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Neutron scattering is a powerful but expensive technique to study materials and discover new matter. Advanced detector technology has significantly improved the efficiency of neutron experiments, increasing the complexity of neutron data reduction and analysis. Machine learning (ML) brings new directions for neutron diffraction data reduction and experiment operation. This work presents an ML-assisted data reduction and analysis method for precise recognition of Bragg peaks and the corresponding regions of interest; it can then automatically screen and align a measured crystal using the recognized peaks, and subsequently plan and optimize the data collection with user-provided information and uncertainty quantification values of detected peaks. This method shows robust performance in different complex sample environments and enables automated single-crystal neutron diffraction.

In materials showing a linear magnetoelectric (ME) effect, unconventional functionalities can be anticipated such as electric control of magnetism and nonreciprocal optical responses. Thus, the search for new linear ME materials is of interest in materials science. Here, using a recently proposed design principle of linear ME materials, which is based on the combination of local structural asymmetry and collinear antiferromagnetism, we demonstrate that an anion-deficient fluorite derivative, Mn3Ta2O8, is a new linear ME material. This is evidenced by the onset of magnetic-field-induced electric polarization in its collinear antiferromagnetic phase below TN = 24 K. Furthermore, we also find an antiferroelectric-like phase transition at TS = 55 K, which is attributable to an off-center displacement of magnetic Mn2+ ions. The present study shows that Mn3Ta2O8 is a rare material that exhibits both ME and antiferroelectric-like transitions. Thus, Mn3Ta2O8 may provide an opportunity to investigate the physics associated with complicated interactions between magnetic (spin) and electric dipole degrees of freedom.

We describe the crystal structure and elementary magnetic properties of a previously unreported ternary intermetallic compound, Cr4PtGa17, which crystallizes in a rhombohedral unit cell in the noncentrosymmetric space group R3m. The crystal structure is closely related to those of XYZ half-Heusler compounds, where X, Y and Z are reported to be single elements only, occupying three different face-centered cubic sublattices. The new material, Cr4PtGa17, can be most straightforwardly illustrated by writing the formula as (PtGa2)(Cr4Ga14)Ga (X=PtGa2, Y = Cr4Ga14, Z = Ga), that is, the X and Y sites are occupied by clusters instead of single elements. The magnetic Cr occupies a breathing pyrochlore lattice. Ferromagnetic ordering is found below TC ~61 K, by both neutron diffraction and magnetometer studies, with a small, saturated moment of ~0.25 muB/Cr observed at 2 K, making Cr4PtGa17 the first ferromagnetically ordered material with a breathing pyrochlore lattice. A magnetoresistance of ~140% was observed at 2 K. DFT calculations suggest that the material has a nearly-half-metallic electronic structure. The new material, Cr4PtGa17, the first realization of both a half-Heusler-type structure and a breathing pyrochlore lattice, might pave a new way to achieve novel types of half-Heusler compounds., 26 pages, 6 figures, 3 tables

Charge order means that two or more distinct charge states accommodate at different atomic sites, resulting in striking variations in the structural and physical properties. Charge-ordered systems are usually electrically insulating. Here, we present the first observation of a charge-ordered metallic state in a CaFe0.95Co0.05O3 single crystal, doped with a small amount of Co, and grown at high pressure. A metal-to-insulator transition occurs on cooling to 260 K owing to the charge order between the disproportionated Fe3+ and Fe5+ states. As the temperature further decreases to 65 K, however, a reentrant metallization transition accompanied by a newly presented antiferromagnetic phase transition takes place, whereas the Fe3+ and Fe5+ charge-ordered state exists robustly. An unprecedented charge-ordered metallic state is thus unveiled to exist in the CaFe0.95Co0.05O3 single crystal. First-principles calculations suggest that the introduction of a moderate amount of Co and peculiar spiral spin texture play an important role in the existence of this novel quantum state. This study opens up a new avenue to study charge-ordered behavior in a metallic system.

Magnetic semimetals are very promising for potential applications in novel spintronic devices. Nevertheless, realizing tunable topological states with magnetism in a controllable way is challenging. Here, we report novel magnetic states and the tunability of topological semimetallic states through the control of Eu spin reorientation in Eu1−xSrxMn1−zSb2. Increasing the Sr concentration in this system induces a surprising reorientation of noncollinear Eu spins to the Mn moment direction and topological semimetallic behavior. The Eu spin reorientations to distinct collinear antiferromagnetic orders are also driven by the temperature/magnetic field and are coupled to the transport properties of the relativistic fermions generated by the 2D Sb layers. These results suggest that nonmagnetic element doping at the rare earth element site may be an effective strategy for generating topological electronic states and new magnetic states in layered compounds involving spatially separated rare earth and transition metal layers.

We report the static and dynamic magnetic properties of LaSrCrO$_4$, a seemingly canonical spin-3/2 square-lattice antiferromagnet that exhibits frustration between magnetic layers -- owing to their AB stacking -- and offers a rare testbed to investigate accidental-degeneracy lifting in magnetism. Neutron diffraction experiments on single-crystal samples uncover a remarkable anticollinear magnetic order below $T_N$ = 170 K characterized by a N\'eel arrangement of the spins within each layer and an orthogonal arrangement between adjacent layers. To understand the origin of this unusual magnetic structure, we analyze the spin-wave excitation spectrum by means of inelastic neutron scattering and bulk measurements. A spectral gap of 0.5 meV, along with a spin-flop transition at 3.2\, T, reflect the energy scale associated with the degeneracy-lifting. A minimal model to explain these observations requires both a positive biquadratic interlayer exchange and dipolar interactions, both of which are on the order of 10$^{-4}$ meV, only a few parts per million of the dominant exchange interaction $J_1 \approx 11$ meV. These results provide direct evidence for the selection of a non-collinear magnetic structure by the combined effect of two distinct degeneracy lifting interactions., Comment: 6 pages of main tex with 16 pages of supplemental material

A new member of the descloizite family, a cobalt vanadate, SrCo(VO4)(OH), has been synthesized as large single crystals using high-temperature and high-pressure hydrothermal methods. SrCo(VO4)(OH) crystallizes in the orthorhombic crystal system in space group P212121 with the following unit cell parameters: a = 6.0157(2) A, b = 7.645(2) A, c = 9.291(3) A, V = 427.29(2) A3, and Z = 4. It contains one-dimensional Co-O-Co chains of edge-sharing CoO6 octahedra along the a-axis connected to each other via VO4 tetrahedra along the b-axis forming a three-dimensional structure. The magnetic susceptibility of SrCo(VO4)(OH) indicates an antiferromagnetic transition at 10 K as well as unusually large spin orbit coupling. Single-crystal magnetic measurements in all three main crystallographic directions displayed a significant anisotropy in both temperature- and field-dependent data. Single-crystal neutron diffraction at 4 K was used to characterize the magnetically ordered state. The Co2+ magnetic spins are arranged in a staggered configuration along the chain direction, with a canting angle that follows the tipping of the CoO6 octahedra. The net magnetization along the chain direction, resulting in ferromagnetic coupling of the a-axis spin components in each chain, is compensated by an antiferromagnetic interaction between nearest neighbor chains. A metamagnetic transition appears in the isothermal magnetization data at 2 K along the chain direction, which seems to correspond to a co-alignment of the spin directions of the nearest neighbor chain. We propose a phenomenological spin Hamiltonian that describes the canted spin configuration of the ground state and the metamagnetic transition in SrCo(VO4)(OH).

In materials showing a linear magnetoelectric (ME) effect, unconventional functionalities can be anticipated such as electric control of magnetism and nonreciprocal optical responses. Thus, the search for new linear ME materials is of interest in materials science. Here, using a recently proposed design principle of linear ME materials, which is based on the combination of local structural asymmetry and collinear antiferromagnetism, we demonstrate that an anion-deficient fluorite derivative, Mn

Magnetic semimetals carry a great promise for potential applications in novel spintronic devices. Nevertheless, it is a challenging topic to realize the tunable topological states by the magnetism in a controllable way. Here, we report novel magnetic states and a tunability of the topological semimetallic states via controlling the Eu spin reorientation in Eu1-xSrxMnSb2. Increasing the Sr concentration in this system induces a surprising reorientation of noncollinear Eu spins to the Mn moment’s direction and an appearance of topological semimetallic behavior. The Eu spin reorientations to distinct collinear antiferromagnetic orders are also driven by the temperature/magnetic field, which are coupled to transport properties of the relativistic fermions generated the 2D Sb layers. These results suggest nonmagnetic element doping to the rare-earth element site may be an effective strategy to generate topological electronic states and new magnetic states in layered compounds involving spatially separated rare-earth and transition metal layers.

We have grown single crystals of ${\mathrm{Na}}_{2}\mathrm{BaNi}{({\mathrm{PO}}_{4})}_{2}$, a spin-1 equilateral triangular lattice antiferromagnet (ETLAF), and performed magnetic susceptibility, specific heat, and thermal conductivity measurements at ultralow temperatures. The main results are as follows: (i) At zero magnetic field, ${\mathrm{Na}}_{2}\mathrm{BaNi}{({\mathrm{PO}}_{4})}_{2}$ exhibits a magnetic ordering at 430 mK with a weak ferromagnetic moment along the $c$ axis. This suggests a canted ${120}^{\ensuremath{\circ}}$ spin structure, which is in a plane including the crystallographic $c$ axis due to the existence of an easy-axis anisotropy and ferromagnetically stacked along the $c$ axis. (ii) With increasing field along the $c$ axis, a 1/3 magnetization plateau is observed, which means that the canted ${120}^{\ensuremath{\circ}}$ spin structure is transformed into an up-up-down (UUD) spin structure. With even higher fields, the UUD phase further evolves into possible V and ${\mathrm{V}}^{\ensuremath{'}}$ phases. (iii) With increasing field along the $a$ axis, the canted ${120}^{\ensuremath{\circ}}$ spin structure is possibly transformed into an umbrella phase and a V phase. Therefore ${\mathrm{Na}}_{2}\mathrm{BaNi}{({\mathrm{PO}}_{4})}_{2}$ is a rare example of a spin-1 ETLAF with single-crystalline form that exhibits easy-axis spin anisotropy and a series of quantum spin state transitions.

We describe the crystal structure and elementary magnetic properties of a previously unreported ternary intermetallic compound, Cr

New surprises continue to be revealed about ${\mathrm{La}}_{2}{\mathrm{CuO}}_{4}$, the parent compound of the original cuprate superconductor. Here we present neutron scattering evidence that the structural symmetry is lower than commonly assumed. The static distortion results in anisotropic Cu-O bonds within the ${\mathrm{CuO}}_{2}$ planes; such anisotropy is relevant to pinning charge stripes in hole-doped samples. Associated with the extra structural modulation is a soft phonon mode. If this phonon were to soften completely, the resulting change in ${\mathrm{CuO}}_{6}$ octahedral tilts would lead to weak ferromagnetism. Hence, we suggest that this mode may be the ``chiral'' phonon inferred from recent studies of the thermal Hall effect. We also note the absence of interaction between the antiferromagnetic spin waves and low-energy optical phonons, in contrast to what is observed in hole-doped samples.

Spin-valley locking in monolayer transition metal dichalcogenides has attracted enormous interest, since it offers potential for valleytronic and optoelectronic applications. Such an exotic electronic state has sparsely been seen in bulk materials. Here, we report spin-valley locking in a Dirac semimetal BaMnSb2. This is revealed by comprehensive studies using first principles calculations, tight-binding and effective model analyses, angle-resolved photoemission spectroscopy measurements. Moreover, this material also exhibits a stacked quantum Hall effect (QHE). The spin-valley degeneracy extracted from the QHE is close to 2. This result, together with the Landau level spin splitting, further confirms the spin-valley locking picture. In the extreme quantum limit, we also observed a plateau in the z-axis resistance, suggestive of a two-dimensional chiral surface state present in the quantum Hall state. These findings establish BaMnSb2 as a rare platform for exploring coupled spin and valley physics in bulk single crystals and accessing 3D interacting topological states., Valley dependent spin polarization called spin-valley locking appears in absence of magnetism but it is limited to rare examples of transition metal dichalcogenides. Here, the authors report evidence of spin-valley locking and stacked quantum Hall effect in a bulk Dirac semimetal BaMnSb2.

Quantum phase transitions in quantum matter occur at zero temperature between distinct ground states by tuning a nonthermal control parameter. Often, they can be accurately described within the Landau theory of phase transitions, similarly to conventional thermal phase transitions. However, this picture can break down under certain circumstances. Here, we present a comprehensive study of the effect of hydrostatic pressure on the magnetic structure and spin dynamics of the spin-1/2 ladder compound C

We report a comprehensive inelastic neutron scattering study of the hybrid molecule-based multiferroic compound $({\mathrm{ND}}_{4}{)}_{2}{\mathrm{FeCl}}_{5}\ifmmode\cdot\else\textperiodcentered\fi{}{\mathrm{D}}_{2}\mathrm{O}$ in the zero-field incommensurate cycloidal phase and the high-field quasicollinear phase. The spontaneous electric polarization changes its direction concurrently with the field-induced magnetic transition, from mostly aligned with the crystallographic $a$ axis to the $c$ axis. To account for such a change in polarization direction, the underlying multiferroic mechanism was proposed to switch from the spin-current model induced via the inverse Dzyaloshinskii-Moriya interaction to the $p\text{\ensuremath{-}}d$ hybridization model. We perform a detailed analysis of the inelastic neutron data of $({\mathrm{ND}}_{4}{)}_{2}{\mathrm{FeCl}}_{5}\ifmmode\cdot\else\textperiodcentered\fi{}{\mathrm{D}}_{2}\mathrm{O}$ using linear spin-wave theory to quantify magnetic interaction strengths and investigate the possible impact of different multiferroic mechanisms on the magnetic couplings. Our result reveals that the spin dynamics of both multiferroic phases can be well described by a Heisenberg Hamiltonian with easy-plane anisotropy. We do not find notable differences between the optimal model parameters of the two phases. The hierarchy of exchange couplings and the balance among frustrated interactions remain the same between two phases, suggesting that magnetic interactions in $({\mathrm{ND}}_{4}{)}_{2}{\mathrm{FeCl}}_{5}\ifmmode\cdot\else\textperiodcentered\fi{}{\mathrm{D}}_{2}\mathrm{O}$ are much more robust than the electric polarization in response to delicate reorganizations of the electronic degrees of freedom in an applied magnetic field.

A new ternary selenide, Na2Mn3Se4, was prepared by a stoichiometric reaction between Na2Se4 and metallic Mn at 923 K. Crystal structure determination revealed a new structure type, built of alternating layers of Na+ ions and [Mn3Se4]2- anionic slabs. Band structure calculations indicate that Na2Mn3Se4 is an indirect band gap semiconductor with Eg = 1.59 eV, although a direct band gap is only marginally larger, at 1.64 eV. The material shows antiferromagnetic (AFM) ordering at 27 K, while the Weiss constant of ∼-400 K suggests much stronger nearest-neighbor AFM exchange between the Mn sites. This discrepancy is attributed to the strong spin frustration caused by a triangulated arrangement of the Mn sites in the [Mn3Se4]2- layer. The magnetic frustration leads to the stabilization of a complex AFM ordered structure with non-collinear arrangement of the Mn magnetic moments, as established from neutron diffraction data.

We present the results of a crystallographic analysis, magnetic characterization including neutron powder diffraction, and theoretical assessment of K2ReI6 prepared using solvent reactions. K2ReI6 crystallizes in the space group P21/n with an inversion center. Magnetic measurements of K2ReI6 sample indicate dominant antiferromagnetic coupling with a Curie–Weiss temperature of θW = −63.3(1) K, effective magnetic moment ∼2.64 μB/Re but show a weak ferromagnetism ordered at ∼24 K. Neutron powder diffraction indicates long-range order of the Re spins below 24 K, with an ordered magnetic moment of 2.2(1) μB/Re at 1.5 K. Therefore, a canted antiferromagnetic structure is concluded. The electronic structures using first-principles calculations suggest that the antiferromagnetic model of K2ReI6 yields the lowest total energy and opens a band gap with ∼1.0 eV width, which is consistent with the UV–vis–NIR optical measurements. After including the spin–orbit coupling (SOC) into the calculation, the band degeneracie...

PIONEER is a high Q-resolution, single-crystal, polarized neutron diffractometer at the Second Target Station (STS), Oak Ridge National Laboratory. It will provide the unprecedented capability of measuring tiny crystals (0.001 mm3, i.e., x-ray diffraction size), ultra-thin films (10 nm thickness), and weak structural and magnetic transitions. PIONEER benefits from the increased peak brightness of STS cold-neutron sources and uses advanced Montel mirrors that are able to deliver a focused beam with a high brilliance transfer, a homogeneous profile, and a low background. Monte Carlo simulations suggest that the optimized instrument has a high theoretical peak brilliance of 2.9 × 1012 n cm−2 sr−1 Å−1 s−1 at 2.5 Å at the sample position, within a 5 × 5 mm2 region and a ±0.3° divergence range. The moderator-to-sample distance is 60 m, providing a nominal wavelength band of 4.3 Å with a wavelength resolution better than 0.2% in the wavelength range of 1.0–6.0 Å. PIONEER is capable of characterizing large-scale periodic structures up to 200 Å. With a sample-to-detector distance of 0.8 m, PIONEER accommodates various sample environments, including low/high temperature, high pressure, and high magnetic/electric field. A large cylindrical detector array (4.0 sr) with a radial collimator is planned to suppress the background scattering from sample environments. Bottom detector banks provide an additional 0.4 sr coverage or can be removed if needed to accommodate special sample environments. We present virtual experimental results to demonstrate the scientific performance of PIONEER in measuring tiny samples.

Stabilizing an easy axis of magnetization in an octahedral Co(II) complex is an extremely challenging task, which is evident from reports that more than 90% possess easy-plane anisotropy. Here, we report a six-coordinate complex, [Co(L 1) 4(Cl) 2] (1, L 1 = thiourea [H 2N-CS-NH 2]), that exhibits a D value of −63(10) cm −1. The presence of an easy axis of magnetization associated with 1 is experimentally proven by detailed magnetic studies and polarized neutron diffraction studies, and the experimental observations are well corroborated by theoretical calculations. From the combined experimental and theoretical investigations (on 1 and many model systems), we unveil the parameters that control stabilization of negative D in a thermodynamically favorable and air-stable Co(II) ion in the common distorted octahedral geometry. This study paves the way for overcoming the current impediments to alleviate the easy axis of magnetization using rational ligand choice.

In two-dimensional (2D) metallic kagome lattice materials, destructive interference of electronic hopping pathways around the kagome bracket can produce nearly localized electrons, and thus electronic bands that are flat in momentum space. When ferromagnetic order breaks the degeneracy of the electronic bands and splits them into the spin-up majority and spin-down minority electronic bands, quasiparticle excitations between the spin-up and spin-down flat bands should form a narrow localized spin-excitation Stoner continuum coexisting with well-defined spin waves in the long wavelengths. Here we report inelastic neutron scattering studies of spin excitations in 2D metallic kagome lattice antiferromagnetic FeSn and paramagnetic CoSn, where angle resolved photoemission spectroscopy experiments found spin-polarized and nonpolarized flat bands, respectively, below the Fermi level. Our measurements on FeSn and CoSn reveal well-defined spin waves extending above 140 meV and correlated paramagnetic scattering around Γ point below 90 meV, respectively. In addition, we observed non-dispersive excitations at ~170 meV and ~360 meV arising mostly from hydrocarbon scattering of the CYTOP-M used to glue the samples to aluminum holder. Therefore, our results established the evolution of spin excitations in FeSn and CoSn, and identified anomalous flat modes overlooked by the neutron scattering community for many years. By exploiting the geometric frustration of a kagome crystal lattice, it is possible to enhance electron localisation and engineer exotic electronic structures such as electronic flat bands. Here, the authors use inelastic neutron scattering to investigate the evolution of spin excitations modes for FeSn and CoSn, finding that an anomalous flat mode actually arises from the material used to fix the sample to the aluminium holder for analysis instead of the expected magnetic flat bands.

$A$Co$_2$Se$_2$ ($A$=K,Rb,Cs) is a homologue of the iron-based superconductor, $A$Fe$_2$Se$_2$. From a comprehensive study of RbCo$_2$Se$_2$ via measurements of magnetization, transport, neutron diffraction, angle-resolved photoemission spectroscopy, and first-principle calculations, we identify a ferromagnetic order accompanied by an orbital-dependent spin-splitting of the electronic dispersions. Furthermore, we identify the ordered moment to be dominated by a $d_{x^2-y^2}$ flatband near the Fermi level, which exhibits the largest spin splitting across the ferromagnetic transition, suggesting an itinerant origin of the ferromagnetism. In the broader context of the iron-based superconductors, we find this $d_{x^2-y^2}$ flatband to be a common feature in the band structures of both iron-chalcogenides and iron-pnictides, accessible via heavy electron doping., 8 pages, 7 figures, accepted by Phys. Rev. B

PbMO3 (M = 3d transition metals) family shows systematic variations in charge distribution and intriguing physical properties due to its delicate energy balance between Pb 6s and transition metal 3d orbitals. However, the detailed structure and physical properties of PbFeO3 remain unclear. Herein, we reveal that PbFeO3 crystallizes into an unusual 2ap × 6ap × 2ap orthorhombic perovskite super unit cell with space group Cmcm. The distinctive crystal construction and valence distribution of Pb2+0.5Pb4+0.5FeO3 lead to a long range charge ordering of the -A-B-B- type of the layers with two different oxidation states of Pb (Pb2+ and Pb4+) in them. A weak ferromagnetic transition with canted antiferromagnetic spins along the a-axis is found to occur at 600 K. In addition, decreasing the temperature causes a spin reorientation transition towards a collinear antiferromagnetic structure with spin moments along the b-axis near 418 K. Our theoretical investigations reveal that the peculiar charge ordering of Pb generates two Fe3+ magnetic sublattices with competing anisotropic energies, giving rise to the spin reorientation at such a high critical temperature., PbFeO3 is part of a family of lead based perovskites with many intriguing properties; however, difficulties in synthesis have hampered investigation. Here, the authors present a detailed study of the structure of PbFeO3 observing unique charge ordering and spin orientation among the constituent ions.