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We present a thorough experimental investigation on single crystals of the rare-earth based frustrated quantum antiferromagnet Pr$_3$BWO$_9$, a purported spin-liquid candidate on the breathing kagome lattice. This material possesses a disordered ground state with an unusual excitation spectrum involving a coexistence of sharp spin-waves and broad continuum excitations. Nevertheless, we show through a combination of thermodynamic, magnetometric and spectroscopic probes with detailed theoretical modeling that it should be understood in a completely different framework. The crystal field splits the lowest quasi-doublet states into two singlets moderately coupled through frustrated superexchange, resulting in a simple effective Hamiltonian of an Ising model in a transverse magnetic field. While our neutron spectroscopy data do point to significant correlations within the kagome planes, the dominant interactions are out-of-plane, forming frustrated triangular spin-tubes through two competing ferro-antiferromagnetic bonds. The resulting ground state is a simple quantum paramagnet, but with significant modifications to both thermodynamic and dynamic properties due to small perturbations to the transverse field Ising model in the form of hyperfine enhanced nuclear moments and weak structural disorder., Comment: 21 pages, 12 figures

The crystal and magnetic structures of the spin $S$=1 hexamer cluster fedotovite-like A$_{2}$Cu$_{3}$O(SO$_4$)$_3$ (A$_2$=K$_2$, NaK, Na$_2$) were studied by neutron powder diffraction at temperatures 1.6-290 K. The crystal structures in all compounds are well refined in the monoclinic space group C2/c. The basic magnetic units of the compounds are copper hexamers which are coupled by weak superexchange interactions giving rise to three-dimensional long-range magnetic order below $3.0$ for the simplest symmetric spin Hamiltonian (obtained from inelastic neutron spectroscopy) of the isolated hexamers in the mean field, amounted to $\left<{s}\right>$=3/8 for side spins Cu1 and Cu2 and $\left<{s}\right>$=1/4 for Cu3 in the middle. The Cu spins are FM coupled in pairs and AFM between neighboring pairs. The experimental magnetic moments of the Cu$^{2+}$ ions turn out to be not completely collinear due to spin frustrations within the weak interhexamer interactions. The sizes of magnetic moments of Cu in the hexamers determined from the diffraction data are in fair agreement with the calculated values.

We revisit the antiferromagnetic structure of $\rm Tb_{14}Ag_{51}$ [P. Fischer., $et\, al$. (2005). PRB, 72 134413] with the propagation vector $[{1\over3},{1\over3},{0}] $ and parent space group $P6/m$ using both magnetic symmetry and irreducible representation arguments. We have found a new magnetic structure under the hexagonal Shubnikov magnetic space group $P\bar{6}'$, which fits much better the experimental data. This new solution was obtained by constraining the spin arrangement to one of the three possible magnetic space groups of maximal symmetry that can be realised by a magnetic ordering transforming according to the 4-dimensional physically irreducible representation that is known to be relevant in this magnetic phase. The refined model, parameterised under $P\bar{6}'$, implicitly includes the presence of a third harmonic with the propagation vector at the gamma point $[0,0,0]$, which has an important weight in the final result. The structure consists of 13 symmetry-independent Tb magnetic moments with the same size of $8.48(2)\mu_B$, propagating cycloidally in the $ab$-plane. The modulation has a substantial deviation from being purely sinusoidal due to the contribution of the mentioned third harmonic., Comment: 4 pages, 1 table, 7 figures

The recent synthesis of the chromium selenide compound LiCrSe$_2$ constitutes a valuable addition to the ensemble of two-dimensional triangular lattice antiferromagnets (2D-TLA). In this work we present the very first comprehensive study of the combined low temperature nuclear and magnetic structure established in this material. Details on the connection between Li-ion dynamics and structural changes are also presented along with a direct link between atomic structure and spin order via a strong magnetoelastic coupling. LiCrSe$_2$ was found to undergo a first order structural transition from a trigonal crystal system with space group $P\bar{3}m1$ to a monoclinic one with space group $C2/m$ at $T_{\rm s}=30$~K. Such restructuring of the lattice is accompanied by a magnetic transition at $T_{\rm N}=30$~K, with the formation of a complex spin arrangement for the Cr$^{3+}$ moments. Refinement of the magnetic structure with neutron diffraction data and complementary muon spin rotation analysis reveal the presence of two incommensurate magnetic domains with a up-up-down-down arrangement of the spins with ferromagnetic (FM) double chains coupled antiferromagnetically (AFM). In addition to this unusual arrangement, the spin axial vector is modulated both in direction and modulus, resulting in a spin density wave-like order with periodic suppression of the Cr moment along the chains. This behavior is believed to appear as a result of strong competition between direct exchange AFM and superexchange FM couplings established between both nearest neighbor and next nearest neighbor Cr$^{3+}$ ions. We finally conjecture that the resulting magnetic order is stabilized via subtle vacancy/charge order within the Li layers, potentially causing a mix of two different magnetic phases within the sample.

From new neutron powder diffraction experiments on the chiral cubic ($P2{_1}3$) magnet manganese germanide MnGe, we analyse all of the possible crystal symmetry-allowed magnetic superstructures that are determined successfully from the data. The incommensurate propagation vectors $k$ of the magnetic structure are found to be aligned with the [100] cubic axes, and correspond to a magnetic periodicity of about 30 $\r{A}$ at 1.8 K. Several maximal crystallographic symmetry magnetic structures are found to fit the data equally well and are presented. These include topologically non-trivial magnetic hedgehog and "skyrmion'' structures in multi-$k$ cubic or orthorhombic 3+3 and orthorhombic 3+2 dimensional magnetic superspace groups respectively, with either potentially responsible for topological Hall effect. The presence of orthorhombic distortions in the space group $P2_12_12_1$ caused by the transition to the magnetically ordered state does not favour the cubic magnetic hedgehog structure, and leave both orthorhombic hedgehog and "skyrmion'' models as equal candidates for the magnetic structures. We also report on a new combined mechanochemical and solid-state chemical route to synthesise MnGe at ambient pressures and moderate temperatures, and compare with samples obtained by the traditional high pressure synthesis., Comment: New high-resolution neutron diffraction data are added that allows us to unambiguously determine a preference for the orthorhombic symmetry

The metallic compound FeP belongs to the class of materials that feature a complex noncollinear spin order driven by magnetic frustration. While its double-helix magnetic structure with a period $\lambda_{\text{s}} \approx 5c$, where $c$ is the lattice constant, was previously well determined, the relevant spin-spin interactions that lead to that ground state remain unknown. By performing extensive inelastic neutron scattering measurements, we obtained the spin-excitation spectra in a large part of the momentum-energy space. The spectra show that the magnons are gapped with a gap energy of $\sim$5 meV. Despite the 3D crystal structure, the magnon modes display strongly anisotropic dispersions, revealing a quasi-one-dimensional character of the magnetic interactions in FeP. The physics of the material, however, is not determined by the dominating exchange, which is ferromagnetic. Instead, the weaker two-dimensional antiferromagnetic interactions between the rigid ferromagnetic spin chains drive the magnetic frustration. Using linear spin-wave theory, we were able to construct an effective Heisenberg Hamiltonian with an anisotropy term capable of reproducing the observed spectra. This enabled us to quantify the exchange interactions in FeP and determine the mechanism of its magnetic frustration., Comment: 13 pages, 7 figures

The minerals A2Cu3O(SO4)3 (A2=Na2, NaK, K2) constitute quantum spin systems with copper hexamers as basic structural units. Strong intra-hexamer spin couplings give rise to an effective triplet ground-state. Weak inter-hexamer spin couplings are responsible for two-dimensional long-range magnetic order in the (b,c)-plane below 3.0

Magnetic topological phases of quantum matter are an emerging frontier in physics and material science. Along these lines, several kagome magnets have appeared as the most promising platforms. Here, we explore magnetic correlations in the transition-metal-based kagome magnet TbMn$_{6}$Sn$_{6}$ using muon spin rotation, combined with local field analysis and neutron diffraction. Our results show that the system exhibits an out-of-plane ferrimagnetic structure $P6/mm'm'$ (comprised by Tb and Mn moments) with slow magnetic fluctuations below $T_{\rm C2}$~=~320~K. These fluctuations exhibit a slowing down below $T_{\rm C1}^{*}$~${\simeq}$~120~K, and we see the formation of static patches with ideal out-of-plane order below $T_{\rm C1}$~${\simeq}$~20~K which grow in a volume with decreasing temperature. The appearance of the static patches has a similar onset to the interesting phenomenon such as spin-polarized Dirac dispersion with a large Chern gap and topological edge states. We further show that the temperature evolution of the anomalous Hall conductivity (AHC) is strongly influenced by the low temperature magnetic crossover. Our presented experimental results show that the onset of the topological electronic properties tied to the Dirac band is promoted only by true static out-of-plane ferrimagnetic order in TbMn$_{6}$Sn$_{6}$ and is washed out by the slow magnetic fluctuations above $T_{\rm C1}$~${\simeq}$~20~K. Remarkably, hydrostatic pressure of 2.1 GPa stabilises static out-of-plane topological ferrimagnetic ground state in the whole volume of the sample. Therefore the exciting perspective arises of a magnetic system in which the topological response can be controlled, and thus explored, over a wide range of parameters., Comment: 21 pages, 12 figures

The manganese tellurate Li2MnTeO6 consists of trigonal spin lattices made up of Mn4+ (d3, S = 3/2) ions. The magnetic properties of this compound were characterized by several experimental techniques, which include magnetic susceptibility, specific heat, dielectric permittivity, electron spin resonance (ESR), nuclear magnetic resonance (NMR) and neutron powder diffraction (NPD) measurements, and by density functional calculations (DFT). The magnetic susceptibility chi(T) demonstrates very unusual behavior. It isdescribed by the Curie-Weiss law at high temperature with Curie-Weiss temperature of Theta = -74 K, exhibits no obvious anomaly indicative of a long-range magnetic ordering at low magnetic fields. At high magnetic fields, however, the character of chi(T) changes showing a maximum at about 9 K. That this maximum of chi(T) reflects the onset of an antiferromagnetic order was confirmed by specific heat measurements, which exhibit a clear lambda-type anomaly at TN around 8.5 K even at zero magnetic field, and by 7Li NMR and dielectric permittivity measurements. The magnetic structure of Li2MnTeO6, determined by neutron powder diffraction measurements at 1.6 K, is described by the 120-degree non-collinear spin structure with the propagation vector k = (1/3, 1/3, 0). Consistent with this finding, the spin exchange interactions evaluated for Li2MnTeO6 by density functional calculations are dominated by the nearest-neighbor antiferromagnetic exchange within each triangular spin lattice. This spin lattice is strongly spin frustrated with f = |Theta|/TN around 8 and exhibits a two-dimensional magnetic character in a broad temperature range above TN.

The high-pressure synthesized quasi-one-dimensional compounds NaMn$_2$O$_4$ and Li$_{0.92}$Mn$_2$O$_4$ are both antiferromagnetic insulators, and here their atomic and magnetic structures were investigated using neutron powder diffraction. The present crystal structural analyses of NaMn2O4 reveal that Mn3+/Mn4+ charge-ordering state exist even at low temperature (down to 1.5 K). It is evident from one of the Mn sites shows a strongly distorted Mn3+ octahedra due to the Jahn-Teller effect. Above TN = 39 K, a two-dimensional short-range correlation is observed, as indicated by an asymmetric diffuse scattering. Below TN, two antiferromagnetic transitions are observed (i) a commensurate long-range Mn3+ spin ordering below 39 K, and (ii) an incommensurate Mn4+ spin ordering below 10 K. The commensurate magnetic structure (kC = 0.5, -0.5, 0.5) follows the magnetic anisotropy of the local easy axes of Mn3+, while the incommensurate one shows a spin-density-wave order with kIC = (0,0,0.216). For Li$_{0.92}$Mn$_2$O$_4$, on the other hand, absence of a long-range spin ordered state down to 1.5 K is confirmed., Comment: 11 pages, 8 figures

We report the discovery of topological magnetism in the candidate magnetic Weyl semimetal CeAlGe. Using neutron scattering we find this system to host several incommensurate, square-coordinated multi-$\vec{k}$ magnetic phases below $T_{\rm{N}}$. The topological properties of a phase stable at intermediate magnetic fields parallel to the $c$-axis are suggested by observation of a topological Hall effect. Our findings highlight CeAlGe as an exceptional system for exploiting the interplay between the nontrivial topologies of the magnetization in real space and Weyl nodes in momentum space., Comment: 6 pages, 5 figures

Quantum materials that feature magnetic long-range order often reveal complex phase diagrams when localized electrons become mobile. In many materials magnetism is rapidly suppressed as electronic charges dissolve into the conduction band. In materials where magnetism persists, it is unclear how the magnetic properties are affected. Here we study the evolution of the magnetic structure in Nd(1-x)Ce(x)CoIn(5) from the localized to the highly itinerant limit. We observe two magnetic ground states inside a heavy-fermion phase that are detached from unconventional superconductivity. The presence of two different magnetic phases provides evidence that increasing charge delocalization affects the magnetic interactions via anisotropic band hybridization.

The compounds A2Cu3O(SO4)3 (A=Na,K) are characterized by copper hexamers which are weakly coupled along the b-axis to realize one-dimensional antiferromagnetic chains below TN=3 K, whereas the interchain interactions along the a- and c-axes are negligible. We investigated the energy-level splittings of the copper hexamers by inelastic neutron scattering below and above TN. The eight lowest-lying hexamer states could be unambiguously assigned and parametrized in terms of a Heisenberg exchange Hamiltonian, providing direct experimental evidence for an S=1 triplet ground-state associated with the copper hexamers. Therefore, the compounds A2Cu3O(SO4)3 serve as novel cluster-based spin-1 antiferromagnets to support Haldane's conjecture that a gap appears in the excitation spectrum below TN, which was verified by inelastic neutron scattering., Comment: 21 pages, 4 figures, 2 tables

The magnetic ground state in highly ordered double perovskites LaSr$_{1-x}$Ca$_x$NiReO$_6$ ($x$ = 0.0, 0.5, 1.0) were studied in view of the Goodenough-Kanamori rules of superexchange interactions. In LaSrNiReO$_6$, Ni and Re sublattices are found to exhibit curious magnetic states, but do not show any long range magnetic ordering. The magnetic transition at $\sim$ 255 K is identified with the Re sublattic magnetic ordering. The sublattice interactions are tuned by modifying the Ni-O-Re bond angles via changing the lattice structure through Ca doping. Upon Ca doping, the Ni and Re sublattices start to display a ferrimagnetically ordered state at low temperature. The neutron powder diffraction reveals a canted alignment between the Ni and the Re sublattices, while the individual sublattice is ferromagnetic. The transition temperature of the ferrimagnetic phase increases monotonically with increasing Ca concentration., Comment: 18 pages, 8 figures

The magnetic ordering of La$_{1/3}$Sr$_{2/3}$FeO$_3$ perovskite has been studied by neutron powder diffraction and $^{57}$Fe M\"ossbauer spectroscopy down to 2 K. From symmetry analysis, a chiral helical model and a collinear model are proposed to describe the magnetic structure. Both are commensurate, with propagation vector k = (0,0,1) in R-3c space group. In the former model, the magnetic moments of Fe adopt the magnetic space group P3$_{2}$21 and have helical and antiferromagnetic ordering propagating along the c axis. The model allows only one Fe site, with a magnetic moment of 3.46(2) $\mu_{\rm{B}}$ at 2 K. In the latter model, the magnetic moments of iron ions adopt the magnetic space group C2/c or C2'/c' and are aligned collinearly. The model allows the presence of two inequivalent Fe sites with magnetic moments of amplitude 3.26(3) $\mu_{\rm{B}}$ and 3.67(2) $\mu_{\rm{B}}$, respectively. The neutron diffraction pattern is equally well fitted by either model. The M\"ossbauer spectroscopy study suggests a single charge state Fe$^{3.66+}$ above the magnetic transition and a charge disproportionation into Fe$^{(3.66-\zeta)+}$ and Fe$^{(3.66+2\zeta)+}$ below the magnetic transition. The compatibility of the magnetic structure models with the M\"ossbauer spectroscopy results is discussed.

We present an experimental study for polycrystalline samples of the diluted magnetic semiconductor Mn(x)Ga(1-x)N (x<0.04) in order to address some of the existing controversial issues. Different techniques were used to characterize the electronic, magnetic, and structural properties of the samples, and inelastic neutron scattering was employed to determine the magnetic excitations associated with Mn monomers and dimers. Our main conclusions are as follows: (i) The valence of the Mn ions is 2+. (ii) The Mn(2+) ions experience a substantial single-ion axial anisotropy with parameter D=0.027(3) meV. (iii) Nearest-neighbor Mn(2+) ions are coupled antiferromagnetically. The exchange parameter J= 0.140(7) meV is independent of the Mn content x, i.e., there is no evidence for hole-induced modifications of J towards a potentially high Curie temperature postulated in the literature., Comment: 19 pages, 1 table, 4 figures

Muon spin relaxation ($\mu$SR) measurements were carried out on SrDy$_2$O$_4$, a frustrated magnet featuring short range magnetic correlations at low temperatures. Zero-field muon spin depolarization measurements demonstrate that fast magnetic fluctuations are present from $T=300$ K down to 20 mK. The coexistence of short range magnetic correlations and fluctuations at $T=20$ mK indicates that SrDy$_2$O$_4$ features a spin liquid ground state. Large longitudinal fields affect weakly the muon spin depolarization, also suggesting the presence of fast fluctuations. For a longitudinal field of $\mu_0H=2$ T, a non-relaxing asymmetry contribution appears below $T=6$ K, indicating considerable slowing down of the magnetic fluctuations as field-induced magnetically-ordered phases are approached., Comment: 6 pages, 4 figures, to be published as a proceeding of HFM2016 in Journal of Physics: Conference Series (JPCS)

Strontium doping transforms manganites of type La(1-x)Sr(x)MnO(3) from an insulating antiferromagnet (x=0) to a metallic ferromagnet (x>0.16) due to the induced charge carriers (holes). Neutron scattering experiments were employed to investigate the effect of Sr doping on a tailor-made compound of composition La(0.7)Sr(0.3)Mn(0.1)Ti(0.3)Ga(0.6)O(3). By the simultaneous doping with Sr2+ and Ti4+ ions the compound remains in the insulating state, so that the magnetic interactions for large Sr doping can be studied in the absence of charge carriers. At TC=215 K there is a first-order reconstructive phase transition from the trigonal R-3c structure to the orthorhombic Pnma structure via an intermediate virtual configuration described by the common monoclinic subgroup P21/c. The magnetic excitations associated with Mn3+ dimers give evidence for two different nearest-neighbor ferromagnetic exchange interactions, in contrast to the undoped compound LaMnyA(1-y)O(3) where both ferromagnetic and antiferromagnetic interactions are present. The doping induced changes of the exchange coupling originates from different Mn-O-Mn bond angles determined by neutron diffraction. The large fourth-nearest-neighbor interaction found for metallic manganites is absent in the insulating state. We argue that the Ruderman-Kittel-Kasuya-Yosida interaction reasonably accounts for all the exchange couplings derived from the spin-wave dispersion in metallic manganites., Comment: 19 pages, 2 tables, 8 figures

Magnetic frustration and low dimensionality can prevent long range magnetic order and lead to exotic correlated ground states. SrDy$_2$O$_4$ consists of magnetic Dy$^{3+}$ ions forming magnetically frustrated zig-zag chains along the c-axis and shows no long range order to temperatures as low as $T=60$ mK. We carried out neutron scattering and AC magnetic susceptibility measurements using powder and single crystals of SrDy$_2$O$_4$. Diffuse neutron scattering indicates strong one-dimensional (1D) magnetic correlations along the chain direction that can be qualitatively accounted for by the axial next-nearest neighbour Ising (ANNNI) model with nearest-neighbor and next-nearest-neighbor exchange $J_1=0.3$ meV and $J_2=0.2$ meV, respectively. Three-dimensional (3D) correlations become important below $T^*\approx0.7$ K. At $T=60$ mK, the short range correlations are characterized by a putative propagation vector $\textbf{k}_{1/2}=(0,\frac{1}{2},\frac{1}{2})$. We argue that the absence of long range order arises from the presence of slowly decaying 1D domain walls that are trapped due to 3D correlations. This stabilizes a low-temperature phase without long range magnetic order, but with well-ordered chain segments separated by slowly-moving domain walls., Comment: 13 pages, 14 figures, 2 tables

We report on the magnetic properties of CsCo$_2$Se$_2$ with ThCr$_2$Si$_2$ structure, which we have characterized through a series of magnetization and neutron diffraction measurements. We find that CsCo$_2$Se2$_2$ undergoes a phase transition to an antiferromagnetically ordered state with a N\'eel temperature of $T_{\rm N} \approx$ 66 K. The nearest neighbour interactions are ferromagnetic as observed by the positive Curie-Weiss temperature of $\Theta \approx$ 51.0 K. We find that the magnetic structure of CsCo$_2$Se$_2$ consists of ferromagnetic sheets, which are stacked antiferromagnetically along the tetragonal \textit{c}-axis, generally referred to as A-type antiferromagnetic order. The observed magnitude of the ordered magnetic moment at $T$ = 1.5 K is found to be only 0.20(1)$\mu_{\rm Bohr}$/Co. Already in comparably small magnetic fields of $\mu_0 H_{MM}$(5K) $\approx$ 0.3 T, we observe a metamagnetic transition that can be attributed to spin-rearrangements of CsCo$_2$Se$_2$, with the moments fully ferromagnetically saturated in a magnetic field of $\mu_0 H_{\rm FM}$(5K) $\approx$ 6.4 T. We discuss the entire experimentally deduced magnetic phase diagram for CsCo$_2$Se$_2$ with respect to its unconventionally weak magnetic coupling. Our study characterizes CsCo$_2$Se$_2$, which is chemically and electronically posed closely to the $A_xFe_{2-y}Se_2$ superconductors, as a host of versatile magnetic interactions.

Strong spin-lattice coupling and prominent frustration effects observed in the 50$\%$ Fe-doped frustrated hexagonal ($h$)LuMnO$_3$ are reported. A N\'{e}el transition at $T_{\mathrm N} \approx$ 112~K and a possible spin re-orientation transition at $T_{\mathrm {SR}} \approx$ 55~K are observed in the magnetization data. From neutron powder diffraction data, the nuclear structure at and below 300~K was refined in polar $P6_3cm$ space group. While the magnetic structure of LuMnO$_3$ belongs to the $\Gamma_4$ ($P6'_3c'm$) representation, that of LuFe$_{0.5}$Mn$_{0.5}$O$_3$ belongs to $\Gamma_1$ ($P6_3cm$) which is supported by the strong intensity for the $\mathbf{(100)}$ reflection and also judging by the presence of spin-lattice coupling. The refined atomic positions for Lu and Mn/Fe indicate significant atomic displacements at $T_{\mathrm N}$ and $T_{\mathrm {SR}}$ which confirms strong spin-lattice coupling. Our results complement the discovery of room temperature multiferroicity in thin films of $h$LuFeO$_3$ and would give impetus to study LuFe$_{1-x}$Mn$_x$O$_3$ systems as potential multiferroics where electric polarization is linked to giant atomic displacements.

Defects intentionally introduced into magnetic materials often have a profound effect on the physical properties. Specifically tailored neutron spectroscopic experiments can provide detailed information on both the local exchange interactions and the local distances between the magnetic atoms around the defects. This is demonstrated for manganese dimer excitations observed for the magnetically diluted three- and two-dimensional compounds KMn(x)Zn(1-x)F(3) and K(2)Mn(x)Zn(1-x)F(4), respectively. The resulting local exchange interactions deviate up to 10% from the average, and the local Mn-Mn distances are found to vary stepwise with increasing internal pressure due to the Mn/Zn substitution. Our analysis qualitatively supports the theoretically predicted decay of atomic displacements according to 1/r**2, 1/r, and constant (for three-, two-, and one-dimensional compounds, respectively) where r denotes the distance of the displaced atoms from the defect., Comment: 21 pages, 4 figures, 3 tables

Pressure-dependent diffraction response of the superconducting phase separated Cs0.72Fe1.57Se2 has been studied using synchrotron radiation up to the pressure of 19 GPa. The main and secondary phases of Cs0.72Fe1.57Se2 have been observed in the whole pressure range. The main ordered phase has been found to undergo an order-disorder transition in the Fe-sublattice at least at P = 11 GPa with the corresponding kinetics on the order of hours. Contrary to the analogous temperature induced transition, the secondary phase has not been suppressed suggesting that its stability pressure range is higher than 19 GPa or the corresponding transformation kinetics is slower at room temperature. Together with the previously reported pressure-dependent resistivity and magnetic susceptibility measurements, this work indicates that superconductivity in the AxFe2-ySe2 (A - alkali metals) phases could be related to the Fe-vacancy ordering in the main phase.

The magnetic properties of NiTa$_2$O$_6$ were investigated by magnetic susceptibility, specific heat, electron paramagnetic resonance, neutron powder diffraction and pulse field magnetization measurements. Accompanying \textit{ab initio} DFT calculations of the spin-exchange constants complemented and supported our experimental findings that NiTa$_2$O$_6$ must be described as a quasi-1D Heisenberg $S$ = 1 spin chain system with a nearest-neighbor only anti-ferromagnetic spin-exchange interaction of 18.92(2) K. Inter-chain coupling is by about two orders of magnitude smaller. Electron paramagnetic resonance measurements on Mg$_{1-x}$Ni$_x$Ta$_2$O$_6$ ($x \approx$ $1\%$) polycrystalline samples enabled us to estimate the single-ion zero-field splitting of the $S$ = 1 states which amounts to less than $4\%$ of the nearest-neighbor spin-exchange interaction. At 0 T NiTa$_2$O$_6$ undergoes long-range anti-ferromagnetic ordering at 10.3(1) K evidenced by a $\lambda$-type anomaly in the specific heat capacity. On application of a magnetic field the specific heat anomaly is smeared out. We confirmed the magnetic structure by neutron powder diffraction measurements and at 2.00(1) K refined a magnetic moment of 1.93(5) $\mu_{\rm{B}}$ per Ni$^{2+}$ ion. Additionally, we followed the magnetic order parameter as a function of temperature. Lastly we found saturation of the magnetic moment at 55.5(5) T with a $g$-factor of 2.14(1), with an additional high field phase above 12.8(1) T. The onset of the new high field phase is not greatly effected by temperature, but rather smears out as one approaches the long-range ordering temperature., Comment: Accepted by Phys. Rev. B

We study the zero-point and thermal ionic motion in La$_2$CuO$_4$ by means of high-resolution neutron diffraction experiments. Our results demonstrate anisotropic motion of O and to a lesser extent of Cu ions, both consistent with the structure of coupled CuO$_6$ octahedra, and quantify the relative effects of zero-point and thermal contributions to ionic motion. By substitution of $^{18}$O, we find that the oxygen isotope effect on the lattice dimensions is small and negative ($-0.01\%$), while the isotope effect on the ionic displacement parameters is significant ($-6$ to $50\%$). We use our results as input for theoretical estimates of the distribution of magnetic interaction parameters, $J$, in an effective one-band model for the cuprate plane. We find that ionic motion causes only small ($1\%$) effects on the average value $\langle J\rangle$, which vary with temperature and O isotope, but results in dramatic ($10$-$20\%$) fluctuations in $J$ values that are subject to significant ($8$-$12\%$) isotope effects. We demonstrate that this motional broadening of $J$ can have substantial effects on certain electronic and magnetic properties in cuprates., Comment: 13 pages, 9 figures

We report superconductivity in a new layered bismuth oxyselenide LaO0.5F0.5BiSe2 with the ZrCuSiAs-type structure composed of alternating superconducting BiSe2 and blocking LaO layers. The superconducting transition temperature is TC = 2.6K, as revealed from DC magnetization, resistivity and muon spin rotation (muSR) experiments. DC magnetization measurements indicate a superconducting volume fraction of approximately 80%, which is at least twice higher in comparison to that found in corresponding sulphide LaO0.5F0.5BiS2. Importantly, the bulk character of superconductivity in LaO0.5F0.5BiSe2 was confirmed by muSR.

We report on muon spin rotation/relaxation and $^{119}$Sn nuclear magnetic resonance (NMR) measurements to study the microscopic superconducting and magnetic properties of the Heusler compound with the highest superconducting transition temperature, \ypd\ ($T_c=5.4$ K). Measurements in the vortex state provide the temperature dependence of the effective magnetic penetration depth $\lambda(T)$ and the field dependence of the superconducting gap $\Delta(0)$. The results are consistent with a very dirty s-wave BCS superconductor with a gap $\Delta(0)=0.85(3)$ meV, $\lambda(0)= 212(1)$ nm, and a Ginzburg-Landau coherence length $\xi_{\mathrm{GL}}(0)\cong 23$ nm. In spite of its very dirty character, the effective density of condensed charge carriers is high compared to the normal state. The \mSR data in a broad range of applied fields are well reproduced by taking into account a field-related reduction of the effective superconducting gap. Zero-field \mSR measurements, sensitive to the possible presence of very small magnetic moments, do not show any indications of magnetism in this compound., Comment: 9 pages, 11 figures

We report the observation of a stepwise "melting" of the low-temperature Na-vacancy order in the layered transition metal oxide Na0.7CoO2. High-resolution neutron powder diffraction indicates the existence of two first-order structural transitions, one at T1 = 290 K, followed by a second at T2 = 400 K. Detailed analysis reveals that both transitions are linked to changes in the Na mobility. Our data are consistent with a two-step disappearance of Na-vacancy order through the successive opening of first quasi-1D (T1 > T > T2) and then 2D (T > T2) Na diffusion paths. These results shed new light on previous, seemingly incompatible, experimental interpretations regarding the relationship between Na-vacancy order and Na dynamics in this material. They also represent an important step towards the tuning of physical properties and the design of tailored functional materials through an improved control and understanding of ionic diffusion., Comment: 5 pages, 4 figures, accepted by PRL

BaFe2Se3 (Pnma, CsAg2I3-type structure), recently assumed to show superconductivity at ~ 11 K, exhibits a pressure-dependent structural transition to the CsCu2Cl3-type structure (Cmcm space group) around 60 kbar, as evidenced from pressure-dependent synchrotron powder diffraction data. Temperature-dependent synchrotron powder diffraction data indicate an evolution of the room-temperature BaFe2Se3 structure towards a high symmetry CsCu2Cl3 form upon heating. Around 425 K BaFe2Se3 undergoes a reversible, first order isostructural transition, that is supported by the differential scanning calorimetry data. The temperature-dependent structural changes occur in two stages, as determined by the alignment of the FeSe4 tetrahedra and corresponding adjustments of the positions of Ba atoms. On further heating, a second order phase transformation into the Cmcm structure is observed at 660 K. A rather unusual combination of isostructural and second-order phase transformations is parameterized within phenomenological theory assuming high-order expansion of Landau potential. A generic phase diagram mapping observed structures is proposed on the basis of the parameterization., Comment: 22 pages, 15 figures

The low-temperature crystal structure of BaCuSi2O6 has been investigated with high-resolution synchrotron x-ray and neutron powder diffraction techniques and has been found to be on average (ignoring the incommensurate modulation) orthorhombic, with the most probable space group Ibam. The Cu-Cu dimers in this material are forming two types of layers with distinctly different interatomic distances. Subtle changes also modify the partially frustrated interlayer Cu-Cu exchange paths. The present results corroborate the interpretation of low-temperature nuclear magnetic resonance and inelastic neutron scattering data in terms of distinct dimer layers.

We report on a new iron selenide superconductor with a TC onset of 45K and the nominal composition Lix(C5H5N)yFe2-zSe2, synthesized via intercalation of dissolved alkaline metal in anhydrous pyridine at room temperature. This superconductor exhibits a broad transition, reaching zero resistance at 10K. Magnetization measurements reveal a superconducting shielding fraction of approximately 30%. Analogous phases intercalated with Na, K and Rb were also synthesized and characterized. The superconducting transition temperature of Lix(C5H5N)yFe2-zSe2 is clearly enhanced in comparison to the known superconductors FeSe0.98 (Tc ~ 8K) and AxFe2-ySe2 (TC ~ 27-32K) and is in close agreement with critical temperatures recently reported for Lix(NH3)yFe2-zSe2. Post-annealing of intercalated material (Lix(C5H5N)yFe2-zSe2) at elevated temperatures drastically enlarges the c-parameter of the unit cell (~44%) and increases the amount of superconducting shielding fraction to nearly 100%. Our findings indicate a new synthesis road leading to possibly even higher critical temperatures in this class of materials by intercalation of organic compounds between Fe-Se layers., Comment: 13 pages, 5 figures

The crystal and magnetic structures of the superconducting iron based chalcogenides RbyFe2-xSe2 have been studied by means of single crystal synchrotron x-ray and high resolution neutron powder diffraction in the temperature range 2-570 K. The ground state of the crystal is an intrinsically phase separated state with two distinct by symmetry phases. The main phase has the iron vacancy ordered \surd5x\surd5 superstructure (I4/m space group) with AFM ordered Fe spins. The minority phase does not have \surd5x\surd5-type of ordering and has smaller in plane lattice constant a and larger tetragonal c-axis and can be well described assuming the parent average vacancy disordered structure (I4/mmm space group) with the refined stoichiometry Rb0.60(5)(Fe1.10(5))Se)2. The minority phase amounts to 8-10% mass fraction. The unit cell volume of the minority phase is 3.2% smaller than the one of the main phase at T = 2 K and has quite different temperature dependence. The minority phase transforms to the main vacancy ordered phase on heating above the phase separation temperature T_P = 475 K. The spatial dimensions of the phase domains strongly increase above TP from 1000 \AA\ to > 2500 \AA\ due to the merging of the regions of the main phase that were separated by the second phase at low temperatures. Additional annealing of the crystals at the temperature T=488 K close to T_P for the long time drastically reduces the amount of the minority phase., Comment: added additional figure and section on high T annealing

We present a detailed investigation of the magnetic and structural properties of magnetically doped 3D topological insulator Bi2Se3. From muon spin relaxation measurements in zero magnetic field, we find that even 5% Fe doping on the Bi site turns the full volume of the sample magnetic at temperatures as high as ~250 K. This is also confirmed by magnetization measurements. Two magnetic "phases" are identified; the first is observed between ~10-250 K while the second appears below ~10 K. These cannot be attributed to impurity phases in the samples. We discuss the nature and details of the observed magnetism and its dependence on doping level., Comment: 7 pages and 6 figures

AxFe2-ySe2 (A=K, Rb, Cs) superconductors may show a complex mixture of structural phases even in a single crystal form. A full sphere of the diffraction intensity has been collected, with the help of synchrotron radiation, for Cs0.8Fe1.6Se2 . In addition to the expected pattern for the tetragonal phase with ordered Fe vacancies, a diffuse scattering from Cs occupational disorder has been observed, together with an extra Bragg contribution from a minor phase. The minor phase, in agreement with previous findings, is compressed in the tetragonal a-b plane and expanded along the c-direction; a set of modulated Bragg rods evidences a planar disorder. Fourfold splitting of the rods as well as the main Bragg peaks for L\neq0 imply that symmetry of the minor phase is not higher than monoclinic. The monoclinic distortion was estimated to be 90.7 degrees. Structured diffuse scattering, observed on top of the Bragg component, relates to the major phase and is attributed to a correlated distribution of Cs ions. Elastic nature of the observed scattering was confirmed by additional inelastic X-ray scattering experiment. Diffuse scattering forms 3D objects that have topological similarity with what one would expect, under assumptions discussed in the text, for a Fermi surface nesting., Comment: 17 pages, 6 figures

We report a neutron diffraction study of the magnetic phase transitions in the charge-density-wave (CDW) TbTe$_3$ compound. We discover that in the paramagnetic phase there are strong 2D-like magnetic correlations, consistent with the pronounced anisotropy of the chemical structure. A long-range incommensurate magnetic order emerges in TbTe$_3$ at $T_{mag1}$ = 5.78 K as a result of continuous phase transitions. We observe that near the temperature $T_{mag1}$ the magnetic Bragg peaks appear around the position (0,0,0.24) (or its rational multiples), that is fairly close to the propagation vector $(0,0,0.29)$ associated with the CDW phase transition in TbTe$_3$. This suggests that correlations leading to the long-range magnetic order in TbTe$_3$ are linked to the modulations that occur in the CDW state.

We introduce a novel method for local structure determination with a spatial resolution of the order of 0.01 Angstroem. It can be applied to materials containing clusters of exchange-coupled magnetic atoms. We use neutron spectroscopy to probe the energies of the cluster excitations which are determined by the interatomic coupling strength J. Since for most materials J is related to the interatomic distance R through a linear relation dJ/dR={\alpha} (for dR/R<<1), we can directly derive the local distance R from the observed excitation energies. This is exemplified for the mixed one-dimensional paramagnetic compound CsMnxMg1 xBr3 (x=0.05, 0.10) containing manganese dimers oriented along the hexagonal c-axis. Surprisingly, the resulting Mn-Mn distances R do not vary continuously with increasing internal pressure, but lock in at some discrete values., Comment: 16 pages, 2 tables, 3 figures

We report on synthesis of single crystals of BaFe2Se3 and study of their crystal and magnetic structures by means of synchrotron single crystal X-ray and neutron powder diffraction. The crystal structure has orthorhombic symmetry and consists of double chains of FeSe4 edge connected tetrahedra intercalated by barium. Below 240 K long range block-spin checkerboard antiferromagnetic (AFM) order is developed. The magnetic structure is similar to one observed in A0.8Fe1.6Se2 (A=K, Rb or Cs) superconductors. The crystals exhibit a transition to the diamagnetic state with an onset transition temperature of Tc ~11 K. Though we observe FeSe as an impurity phase (<0.8% mass fraction) the diamagnetism unlikely can be attributed to the FeSe-superconductor which has Tc\approx8.5K., Comment: 12 pages, 6 figures, added erratum (page 12) for Figure 4b showing tau2 structure

Polycrystalline samples and single crystals of SmFeAs1-xPxO1-y were synthesized and grown employing different synthesis methods and annealing conditions. Depending on the phosphorus and oxygen content, the samples are either magnetic or superconducting. In the fully oxygenated compounds the main impact of phosphorus substitution is to suppress the N\'eel temperature TN of the spin density wave (SDW) state, and to strongly reduce the local magnetic field in the SDW state, as deduced from muon spin rotation measurements. On the other hand the superconducting state is observed in the oxygen deficient samples only after heat treatment under high pressure. Oxygen deficiency as a result of synthesis at high pressure brings the Sm-O layer closer to the superconducting As/P-Fe-As/P block and provides additional electron transfer. Interestingly, the structural modifications in response to this variation of the electron count are significantly different when phosphorus is partly substituting arsenic. Point contact spectra are well described with two superconducting gaps. Magnetic and resistance measurements on single crystals indicate an in-plane magnetic penetration depth of 200 nm and an anisotropy of the upper critical field slope of 4-5. PACS number(s): 74.70.Xa, 74.62.Bf, 74.25.-q, 81.20.-n, Comment: 36 pages, 13 figures, 2 tables

Inelastic neutron scattering was employed to study the magnetic excitations of Mn3+ dimers in LaMn0.1Ga0.9O3. The nearest-neighbor interaction of Mn3+ ions is ferromagnetic in the basal (a,b)-plane, but antiferromagnetic along the c-direction, thus two different types of dimer excitations are simultaneously present in the experiments. From the observed energy spectra we derive Heisenberg-type exchange interactions Jab=0.210(4) meV and Jc=-0.285(5) meV as well as an axial anisotropy parameter D=0.036(6) meV. These parameters considerably differ from those derived for the isostructural parent compound LaMnO3 due to structural effects., Comment: 21 pages, 5 figures, 3 tables

Temperature-dependent synchrotron powder diffraction on Cs0.83(Fe0.86Se)2 revealed first order I4/m to I4/mmm structural transformation around 216{\deg}C associated with the disorder of the Fe vacancies. Irreversibility observed during the transition is likely associated with a mobility of intercalated Alkali atoms. Pressure-dependent synchrotron powder diffraction on Cs0.83(Fe1-ySe)2, Rb0.85(Fe1-ySe)2 and K0.8(Fe1-ySe)2 (y ~ 0.14) indicated that the I4/m superstructure reflections are present up to pressures of 120 kbar. This may indicate that the ordering of the Fe vacancies is present in both superconducting and non-superconductive states., Comment: 11 pages, 5 figures, 1 table

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 ordered only on the fully occupied site we have sorted out all eight irreducible representations (irreps) for the propagation vector k=0 and have found that irreps tau_2 and tau_7 well fit the experimental data with the moments along c-axis. The moment amplitudes amounted to 2.15(3) mu_B, 2.55(3) mu_B for tau_2 and 2.08(6) mu_B, 2.57(3) mu_B for tau_7 for Rb- and K-crystals respectively. Irrep tau_2 corresponds to the Shubnikov group I4/m' and gives a constant moment antiferromagnetic configuration, whereas tau_7 does not have Shubnikov counterpart and allows two different magnetic moments in the structure., Comment: 5 pages, 1 table, 4 figures

Neutron and x-ray powder and single crystal synchrotron diffraction of CsyFe2-xSe2 show the presence of superstructure reflections with propagation vector k=[2/5, 1/5, 1] with respect to the average crystal structure I4/mmm (a = 4, c = 15A). The propagation vector star corresponds to the 5 times bigger unit cell given by transformation A=2a+b, B= -a+2b, C= c. A solution for the atomic structure is found in the space groups P42/n and I4/m with an ordered pattern of iron vacancies corresponding to the iron deficiency x = 0.29 and Cs stoichiometry y = 0.83. The superstructure satellites are more pronounced in the neutron diffraction patterns suggesting that they can have some magnetic contribution. We have sorted out possible symmetry adapted magnetic configurations and found that the presence of AFM ordering with the ordered magnetic moment of Fe with 2{\mu}B does not contradict to the experimental data. However, the solutions space is highly degenerate and we cannot choose a specific solution. Instead we propose possible magnetic configurations with the Fe magnetic moments in (ab)-plane or along c-axis. The superstructure is destroyed above Ts ~ 500 K by a first-order-like transition., Comment: 5 pages, 5 figures, 3 tables, Submitted to Phys Rev B, no change in manuscript. Fixed references to be automatically recognized by arxive system

We report on muon-spin rotation/relaxation (\muSR), electrical resistivity, magnetization and differential scanning calorimetry measurements performed on a high-quality single crystal of Cs_0.8(FeSe_0.98)_2. Whereas our transport and magnetization data confirm the bulk character of the superconducting state below T_c = 28.5(2)K, the \muSR data indicate that the system is {\it magnetic} below T_N = 478.5(3)K, where a first-order transition occurs. The first-order character of the magnetic transition is confirmed by differential scanning calorimetry data. Taken all together, these data indicate in Cs_0.8(FeSe_0.98)_2 a microscopic coexistence between the superconducting phase and a strong magnetic phase. The observed ratio between T_N and T_c is the highest one reported to date for a magnetic superconductor., Comment: 4 pages, 4 figures. Accepted for publication by Phys. Rev. Lett

We report on the synthesis of large single crystals of a new FeSe-layer superconductor Cs0.8(FeSe0.98)2. X-ray powder diffraction, neutron powder-diffraction and magnetization measurements have been used to compare the crystal structure and the magnetic properties of Cs0.8(FeSe0.98)2 with those of the recently discovered potassium intercalated system KxFe2Se2. The new compound Cs0.8(FeSe0.98)2 shows a slightly lower superconducting transition temperature (Tc=27.4 K) in comparison to 29.5 in K0.8(FeSe0.98)2). The volume of the crystal unit cell increases by replacing K by Cs - the c-parameter grows from 14.1353(13) {\AA} to 15.2846(11) {\AA}. For the so far known alkali metal intercalated layered compounds (K0.8Fe2Se2 and Cs0.8(FeSe0.98)2) the Tc dependence on the anion height (distance between Fe-layers and Se-layers) was found to be analogous to those reported for As-containing Fe-superconductors and Fe(Se1-xChx), where Ch=Te, S., Comment: 8 pages, 4 figures

We report investigation of structural phase transitions in technologically important material sodium niobate as a function of temperature on heating over 300-1075 K. Our high resolution powder neutron diffraction data show variety of structural phase transitions ranging from non-polar antiferrodistortive to ferroelectric and antiferroelectric in nature. Discontinuous jump in lattice parameters is found only at 633 K that indicates that the transition of orthorhombic antiferroelectric P (space group Pbcm) to R (space group Pbnm) phase is first order in nature, while other successive phase transitions are of second order. New superlattice reflections appear at 680 K (R phase) and 770 K (S phase) that could be indexed using an intermediate long-period modulated orthorhombic structure whose lattice parameter along <001> direction is 3 and 6 times that of the CaTiO3-like Pbnm structure respectively. The correlation of superlattice reflections with the phonon instability is discussed. The critical exponent ({\beta}) for the second order tetragonal to cubic phase transition at 950 K, corresponds to a value {\beta}$\approx 1/3$, as obtained from the temperature variation of order parameters (tilt angle and intensity of superlattice reflections). It is argued that this exponent is due to a second order phase transition close to a tricritical point. Based on our detailed temperature dependent neutron diffraction studies, the phase diagram of sodium niobate is presented that resolves existing ambiguities in the literature., Comment: 21 Pages, 8 Figures

We present a systematic study of the electronic structure in A-site ordered manganites as function of doping and temperature. The energy dependencies observed with soft x-ray resonant diffraction (SXRD) at the Mn L_{2,3} edges are compared with structural investigations using neutron powder diffraction as well as with cluster calculations. The crystal structures obtained with neutron powder diffraction reflect the various orbital and charge ordered phases and show an increase of the Mn-O-Mn bond angle as function of doping and temperature. Cluster calculations show that the observed spectral changes in SXRD as a function of doping are more pronounced than expected from an increase in bandwitdh due to the increase in Mn-O-Mn bond angle, and are best described by holes that are distributed at the neighbouring oxygen ions. These holes are not directly added to the Mn 3d shell, but centered at the Mn site. In contrast, the spectral changes in SXRD as function of temperature are best described by an increase of magnetic correlations. This demonstrates the strong correlations between orbitals and magnetic moments of the 3d states.