From One- to Two-Magnon Excitations in the S=3/2 Magnet ß-CaCr_{2}O_{4}.

We apply neutron spectroscopy to measure the magnetic dynamics in the S=3/2 magnet ß-CaCr_{2}O_{4} (T_{N}=21 K). The low-energy fluctuations, in the ordered state, resemble large-S linear spin waves from the incommensurate ground state. However, at higher energy transfers, these semiclassical and harmonic dynamics are replaced by an energy and momentum broadened continuum of excitations. Applying kinematic constraints required for energy and momentum conservation, sum rules of neutron scattering, and comparison against exact diagonalization calculations, we show that the dynamics at high-energy transfers resemble low-S one-dimensional quantum fluctuations. ß-CaCr_{2}O_{4} represents an example of a magnet at the border between classical Néel and quantum phases, displaying dual characteristics.

Long-Range Order in the Dipolar XY Antiferromagnet Er_{2}Sn_{2}O_{7}.

Er_{2}Sn_{2}O_{7} remains a puzzling case among the extensively studied frustrated compounds of the rare-earth pyrochlore family. Indeed, while a first-order transition towards a long-range antiferromagnetic state with the so-called Palmer-Chalker structure is theoretically predicted, it has not yet been observed, leaving the issue as to whether it is a spin-liquid candidate open. We report on neutron scattering and magnetization measurements which evidence a second-order transition towards this Palmer-Chalker ordered state around 108 mK. Extreme care was taken to ensure a proper thermalization of the sample, which has proved to be crucial to successfully observe the magnetic Bragg peaks. At the transition, a gap opens in the excitations, superimposed on a strong quasielastic signal. The exchange parameters, refined from a spin-wave analysis in applied magnetic field, confirm that Er_{2}Sn_{2}O_{7} is a realization of the dipolar XY pyrochlore antiferromagnet. The proximity of competing phases and the strong XY anisotropy of the Er^{3+} magnetic moment might be at the origin of enhanced fluctuations, leading to the unexpected nature of the transition, the low ordering temperature, and the observed multiscale dynamics.

Oxygen storage capacity and structural flexibility of LuFe2O4+x (0≤x≤0.5).

Combining functionalities in devices with high performances is a great challenge that rests on the discovery and optimization of materials. In this framework, layered oxides are attractive for numerous purposes, from energy conversion and storage to magnetic and electric properties. We demonstrate here the oxygen storage ability of ferroelectric LuFe2O4+x within a large x range (from 0 to 0.5) and its cycling possibility. The combination of thermogravimetric analyses, X-ray diffraction and transmission electron microscopy evidences a complex oxygen intercalation/de-intercalation process with several intermediate metastable states. This topotactic mechanism is mainly governed by nanoscale structures involving a shift of the cationic layers. The ferrite is highly promising because absorption begins at a low temperature (~=200 °C), occurs in a low oxygen pressure and the uptake of oxygen is reversible without altering the quality of the crystals. The storage/release of oxygen coupled to the transport and magnetic properties of LnFe2O4 opens the door to new tunable multifunctional applications.

Following the guidelines for communicating commensurate magnetic structures: real case examples.

A few real case examples are presented on how to report magnetic structures, with precise step-by-step explanations, following the guidelines of the IUCr Commission on Magnetic Structures [Perez-Mato et al. (2024). Acta Cryst. B80, 219-234]. Four examples have been chosen, illustrating different types of single-k magnetic orders, from the basic case to more complex ones, including odd-harmonics, and one multi-k order. In addition to acquainting researchers with the process of communicating commensurate magnetic structures, these examples also aim to clarify important concepts, which are used throughout the guidelines, such as the transformation to a standard setting of a magnetic space group.

Magnetic anisotropy, magnetization reversal and switching in Ni4Nb2O9single crystals.

Ni4Nb2O9is an insulating compensated ferrimagnet withTN= 77 K andTcomp= 33 K. We report here the study of the magnetic anisotropy using millimeter-size crystals grown in an image furnace. The magnetization measurements, vs temperature, performed withHaligned along the three main crystallographic axes, show similar Curie-Weiss temperatures (Θp≈ 190 K) and rather similar effective paramagnetic moments (from 3.5µBto 3.6µB). This suggests that the strongest magnetic interaction is the antiferromagnetic one, coupling the ferromagnetic distorted honeycomb layers and zigzag ribbons via face sharing NiO6octahedra. This strong antiferromagnetic coupling is supported by DFT calculations that do not evidence any inter site ferromagnetic interaction, leading to total compensation between magnetic moments of both Ni2+sites. Measurements vs magnetic field belowTNreveal an anisotropic behaviour, with square magnetization loops forHin theabplane, whereas linearM(H) curves without hysteresis are observed forH‖c. This anisotropy betweenabplane andcaxis occurs also in the magnetization reversal (MR), which is observed in theabplane only. Starting fromM(H) virgin curves collected just belowTcomp= 33 K withH‖aorH‖b, the memory-like effect was tested through magnetization switching induced byHorTalternating changes. BelowTcomp, smallerHis needed to switchMsymmetrically forHalongbthan alonga, and, forTswitching (2 K interval, constantH), a largerMchange is obtained alongathan alongb. The comparison with ferrimagnetic oxides which exhibit MR, like spinels or rare earth orthoferrites, shows that Ni4Nb2O9is unique since only one magnetic cation over two sites in octahedral coordination is at play, thus providing a unique platform to studyMswitching but also a challenge for theoretical interpretation.

Guidelines for communicating commensurate magnetic structures. A report of the International Union of Crystallography Commission on Magnetic Structures.

A report from the International Union of Crystallography Commission on Magnetic Structures outlining the recommendations for communicating commensurate magnetic structures.

Magnetic order and disorder environments in superantiferromagnetic [Formula: see text] nanoparticles.

Magnetic nanoparticles exhibit two different local symmetry environments, one ascribed to the core and one corresponding to the nanoparticle surface. This implies the existence of a dual spin dynamics, leading to the presence of two different magnetic arrangements governed by different correlation lengths. In this work, two ensembles of [Formula: see text] nanoparticles with mean sizes of 18 nm and 13 nm have been produced to unravel the magnetic couplings established among the magnetic moments located within the core and at the nanoparticle surface. To this end, we have combined neutron diffraction measurements, appropriate to investigate magnetically-ordered spin arrangements, with time-dependent macroscopic AC susceptibility measurements to reveal memory and aging effects. The observation of the latter phenomena are indicative of magnetically-frustrated states. The obtained results indicate that, while the [Formula: see text] magnetic moments located within the nanoparticle core keep the bulk antiferromagnetic commensurate structure in the whole magnetic state, the correlations among the surface spins give rise to a collective frustrated spin-glass phase. The interpretation of the magnetic structure of the nanoparticles is complemented by specific-heat measurements, which further support the lack of incommensurability in the nanoparticle state.

Enhanced magnetism and suppressed magnetoelastic coupling induced by electron doping in Ca1-xYxMnReO6.

The Ca2MnReO6double perovskite is a spin-orbit-assisted Mott insulator with exotic magnetic properties, including a largely non-collinear Mn2+spin arrangement and nearly orthogonal coupling between such spins and the much smaller Re 5dmagnetic moments. Here, the electron-doped compound Ca1-xYxMnReO6(x= 0.1, 0.2 and 0.3) is reported and a detailed investigation is conducted forx= 0.3. Neutron and x-ray powder diffraction confirm that nearly full chemical order is maintained at the Mn and Re sites under the Y substitution at the Ca site. X-ray absorption measurements and an analysis of the Mn-O/Re-O bond distances show that the Mn oxidation state remains stable at +2 whereas Re is reduced upon doping. The electron doping increases the magnetic ordering temperature fromTc= 121 to 150 K and also enhances significantly the ferromagnetic component of the Mn spins at the expense of the antiferromagnetic component at the base temperature (T= 3 K). The lattice parameter anomalies atTcobserved in the parent compound are suppressed by the electron doping. The possible reasons for the enhanced magnetism and the suppressed magnetoelastic coupling in Ca1.7Y0.3MnReO6are discussed.

Magnetic structures of Fe32+δGe33As2 and Fe32+δ'Ge35-xPx intermetallic compounds: a neutron diffraction and 57Fe Mössbauer spectroscopy study.

Fe32+δGe33As2 and Fe32+δ'Ge35-xPx are quasi-binary intermetallic compounds that possess a rare variant of intergrowth-type crystal structure, which is a combination of the column shaped Co2Al5 and MgFe6Ge6 structure type blocks. The compounds are antiferromagnets with the Néel temperatures around 125 K. Neutron powder diffraction experiments on the samples with δ≈ 0.1, δ'≈ 0.5 and x≈ 3 reveal commensurate magnetic ordering of low symmetry in both compounds and a non-monotonic change in the intensities of magnetic reflections. On the other hand, temperature dependence of the hyperfine fields obtained from 57Fe Mössbauer spectroscopy indicates a gradual, monotonic increase in local magnetic fields upon cooling. We interpret these results as a spin reorientation within the Co2Al5-type block of the crystal structure, with the possible formation of a non-collinear magnetic order at low temperatures. Between the compounds, the reorientation occurs at significantly different temperatures, however the resulting magnetic structures themselves are similar as well as the average values of the magnetic moments and the hyperfine fields.

Features of structure, magnetic state and electrodynamic performance of SrFe12-xInxO19.

Indium-substituted strontium hexaferrites were prepared by the conventional solid-phase reaction method. Neutron diffraction patterns were obtained at room temperature and analyzed using the Rietveld methods. A linear dependence of the unit cell parameters is found. In3+ cations are located mainly in octahedral positions of 4fVI and 12 k. The average crystallite size varies within 0.84-0.65 µm. With increasing substitution, the TC Curie temperature decreases monotonically down to ~ 520 K. ZFC and FC measurements showed a frustrated state. Upon substitution, the average and maximum sizes of ferrimagnetic clusters change in the opposite direction. The Mr remanent magnetization decreases down to ~ 20.2 emu/g at room temperature. The Ms spontaneous magnetization and the keff effective magnetocrystalline anisotropy constant are determined. With increasing substitution, the maximum of the ε/ real part of permittivity decreases in magnitude from ~ 3.3 to ~ 1.9 and shifts towards low frequencies from ~ 45.5 GHz to ~ 37.4 GHz. The maximum of the tg(α) dielectric loss tangent decreases from ~ 1.0 to ~ 0.7 and shifts towards low frequencies from ~ 40.6 GHz to ~ 37.3 GHz. The low-frequency maximum of the µ/ real part of permeability decreases from ~ 1.8 to ~ 0.9 and slightly shifts towards high frequencies up to ~ 34.7 GHz. The maximum of the tg(δ) magnetic loss tangent decreases from ~ 0.7 to ~ 0.5 and shifts slightly towards low frequencies from ~ 40.5 GHz to ~ 37.7 GHz. The discussion of microwave properties is based on the saturation magnetization, natural ferromagnetic resonance and dielectric polarization types.