phases, is observed around 260 K. Based on the polarization and azimuthal angle dependence of the diffraction …
In a recent letter, E. Nazarenko et al [Phys. Rev. Lett. 97, 056403 (2006) and cond-mat/0606596] have investigated the low temperature phase of magnetite by means of resonant X-ray scattering. The paper puts forward the quantitative determination of an effective charge ordering (CO) of 0.24 electron among the octahedral iron atoms in the insulating phase. The comment puts in evidence that the analysis performed by Nazarenko et al is wrong and that some of their conclusions are unsupported .
Various MSr2YCu2Oz (M1212 with M = Fe, Co, Al and Ga) compounds have been synthesized through a solid state reaction route. All these compounds are derived from the basic CuBa2YCu2O7 structure. Rietveld structural refinement of the room-temperature neutron diffraction data for Fe-1212 reveals that nearly half of Fe remains at the M site, while the other half goes to the Cu site in the CuO2 plane. For the M = Co, Al and Ga compounds, the basic unit cell gets doubled due to two distinct M sites in the M-O layer and the space group Ima2, without any cation intermixing is found more appropriate. F…
To clarify the magnetic properties of cluster-glass states in Sr1-xLaxRuO3 (0.3 <= x <= 0.5), we report herein the results of muon spin relaxation (muSR) and neutron powder diffraction measurements. The muSR experiments showed that magnetic clusters start developing well above the peak temperature T^* in the ac susceptibility. The volume fraction of the magnetically ordered region increases continuously with decreasing temperature, showing no anomaly at T^*, and reaches nearly 100% at the lowest temperature. The temperature variation of the volume fraction is essentially independent of the La …
We report the first direct resonant soft x-ray scattering observations of orbital ordering. We have studied the low temperature phase of La$_{0.5}$Sr$_{1.5}$MnO$_4$, a compound that displays charge and orbital ordering. Previous claims of orbital ordering in such materials have relied on observations at the Manganese $K$ edge. These claims have been questioned in several theoretical studies. Instead we have employed resonant soft x-ray scattering at the manganese $L_{III}$ and $L_{II}$ edges which probes the orbital ordering directly. Energy scans at constant wavevector are compared to theoret…
We used neutron powder diffraction to obtain the local and long-range structure of La0.5Ca0.5MnO3 at room temperature and 20K. By combining Rietveld and pair distribution function analysis of the total neutron scattering data, we have analyzed the structure of the compound using two competing models describing the low temperature phase: first the charge ordered/orbital ordered model and second the Mn-Mn dimer model. These structural models fit the 20K neutron powder diffraction pattern equally well using Rietveld analysis. Therefore, pair distribution function analysis is used to probe the loc…
The spatial charge arrangement of a typical quasi-two-dimensional organic conductor alpha-(BEDT-TTF)2I3 is revealed by single crystal structure analysis using synchrotron radiation. The results show that the horizontal stripe type structure, which was suggested by mean field theory, is established. We also find the charge disproportion above the metal-insulator transition temperature and a significant change in transfer integrals caused by the phase transition. Our result elucidates the insulating phase of this material as a 2k_F charge density localization.
The structure of Na0.5CoO2, the low temperature insulator that separates the magnetic and superconducting regions in the NaxCoO2.yH2O phase diagram, is studied by high resolution powder neutron diffraction at temperatures between 10 and 300 K. Profile analysis confirms that it has an orthorhombic symmetry structure, space group Pnmm, consisting of layers of edge-sharing CoO6 octahedra in a triangular lattice, with Na ions occupying ordered positions in one-dimensional chains in the interleaving planes. The oxygen content is found to be stoichiometric within 1%, indicating that the Na concentra…
Neutron elastic scattering measurements have been performed under the hydrostatic pressure in order to investigate the spin structure of the pressure-induced magnetic ordering in the spin gap system TlCuCl$_3$. Below the ordering temperature $T_{\rm N}=16.9$ K for the hydrostatic pressure $P=1.48$ GPa, magnetic Bragg reflections were observed at the reciprocal lattice points ${\mib Q}=(h, 0, l)$ with integer $h$ and odd $l$, which are equivalent to those points with the lowest magnetic excitation energy at ambient pressure. This indicates that the spin gap closes due to the applied pressure. T…
We report evidence for phase coexistence of orbital orderings of different symmetry in SmVO$_3$ by high resolution X-Ray powder diffraction. The phase coexistence is triggered by an antiferromagnetic ordering of the vanadium spins near 130K, below an initial orbital ordering near 200K. The phase coexistence is the result of the intermediate ionic size of samarium coupled to exchange striction at the vanadium spin ordering.
The magnetic structures and the magnetic phase transitions in the Mn-doped orthoferrite TbFeO$_3$ studied using neutron powder diffraction are reported. Magnetic phase transitions are identified at $T^\mathrm{Fe/Mn}_N \approx$ 295~K where a paramagnetic-to-antiferromagnetic transition occurs in the Fe/Mn sublattice, $T^\mathrm{Fe/Mn}_{SR} \approx$ 26~K where a spin-reorientation transition occurs in the Fe/Mn sublattice and $T^\mathrm{R}_N \approx$ 2~K where Tb-ordering starts to manifest. At 295~K, the magnetic structure of the Fe/Mn sublattice in TbFe$_{0.5}$Mn$_{0.5}$O$_3$ belongs to the ir…
Neutron diffraction measurements on a single crystal of CeGe1.76 reveal a complex series of magnetic transitions at low temperature. At T_N = 7 K, there is a transition from a paramagnetic state at higher temperature to an incommensurate magnetic structure characterized by a magnetic propagation vector (0 0 tau) with tau approx. 1/4 and the magnetic moment along the a axis of the orthorhombic unit cell. Below T_LI = 5 K, the magnetic structure locks in to a commensurate structure with tau = 1/4 and the magnetic moment remains along the a axis. Below T* = 4 K, we find additional half-integer an…
Magnetic ordering in TbMnO3 was revisited by a neutron diffraction study. In addition to the previously reported A-type and G-type modulated structures with a propagation vector (0,q_Mn,0), we found C-type and F-type orderings of the Mn moments. All the components appear below T_N^Mn = 46 K, and the G, C,and F-type components are enhanced below T_lock = 28 K, where q_Mn ordering locks at its low temperature value. The locking of the propagation vector also yields the squaring up of the spin arrangement. The magnetic moments of Tb ions show a quasi long-range ordering below T_N^Tb = 7 K. It dra…
We performed magnetic susceptibility and neutron powder diffraction experiments on the ternary compound Pr5Ru3Al2. It belongs to the noncentrosymmetric and nonmirrorsymmetric cubic I213 space group. The previously reported ferromagnetic transition at 24 K was not detected in our improved quality samples. Instead, magnetic ordering was observed in the DC magnetic susceptibility at 3.8 K. Neutron powder diffraction further indicates that an incommensurate magnetic structure is established below 3.8 K, with the magnetic modulation vector (0.066, 0.066, 0.066) (r.l.u.). Using the magnetic represen…
Magnetic and crystal structures of superconducting X yFe 2-xSe 2 (X= Rb and K with Tc=31.5 K and 29.5 K) have been studied by neutron powder diffraction at room temperature. Both crystals show ordered iron vacancy pattern and the crystal structure is well described in the I4/m space group with the lattice constants a=8.799, c=14.576 and a=8.730, c=14.115 A, and the refined stoichiometry x=0.30(1), y=0.83(2) and x=0.34(1), y=0.83(1) for Rb- and K-crystals respectively. The structure contains one fully occupied iron position and one almost empty vacancy position. Assuming that the iron moment is…
The solid solution Cs2-xRbxSnCu3F12 (x = 0, 0.5, 1.0, 1.5) has been investigated crystallographically between 100 and 300 K using synchrotron X-ray powder diffraction and, in the case of x = 0, neutron powder diffraction.
Electron microdiffraction study of phase transition in La2/3Ca1/3MnO3 revealed temperature dependent (h+1/2,0,l) diffraction spots. Their intensity peaks at Tc. Quantitative electron diffraction intensity analysis shows that they come from nanometer-sized domains with modulated transverse atomic displacements in the orthorhombic a-c plane, which has two types of Mn ions and thus charge ordering. The average domain is ~3.6 nm in diameter and ~1.5 nm in height (along the b-axis). The number of domains increases and then decreases, as the sample is cooled through Tc.
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…
High resolution X-ray powder-diffraction experiments on a well-characterized polycrystalline sample of the spin liquid Tb2Ti2O7 reveal that it shows normal positive thermal-expansion above 4 K, which does not agree with the intriguing anomalous negative thermal-expansion due to a magneto-elastic coupling reported for a single crystal sample below 20 K. We also performed a Rietveld profile refinement of a powder-diffraction pattern taken at a room temperature, and confirmed that it is consistent with the fully ordered cubic pyrochlore structure.
Low temperature magnetic and structural behavior of the extended Kagome system YBaCo4O7 has been studied by single crystal neutron diffraction and high-resolution powder X-ray diffraction. Long-range magnetic ordering associated with a structural transition from orthorhombic Pbn2_1 to monoclinic P2_1 symmetry has been found at T_1 ~ 100 K. The interplay between the structural and magnetic degrees of freedom testifies that the degeneracy of the magnetic ground state, present in the orthorhombic phase, is lifted through a strong magnetoelastic coupling, as observed in other frustrated systems. A…
We have investigated the physical properties of a pyrochlore hafnate Nd2Hf2O7 using ac magnetic susceptibility χ_ac(T), dc magnetic susceptibility χ(T), isothermal magnetization M(H) and heat capacity C_p(T) measurements, and determined the magnetic ground state by neutron powder diffraction study. An upturn is observed below 6 K in C_p(T)/T, however both C_p(T) and χ(T) do not show any clear anomaly down to 2 K. The χ_ac(T) shows a well pronounced anomaly indicating an antiferromagnetic transition at T_N = 0.55 K. The long range antiferromagnetic ordering is confirmed by neutron diffraction. …
Orthoferrites are a class of magnetic materials with a magnetic ordering temperature above 600 K, predominant G-type antiferromagnetic ordering of the Fe-spin system and, depending on the rare-earth ion, a spin reorientation of the Fe spin taking place at lower temperatures. DyFeO3 is of particular interest since the spin reorientation is classified as a Morin transition with the transition temperature depending strongly on the Dy-Fe interaction. Here, we report a detailed study of the magnetic and structural properties of microcrystalline DyFeO3 powder and bulk single crystal using neutron di…
We report a detailed examination the magnetic structure of anhydrous cupric chloride CuCl2 carried out by powder neutron diffraction, magnetic susceptibility and specific heat measurements on polycrystalline and single crystal samples as well as an evaluation of the spin exchange interactions by first principles density functional theory (DFT) calculations. Anhydrous CuCl2 shows one dimensional antiferromagnetic behavior and long range antiferromagnetic ordering below a Neel temperature of 23.9 K. Neutron powder and single crystal diffraction reveal that, below 23.9K, CuCl2 undergoes a phase t…
