Single-crystal Neutron Research Articles

Infrared furnace for in situ neutron single-crystal diffraction studies in controlled gas atmospheres at high temperatures

To understand oxygen diffusion mechanisms in non-stoichiometric oxides, the possibility to explore structural changes as a function of the oxygen partial pressure with temperature and related oxygen bulk stoichiometry is mandatory. This article reports on the realization of a high-temperature furnace, suitable for single-crystal neutron diffraction, working continuously at temperatures of up to 1000°C at different and adjustable partial gas pressures of up to 2 bar (1 bar = 100 kPa). This allows exploration of the phase diagrams of non-stoichiometric oxides under in situ conditions and controlled oxygen partial pressure. As a pilot study, the structural changes of Pr2NiO4+δ were explored at room temperature (δ ≃ 0.24) and at 900°C under 1 bar P(O2) (δ ≃ 0.13) as well as under secondary vacuum (approximately 10−5 mbar) conditions yielding a δ close to zero. The strong anharmonic displacements of the apical oxygen atoms along the [110] shallow diffusion pathway, which were previously observed at room temperature and 400°C, become more isotropic at 900°C. The study shows that the anisotropic oxygen displacements, here related to lattice instabilities, play a major role in understanding oxygen diffusion pathways and related activation energies at moderate temperatures. This also shows the importance of the availability of reaction cells for single-crystal neutron diffraction to explore the phase diagram and associated structural changes of non-stoichiometric oxygen ion conductors and respective diffusion mechanisms.

Magnetic structure investigation of the intercalated transition metal dichalcogenide V1/3NbS2

We investigate the temperature evolution of the magnetic structure of ${\mathrm{V}}_{1/3}{\mathrm{NbS}}_{2}$ using neutron diffraction techniques. We find that ${\mathrm{V}}_{1/3}{\mathrm{NbS}}_{2}$ has two propagation vectors: ${\mathbf{k}}_{\mathbf{0}}=(0,0,0)$ and ${\mathbf{k}}_{\mathbf{1}}=(0,0,\frac{1}{3})$. The ${\mathbf{k}}_{\mathbf{0}}$ vector can be associated with an antiferromagnetic ordering of in-plane moments with a refined value of $0.90(5){\ensuremath{\mu}}_{\mathrm{B}}$, and ${\mathbf{k}}_{\mathbf{1}}$ can be associated with moments along the $c$ axis in an up-down-down configuration with refined values of $1.21(12){\ensuremath{\mu}}_{\mathrm{B}}$ and $0.61(6){\ensuremath{\mu}}_{\mathrm{B}}$. Both ${\mathbf{k}}_{\mathbf{0}}$ and ${\mathbf{k}}_{\mathbf{1}}$ magnetic components couple with an out-of-plane ferromagnetic moment consistent with magnetization data. Furthermore, single-crystal neutron diffraction shows evidence of diffuse magnetic scattering between the (010) and ($01\ifmmode\pm\else\textpm\fi{}\frac{1}{3}$) Bragg peaks. We also characterize the field and temperature evolution of the magnetic structure in ${\mathrm{V}}_{1/3}{\mathrm{NbS}}_{2}$ by magnetic susceptibility and heat capacity measurements. The dc susceptibility measurements give an antiferromagnetic transition temperature of ${T}_{\mathrm{N}}=50$ K, and the field scans reveal that the moment does not saturate at magnetic fields up to 100 kOe.

Magnetic ordering inLa1.5Ca0.5CoO4revealed by resonant magnetic x-ray scattering and neutron diffraction

We report a comprehensive study on the magnetic ground state of ${\mathrm{La}}_{1.5}{\mathrm{Ca}}_{0.5}\mathrm{Co}{\mathrm{O}}_{4}$ combining single crystal neutron diffraction and resonant magnetic x-ray scattering at the $\mathrm{Co}\phantom{\rule{0.16em}{0ex}}{L}_{2,3}$ edges. Three single-crystal samples obtained from the same boule were investigated exhibiting magnetic phase transitions from a high-temperature paramagnetic phase to an antiferromagnetic phase at ${T}_{\mathrm{N}}\ensuremath{\approx}52\phantom{\rule{0.16em}{0ex}}\mathrm{K}$. Single crystal neutron diffraction reveals that the crystal structure at room temperature shows an orthorhombic $A$-centered lattice but with $a$ and $b$ axes almost equal in length. The structural phase transition (charge-ordering-like) from the parent tetragonal cell takes place above 523 K into the space group $A2mm$ where two nonequivalent compressed and expanded $\mathrm{Co}{\mathrm{O}}_{6}$ octahedra are ordered showing a checkerboard pattern in the $ab$ plane. The charge segregation between the nonequivalent Co sites is about 0.4(1) electrons. Resonant magnetic x-ray reflections indexed as ${(1/4,\phantom{\rule{0.16em}{0ex}}1/4,\phantom{\rule{0.16em}{0ex}}0)}_{\mathrm{t}}$, ${(1/4,\phantom{\rule{0.16em}{0ex}}1/4,\phantom{\rule{0.16em}{0ex}}1)}_{\mathrm{t}}$, and ${(1/4,\phantom{\rule{0.16em}{0ex}}1/4,\phantom{\rule{0.16em}{0ex}}1/2)}_{\mathrm{t}}$ in the parent tetragonal cell were observed at low temperature at the $\mathrm{Co}\phantom{\rule{0.16em}{0ex}}{L}_{2,3}$-edge energy range. The resonant spectral shape, with a noticeable absence of any resonant enhancement at the $\mathrm{Co}\phantom{\rule{0.16em}{0ex}}{L}_{2}$ edge, indicates that only ${\mathrm{Co}}^{2+}$-like ions participate in the magnetic ordering. The polarization analysis discloses that the orientation of Co magnetic moments is the same for the three magnetic orders and they are long-range ordered along the diagonal in the $ab$ plane of the parent tetragonal cell with a slight tilt in the $c$ axis. Despite the onset temperatures for the three resonant magnetic reflections being the same, $\ensuremath{\approx}55\phantom{\rule{0.16em}{0ex}}\mathrm{K}$, different thermal behavior is observed between ${(1/4,\phantom{\rule{0.16em}{0ex}}1/4,\phantom{\rule{0.16em}{0ex}}1/2)}_{\mathrm{t}}$ and ${(1/4,1/4,L)}_{\mathrm{t}}$ ($L=\mathrm{integer}$) reflections whose intensities maximize at different temperatures, suggesting the coexistence of two magnetic arrangements. Moreover, the intensity of the ${(1/4,\phantom{\rule{0.16em}{0ex}}1/4,\phantom{\rule{0.16em}{0ex}}1/2)}_{\mathrm{t}}$ magnetic reflection is at least ten times larger than that of the ${(1/4,1/4,L)}_{\mathrm{t}}$ $(L=\mathrm{integer})$ ones. On the other hand\, neutron diffraction measurements only detect a single type of antiferromagnetic ordering following the propagation vector $\mathbit{k}={(1/4,\phantom{\rule{0.16em}{0ex}}1/4,\phantom{\rule{0.16em}{0ex}}1/2)}_{\mathrm{t}}$ that involves half of the Co atoms in the unit cell. We conclude that the bulk magnetic order in ${\mathrm{La}}_{1.5}{\mathrm{Ca}}_{0.5}\mathrm{Co}{\mathrm{O}}_{4}$ corresponds then to this propagation vector $\mathbit{k}={(1/4,\phantom{\rule{0.16em}{0ex}}1/4,\phantom{\rule{0.16em}{0ex}}1/2)}_{\mathrm{t}}$ while ${(1/4,\phantom{\rule{0.16em}{0ex}}1/4,\phantom{\rule{0.16em}{0ex}}0)}_{\mathrm{t}}$ and ${(1/4,\phantom{\rule{0.16em}{0ex}}1/4,\phantom{\rule{0.16em}{0ex}}1)}_{\mathrm{t}}$ magnetic reflections correspond to a minority magnetic phase that must be due to changes in the oxygen stoichiometry near the surface.

Neutron Scattering as a Powerful Tool to Investigate Magnetic Shape Memory Alloys: A Review

Magnetic shape memory alloys (MSMAs) are an interesting class of smart materials characterized by undergoing macroscopic deformations upon the application of a pertinent stimulus: temperature, stress and/or external magnetic fields. Since the deformation is rapid and contactless, these materials are being extensively investigated for a plethora of applications, such as sensors and actuators for the medical, automotive and space industries, energy harvesting and damping devices, among others. These materials also exhibit a giant magnetocaloric effect, whereby they are very promising for magnetic refrigeration. The applications in which they can be used are extremely dependent on the material properties, which are, in turn, greatly conditioned by the structure, atomic ordering and magnetism of a material. Particularly, exploring the material structure is essential in order to push forward the current application limitations of the MSMAs. Among the wide range of available characterization tools, neutron scattering techniques stand out in acquiring advanced knowledge about the structure and magnetism of these alloys. Throughout this manuscript, a comprehensive review about the characterization of MSMAs using neutron techniques is presented. Several elastic neutron scattering techniques will be explained and exemplified, covering neutron imaging techniques—such as radiography, tomography and texture diffractometry; diffraction techniques—magnetic (polarized neutron) diffraction, powder neutron diffraction and single crystal neutron diffraction, reflectometry and small angle neutron scattering. This will be complemented with a few examples where inelastic neutron scattering has been employed to obtain information about the phonon dispersion in MSMAs.

Site Mixing for Engineering Magnetic Topological Insulators

The van der Waals compound, MnBi$_2$Te$_4$, is the first intrinsic magnetic topological insulator, providing a materials platform for exploring exotic quantum phenomena such as the axion insulator state and the quantum anomalous Hall effect. However, intrinsic structural imperfections lead to bulk conductivity, and the roles of magnetic defects are still unknown. With higher concentrations of same types of magnetic defects, the isostructural compound MnSb$_2$Te$_4$ is a better model system for a systematic investigation of the connections among magnetic, topology and lattice defects. In this work, the impact of antisite defects on the magnetism and electronic structure is studied in MnSb$_2$Te$_4$. Mn-Sb site mixing leads to complex magnetic structures and tunes the interlayer magnetic coupling between antiferromagnetic and ferromagnetic. The detailed nonstoichiometry and site-mixing of MnSb$_2$Te$_4$ crystals depend on the growth parameters, which can lead to $\approx$40\% of Mn sites occupied by Sb and $\approx$15\% of Sb sites by Mn in as-grown crystals. Single crystal neutron diffraction and electron microscopy studies show nearly random distribution of the antisite defects. Band structure calculations suggest that the Mn-Sb site-mixing favors a FM interlayer coupling, consistent with experimental observation, but is detrimental to the band inversion required for a nontrivial topology. Our results suggest a long range magnetic order of Mn ions sitting on Bi sites in MnBi$_2$Te$_4$. The effects of site mixing should be considered in all layered heterostructures that consist of alternating magnetic and topological layers, including the entire family of MnTe(Bi$_2$Te$_3$)$_n$, its Sb analogs and their solid solution.

Canted antiferromagnetic order and spin dynamics in the honeycomb-lattice compound Tb2Ir3Ga9

Single crystal neutron diffraction, inelastic neutron scattering, bulk magnetization measurements, and first-principles calculations are used to investigate the magnetic properties of the honeycomb lattice $\rm Tb_2Ir_3Ga_9$. While the $R\ln2$ magnetic contribution to the low-temperature entropy indicates a $\rm J_{eff}=1/2$ moment for the lowest-energy crystal-field doublet, the Tb$^{3+}$ ions form a canted antiferromagnetic structure below 12.5 K. Due to the Dzyalloshinskii-Moriya interactions, the Tb moments in the $ab$ plane are slightly canted towards $b$ by $6^\circ$ with a canted moment of 1.22 $\mu_{\rm B} $ per formula unit. A minimal $xxz$ spin Hamiltonian is used to simultaneously fit the spin-wave frequencies along the high symmetry directions and the field dependence of the magnetization along the three crystallographic axes. Long-range magnetic interactions for both in-plane and out-of-plane couplings up to the second nearest neighbors are needed to account for the observed static and dynamic properties. The $z$ component of the exchange interactions between Tb moments are larger than the $x$ and $y$ components. This compound also exhibits bond-dependent exchange with negligible nearest exchange coupling between moments parallel and perpendicular to the 4$f$ orbitals. Despite the $J_{{\rm eff}}=1/2$ moments, the spin Hamiltonian is denominated by a large in-plane anisotropy $K_z \sim -1$ meV. DFT calculations confirm the antiferromagnetic ground state and the substantial inter-plane coupling at larger Tb-Tb distances.

Insights into Host–Guest Binding in Hydroquinone Clathrates: Single-Crystal X-ray and Neutron Diffraction, and Complementary Computational Studies on the Hydroquinone-CO2 Clathrate

High-resolution 100 K X-ray and neutron single-crystal diffraction data of the non-stoichiometric hydroquinone-CO2 (HQ-CO2) clathrate are combined, with the aim of providing further insight into ho...

Magnetostructural coupling in ilmenite-type NiTiO3

We report the ground state magnetic structure and in-field magnetostrictive effects of $\mathrm{Ni}\mathrm{Ti}{\mathrm{O}}_{3}$ studied by means of zero-field and in-field single-crystal neutron diffraction, magnetization, and high-resolution dilatometry experiments. Zero-field neutron diffraction on $\mathrm{Ni}\mathrm{Ti}{\mathrm{O}}_{3}$ single crystals confirms an easy-plane antiferromagnet with a multidomain ground state. Upon application of external magnetic fields, neutron diffraction shows the evolution of domains with spins perpendicular to the applied field. The rotation of spins in the multidomain state exhibits pronounced lattice changes in the magnetostriction measurements. We see magnetization and magnetostriction measurements scale with each other in the multidomain state in accordance with phenomenological theories, revealing the strong coupling of spins to the lattice.

Deterioration of hydrogen-bonded superprotonic conductors belonging to CsHSO4–CsH2PO4–H2O salt system: a single-crystal neutron diffraction investigation

Single-crystal neutron diffraction investigation on Cs4(HSO4)3(H2PO4) and Cs6H(HSO4)3(H2PO4)4 superprotonic crystals, belonging to CsHSO4–CsH2PO4–H2O salt system, is under taken to elucidate the precise hydrogen atom positions in these crystals. The investigation revealed that these crystals are very sensitive to the ambient conditions and can undergo deterioration due to fluctuation in air moisture content. Cs6H(HSO4)3(H2PO4)4 crystals are more stable as compared to Cs4(HSO4)3(H2PO4). Crystal structure of Cs6H(HSO4)3(H2PO4)4 is obtained both before and after deterioration, it is found that the asymmetric O–HO hydrogen bond between the PO4 and SO4 ions of this crystal becomes stronger after deterioration. This led to the shrinkage of the unit cell, and most likely prevented further deterioration. Diabatic state model for hydrogen bonds is used to obtain the energy contour for the O–H···O hydrogen bond of Cs6H(HSO4)3(H2PO4)4 crystal. The influence of this change in the hydrogen bonding on the proton conduction ability of the crystal is discussed.

Tuning the flat bands of the kagome metal CoSn with Fe, In, or Ni doping

CoSn is a Pauli paramagnet with relatively flat d-bands centered about 100 meV below the Fermi energy Ef. Single crystals of CoSn lightly doped with Fe, In, or Ni are investigated using x-ray and neutron scattering, magnetic susceptibility and magnetization, ac susceptibility, specific heat and resistivity measurements. Within the rigid band approximation, hole doping with a few percent of Fe or In should move the flat bands closer to Ef, whereas electron doping with Ni should move the flat bands further away from Ef. We provide evidence that this indeed occurs. Fe and In doping drive CoSn toward magnetism, while Ni doping suppresses CoSn's already weak magnetic response. The resulting ground state is different for Fe versus In doping. For Fe-doped crystals, Co1-xFexSn, with 0.02 < x < 0.27, the magnetic and specific heat data are consistent with the formation of a spin glass, with a glass transition temperature, Tg, ranging from 1 K for x=0.02 to 10 K for x= 0.27. Powder and single crystal neutron diffraction found no evidence of long-range magnetic order below Tg with x = 0.17. For In-doped crystals, CoSn1-yIny, both the magnetic susceptibility and the Sommerfeld coefficient, gamma, increase substantially relative to pure CoSn, but with no clear indication of a magnetic transition for 0.05 < y < 0.2. CoSn crystals doped with Ni (Co0.93Ni0.07Sn) have a significantly smaller magnetic susceptibility and gamma than pure CoSn, consistent with the flat bands further from Ef.

Inelastic neutron scattering determination of the spin Hamiltonian for BaCdVO(PO4)2

Single crystal inelastic neutron scattering is used to study spin wave excitations in the fully polarized state of the frustrated quantum ferro-antiferromagnet BaCdVO(PO$_4$)$_2$. The data analysis is based on a Heisenberg spin Hamiltonian that includes as many distinct nearest-neighbor and next-nearest neighbor interactions as allowed by crystal symmetry. All 8 such exchange constants are obtained in a simultaneous fit to over 150 scans across the dispersion manifold. This establishes a definitive quantitative model of this material. It turns out to be substantially different from the one assumed in numerous previous studies based on powder experiments.

High-resolution optical spectroscopy, magnetic properties, and single-crystal neutron diffraction of multiferroic HoFe3(BO3)4 : Magnetic structure

The magnetic structure is usually determined by the neutron diffraction measurements. However, in the case of complex multisublattice magnetics, this method fails to give an unambiguous result. Here, on the example of multiferroic ${\mathrm{HoFe}}_{3}{({\mathrm{BO}}_{3})}_{4}$, we show that in the case of rare-earth (RE) compounds the right magnetic structure can be determined by additionally using optical spectroscopy and a theoretical analysis based on spectroscopic data. ${\mathrm{HoFe}}_{3}{({\mathrm{BO}}_{3})}_{4}$ demonstrates a series of phase transitions and interesting magnetic and magnetoelectric properties. The available information on the magnetic structure of the compound, necessary for understanding and utilizing these properties, is contradictory. To resolve the existing ambiguities, we apply a combined approach. The high-resolution spectroscopy data deliver a set of the ${\mathrm{Ho}}^{3+}$ crystal-field (CF) levels in the paramagnetic and both easy-plane and easy-axis magnetic phases. These data are used to determine CF and ${\mathrm{Ho}}^{3+}\text{\ensuremath{-}}{\mathrm{Fe}}^{3+}$ exchange parameters and, then, to calculate the temperature dependencies of the magnetic susceptibility tensor of ${\mathrm{HoFe}}_{3}{({\mathrm{BO}}_{3})}_{4}$. Based on these calculations, we suggest an easy-plane antiferromagnetic structure with a collinear arrangement of the Fe spins along the $a$ axis and induced noncolinear moments of magnetically nonequivalent Ho ions. The suggested structure is further confirmed by single-crystal elastic neutron scattering experiments. We argue that specific features of the magnetic properties of RE iron borates isostructural to ${\mathrm{HoFe}}_{3}{({\mathrm{BO}}_{3})}_{4}$ are governed by the energy patterns and the symmetry properties of the wave functions of the lower CF levels of the RE ground multiplet in the crystal field of the ${C}_{2}$ symmetry.

Neutron and XRD Single-Crystal Diffraction Study and Vibrational Properties of Whitlockite, the Natural Counterpart of Synthetic Tricalcium Phosphate

A crystal chemical investigation of a natural specimen of whitlockite, ideally Ca9Mg(PO4)6[PO3(OH)], from Palermo Mine (USA), was achieved by means of a combination of electron microprobe analysis (EMPA) in WDS mode, single-crystal neutron diffraction probe (NDP) and single-crystal X-ray diffraction (XRD), and Fourier transform infrared (FTIR) spectroscopy. The crystal-chemical characterization resulted in the empirical formula (Ca8.682Na0.274Sr0.045)Σ9.000(Ca0.034□0.996)Σ1.000(Mg0.533Fe2+0.342Mn2+0.062Al0.046)Σ0.983(P1.006O4)6[PO3(OH0.968F0.032)Σ1.000]. Crystal-structure refinement, in the space group R3c, converged to R1 = 7.12% using 3273 unique reflections from NDP data and to R1 = 2.43% using 2687 unique reflections from XRD data. Unit cell parameters from NDP are a = 10.357(3) Å, c = 37.095(15) Å and V = 3446(2) Å3, and from XRD, the parameters are a = 10.3685(4) Å, c = 37.1444(13) Å and V = 3458.2(3) Å3. NDP results allowed a deeper definition of the hydrogen-bond system and its relation with the structural unit [PO3(OH)]. The FTIR spectrum is very similar to that of synthetic tricalcium phosphate Ca3(PO4)2 and displays minor band shifts due to slightly different P-O bond lengths and to the presence of additional elements in the structure. A comparison between whitlockite, isotypic phases from the largest merrillite group, and its synthetic counterpart Ca3(PO4)2 is provided, based on the XRD/NDP and FTIR results.

Crystal and magnetic structure of the (trimim)[FeBr4] molten salt: A temperature dependence study

A new imidazolium-based halometallate complex with formula (trimim)[FeBr4] (trimim: 1,2,3-trimethylimidazolium) has been synthesized and characterized as a function of the temperature. The structural phase transitions, magnetic properties and magnetic structure of this compound have been thoroughly studied. The crystal structure evolution from 1.8 to 400 K has been investigated by a combination of synchrotron X-ray and neutron powder diffraction, as well as single crystal X-ray and neutron diffraction. Four different phases were found: phase I, from 400 to 350 K, with the orthorhombic Cmc21 space group; phase II, from 350 to 160 K, which was modelled with the monoclinic P21/m space group; and phase III, stable down to 13 K and showing the monoclinic Cm space group. The transition from phase III to II involves the appearance of disorder in the organic cations. Magnetometry measurements indicate a long-range magnetic order below 13 K, which was confirmed by single crystal and powder neutron X-ray diffraction analyses. The occurrence of new reflections that were not possible to index with the phase III unit cell suggests a symmetry breaking, giving rise to the phase IV. A joint refinement (single-crystal and powder data) revealed that the latter phase exhibits the magnetic Shubnikov Ccc space group. This model consists of a strictly antiferromagnetic structure with ferromagnetic interactions within the unit cell, which is compatible with the magnetometry results.

Neutron scattering investigation of proposed Kosterlitz-Thouless transitions in the triangular-lattice Ising antiferromagnet TmMgGaO4

The transverse-field Ising model on the triangular lattice is expected to host an intermediate finite-temperature Kosterlitz-Thouless (KT) phase through a mapping of the spins on each triangular unit to a complex order parameter. TmMgGaO$_4$ is a candidate material to realize such physics due to the non-Kramers nature of Tm$^{3+}$ ion and the resulting two-singlet single-ion ground state. Using inelastic neutron scattering, we confirm this picture by determining the leading parameters of the low-energy effective Hamiltonian of TmMgGaO$_4$. Subsequently, we track the predicted KT phase and related transitions by inspecting the field and temperature dependence of the ac susceptibility. We further probe the spin correlations in both reciprocal space and real space via single crystal neutron diffraction and magnetic total scattering techniques, respectively. Magnetic pair distribution function analysis provides evidence for the formation of vortex-antivortex pairs that characterize the proposed KT phase around 5~K. Although structural disorder influences the field-induced behavior of TmMgGaO$_4$, the magnetism in zero field appears relatively free from these effects. These results position TmMgGaO$_4$ as a strong candidate for a solid-state realization of KT physics in a dense spin system.

Operando single crystal neutron diffraction reveals insight into the field response mechanisms in the hydrogen-bonded KH2PO4 ferroelectric

The mechanism that facilitates polarization reorientation in KH2PO4 (KDP) was investigated using operando single-crystal neutron diffraction. Diffraction data were measured from a KDP single crystal during the application of alternating electric fields and were then binned into 40 increments to enable field-dependent single-crystal structure refinements. The field-dependent structures are compared with an as-grown crystal to determine how the lattice and atomic sites evolve in response to the applied electric fields. These analyses provide evidence that the reorientation of the macroscopic polarization is facilitated through a cooperative change in hydrogen bonding, which results in the reversal of the spontaneous dipole. In addition, a decrease in secondary extinction near the coercive field indicates that the inversion of the macroscopic polarization is achieved through the nucleation and subsequent growth of new domains.

High-field spin-flop state in green dioptase

The high-field magnetic properties and magnetic order of the gem mineral green dioptase Cu$_6[$Si$_6$O$_{18}]\cdot 6$H$_2$O have been studied by means of single-crystal neutron diffraction in magnetic fields up to $21~$T and magnetization measurements up to $30~$T. In zero field, the Cu$^{2+}$-moments in the antiferromagnetic chains are oriented along the $c$-axis with a small off-axis tilt. For a field applied parallel to the $c$-axis, the magnetization shows a spin-flop-like transition at $B^*=12.2~$T at $1.5~$K. Neutron diffraction experiments show a smooth behavior in the intensities of the magnetic reflections without any change in the periodicity of the magnetic structure. Bulk and microscopic observations are well described by a model of ferromagnetically coupled antiferromagnetic $XXZ$ spin-$\frac{1}{2}$ chains, taking into account a change of the local easy-axis direction. We demonstrate that the magnetic structure evolves smoothly from a deformed N\'eel state at low fields to a deformed spin-flop state in a high field via a strong crossover around $B^*$. The results are generalized for different values of interchain coupling and spin anisotropy.

Correlated Li-ion migration in the superionic conductor Li10GeP2S12

A combination of single-crystal neutron diffraction experiments at low temperature and first-principles calculations revealed that a correlated migration of the densely packed Li ions governs the overall Li-ion conduction in Li10GeP2S12.

Structural, electronic, and magnetic properties of nearly ideal Jeff=12 iridium halides

Heavy transition metal magnets with $J_{\rm eff}$ $=$ 1/2 electronic ground states have attracted recent interest due to their penchant for hosting new classes of quantum spin liquids and superconductors. Unfortunately, model systems with ideal $J_{\rm eff}$ $=$ 1/2 states are scarce due to the importance of non-cubic local distortions in most candidate materials. In this work, we identify a family of iridium halide systems [i.e. K$_2$IrCl$_6$, K$_2$IrBr$_6$, (NH$_4$)$_2$IrCl$_6$, and Na$_2$IrCl$_6 \cdotp $ 6(H$_2$O)] with Ir$^{4+}$ electronic ground states in extremely close proximity to the ideal $J_{\rm eff}$ $=$ 1/2 limit, despite a variation in the low-temperature global crystal structures. We also find ordered magnetic ground states for the three anhydrous systems, with single crystal neutron diffraction on K$_2$IrBr$_6$ revealing Type-I antiferromagnetism. This spin configuration is consistent with expectations for significant Kitaev exchange in a face-centered-cubic magnet.

Noncollinear magnetic structure and magnetoelectric coupling in buckled honeycomb Co4Nb2O9 : A single-crystal neutron diffraction study

Through analysis of single crystal neutron diffraction data, we present the magnetic structures of magnetoelectric Co4Nb2O9 under various magnetic fields. In zero-field, neutron diffraction experiments below TN=27 K reveal that the Co2+ moments order primarily along the a* direction without any spin canting along the c axis, manifested by the magnetic symmetry C2/c'. The moments of nearest neighbor Co atoms order ferromagnetically with a small cant away from the next nearest neighbor Co moments along the c axis. In the applied magnetic field H//a, three magnetic domains were aligned with their major magnetic moments perpendicular to the magnetic field with no indication of magnetic phase transitions. The influences of magnetic fields on the magnetic structures associated with the observed magnetoelectric coupling are discussed.