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Altermagnets (AMs) are a new class of magnetic materials that combine the beneficial spintronics properties of ferromagnets and antiferromagnets, garnering significant attention recently. Here, we have identified altermagnetism in a layered intercalated transition metal diselenide, CoNb$_4$Se$_8$, which crystallizes with an ordered sublattice of intercalated Co atoms between NbSe$_2$ layers. Single crystals are synthesized, and the structural characterizations are performed using single crystal diffraction and scanning tunneling microscopy. Magnetic measurements reveal easy-axis antiferromagnetism below 168 K. Density functional theory (DFT) calculations indicate that A-type antiferromagnetic ordering with easy-axis spin direction is the ground state, which is verified through single crystal neutron diffraction experiments. Electronic band structure calculations in this magnetic state display spin-split bands, confirming altermagnetism in this compound. The layered structure of CoNb$_4$Se$_8$ presents a promising platform for testing various predicted properties associated with altermagnetism.

We report a comprehensive investigation of the lattice and magnetic structure in van der Waals antiferromagnet VBr3, characterized by a BiI3-type structure at room temperature. Neutron diffraction experiments were performed on both polycrystalline and single-crystalline VBr3 samples, revealing clear magnetic Bragg peaks emerging below the N\'eel temperature of TN = 26.5 K. These magnetic Bragg peaks can be indexed by k = (0, 0.5, 1) in hexagonal notation. Our refinement analysis suggests that the antiferromagnetic order in VBr3 manifests as a zigzag structure. Moreover, we observed peak splitting for nuclear Bragg peaks in the HK-plane below the structure transition temperature of Ts = 94 K, indicating the breaking of 3-fold symmetry within the ab-plane., Comment: 13 pages, 4 figures

The discovery of ferroelectricity in hafnia-based materials have boosted the potential of incorporating ferroelectrics in advanced electronics, thanks to their compatibility with silicon technology. However, comprehending why these materials defy the common trend of reduced ferroelectric ordering at the nanoscale, and the mechanism that stabilizes the ferroelectric phase (absent in hafnia phase diagram) presents significant challenges to traditional knowledge of ferroelectricity. In this work, we show that the formation of the orthorhombic ferroelectric phase (o-FE, space group Pca21) of the single-crystalline epitaxial films of 10% La-doped HfO2 (LHO) on (111)-oriented yttria stabilized zirconia (YSZ) relies on the stability of the high-pressure orthorhombic antiferroelectric phase (o-AFE, space group Pbca). Our detailed structural characterizations demonstrate that as-grown LHO films represent largely the o-AFE phase being thermodynamically stabilized by the compressive strain. Our Kelvin probe force microscopy studies show, under mechanical poling, the o-AFE phase is converted to the o-FE phase which remains stable under ambient conditions. We find that the orthorhombic phase stability is enhanced in thinner films down to one-unit-cell thickness, a trend that is unknown in any other ferroelectric films. This is due to the vanishing depolarization field of the o-AFE phase and the isomorphic LHO/YSZ interface, supporting strain-enhanced ferroelectricity in the ultrathin films. This results in an unprecedented increase of the Curie temperature up to 850 {\deg}C, the highest reported for sub-nanometer-thick ferroelectrics. Overall, our findings opens the way for advanced engineering of hafnia-based materials for ferroelectric applications and heralding a new frontier of high-temperature ferroelectrics at the two-dimensional limit.

The field of spintronics has seen a surge of interest in altermagnetism due to novel predictions and many possible applications. MnTe is a leading altermagnetic candidate that is of significant interest across spintronics due to its layered antiferromagnetic structure, high Neel temperature (TN ~ 310 K) and semiconducting properties. We present results on molecular beam epitaxy (MBE) grown MnTe/InP(111) films. Here, it is found that the electronic and magnetic properties are driven by the natural stoichiometry of MnTe. Electronic transport and in situ angle-resolved photoemission spectroscopy show the films are natively metallic with the Fermi level in the valence band and the band structure is in good agreement with first principles calculations for altermagnetic spin-splitting. Neutron diffraction confirms that the film is antiferromagnetic with planar anisotropy and polarized neutron reflectometry indicates weak ferromagnetism, which is linked to a slight Mn-richness that is intrinsic to the MBE grown samples. When combined with the anomalous Hall effect, this work shows that the electronic response is strongly affected by the ferromagnetic moment. Altogether, this highlights potential mechanisms for controlling altermagnetic ordering for diverse spintronic applications., Comment: Accepted in Advanced Functional Materials

Magnetic topological insulators provide a platform for emergent phenomena arising from the interplay between magnetism and band topology. Here we report the single crystal growth, crystal structure, magnetic and transport properties, as well as the neutron scattering studies of topological insulator series (Ge$_{1-\delta-x}$Mn$_x$)$_2$Bi$_2$Te$_5$ ($x\leq 0.47$, $0.11 \leq \delta \leq 0.20$). Upon doping up to $x = 0.47$, the lattice parameter $c$ decreases by 0.8\%, while the lattice parameter $a$ remains nearly unchanged. Significant Ge vacancies and Ge/Bi site mixing are revealed via elemental analysis as well as refinements of the neutron and X-ray diffraction data, resulting in holes dominating the charge transport. At $x = 0.47$, below 10.8 K, a bilayer A-type antiferromagnetic ordered state emerges, featuring an ordered moment of 3.0(3) $\mu_{B}$/Mn at 5 K, with the $c$ axis as the easy axis. Magnetization data unveil a much stronger interlayer antiferromagnetic exchange interaction and a much smaller uniaxial anisotropy compared to MnBi$_{2}$Te$_{4}$. We attribute the former to the shorter superexchange path and the latter to the smaller ligand-field splitting in (Ge$_{1-\delta-x}$Mn$_x$)$_2$Bi$_2$Te$_5$. Our study demonstrates that this series of materials holds promise for the investigation of the Layer Hall effect and quantum metric nonlinear Hall effect., Comment: 9 pages, 5 figures

Multiple recent studies have identified the metallic antiferromagnet Mn$_2$Au to be a candidate for spintronic applications due to apparent in-plane anisotropy, preserved magnetic properties above room temperature, and current-induced N\'eel vector switching. Crystal growth is complicated by the fact that Mn$_2$Au melts incongruently. We present a bismuth flux method to grow millimeter-scale bulk single crystals of Mn$_2$Au in order to examine the intrinsic anisotropic electrical and magnetic properties. Flux quenching experiments reveal that the Mn$_2$Au crystals precipitate below 550{\deg}C, about 100{\deg}C below the decomposition temperature of Mn$_2$Au. Bulk Mn$_2$Au crystals have a room-temperature resistivity of 16-19 $\mu\Omega$-cm and a residual resistivity ratio of 41. Mn$_2$Au crystals have a dimensionless susceptibility on the order of 10$^{-4}$, comparable to calculated and experimental reports on powder samples. Single-crystal neutron diffraction confirms the in-plane magnetic structure. The tetragonal symmetry of Mn$_2$Au constrains the $ab$-plane magnetic susceptibility to be constant, meaning that $\chi_{100}=\chi_{110}$ in the low-field limit, below any spin-flop transition. We find that three measured magnetic susceptibilities $\chi_{100}$, $\chi_{110}$, and $\chi_{001}$ are the same order of magnitude and agree with the calculated prediction, meaning the low-field susceptibility of Mn$_2$Au is quite isotropic, despite clear differences in $ab$-plane and $ac$-plane magnetocrystalline anisotropy. Mn$_2$Au is calculated to have an extremely high in-plane spin-flop field above 30 T, which is much larger than that of another in-plane antiferromagnet Fe$_2$As (less than 1 T). The subtle anisotropy of intrinsic susceptibilities may lead to dominating effects from shape, crystalline texture, strain, and defects in devices that attempt spin readout in Mn$_2$Au., Comment: 9 pages, 10 figures, 15 pages supplemental

A supersolid is a quantum entangled state of matter that combines features of both superfluids and solids. Despite predictions of its analog in quantum magnets, the experimental realization was lacking until recent claims in triangular-lattice compounds. Here, we report the magnetic phase diagram and neutron scattering for a spin-1/2 triangular-lattice antiferromagnet, K$_2$Co(SeO$_3$)$_2$. In zero field, neutron spectroscopy reveals the gradual development of a $\sqrt3 \times sqrt3$ magnetic order associated with $Z_3$ symmetry breaking for temperatures 5 K < T < 15 K. Below 5 K, the emergence of a Goldstone mode from low-energy continuum scattering suggests that the system enters a supersolid phase characterized by the breaking of both $Z_3$ and spin rotational U(1) symmetry. In c-axis-oriented magnetic fields 1.1 T < B < 21 T, a prominent 1/3 magnetization plateau phase emerges, accompanied by a distinct high-field supersolid phase (18 T < B < 21 T). From the coherent spin wave excitations in the 1/3 magnetized plateau phase, we infer the spin Hamiltonian, which features nearest neighbor interactions with $J_z$ = 2.98(2) meV and $J_{\rm perp}$ = 0.21(3) meV. Our work demonstrates that K$_2$Co(SeO$_3$)$_2$ is a spectacular example of a spin-1/2 triangular-lattice quantum Ising antiferromagnet, documents its magnetic phase diagram highlighting two supersolid phases, and provides spectroscopic evidence of zero-field supersolidity., Comment: 13 pages, 5 figures

The pursuit of discovering new high-temperature superconductors that diverge from the copper-based paradigm1-3 carries profound implications for elucidating mechanisms behind superconductivity and may also enable new applications4-8. Here, our investigation reveals that application of pressure effectively suppresses the spin and charge order in trilayer nickelate La4Ni3O10-{\delta} single crystals, leading to the emergence of superconductivity with a maximum critical temperature (Tc) of around 30 K at 69.0 GPa. The DC susceptibility measurements confirm a substantial diamagnetic response below Tc, indicating the presence of bulk superconductivity with a volume fraction exceeding 80%. In the normal state, we observe a "strange metal" behavior, characterized by a linear temperature-dependent resistance extending up to 300 K. Furthermore, the layer-dependent superconductivity observed hints at a unique interlayer coupling mechanism specific to nickelates, setting them apart from cuprates in this regard. Our findings provide crucial insights into the fundamental mechanisms underpinning superconductivity, while also introducing a new material platform to explore the intricate interplay between the spin/charge order, flat band structures, interlayer coupling, strange metal behavior and high-temperature superconductivity., Comment: Supplementary information included

A spin-1/2 triangular-lattice antiferromagnet is a prototypical frustrated quantum magnet, which exhibits remarkable quantum many-body effects that arise from the synergy between geometric spin frustration and quantum fluctuations. It can host quantum frustrated magnetic topological phenomena like quantum spin liquid (QSL) states, highlighted by the presence of fractionalized quasiparticles within a continuum of magnetic excitations. In this work, we use neutron scattering to study CoZnMo$_3$O$_8$, which has a triangular lattice of Jeff = 1/2 Co2+ ions with octahedral coordination. We found a wave-vector-dependent excitation continuum at low energy that disappears with increasing temperature. Although these excitations are reminiscent of a spin excitation continuum in a QSL state, their presence in CoZnMo$_3$O$_8$ originates from magnetic intersite disorder-induced dynamic spin states with peculiar excitations. Our results, therefore, give direct experimental evidence for the presence of a disorder-induced spin excitation continuum.

The kagome metals display an intriguing variety of electronic and magnetic phases arising from the connectivity of atoms on a kagome lattice. A growing number of these materials with vanadium kagome nets host charge density waves (CDWs) at low temperatures including ScV$_6$Sn$_6$, CsV$_3$Sb$_5$, and V$_3$Sb$_2$. Curiously, only the Sc version of the $R$V$_6$Sn$_6$ HfFe$_6$Ge$_6$-type materials hosts a CDW ($R = $Gd-Lu, Y, Sc). In this study we investigate the role of rare earth size in CDW formation in the $R$V$_6$Sn$_6$ compounds. Magnetization measurements on our single crystals of (Sc,Lu)V$_6$Sn$_6$ and (Sc,Y)V$_6$Sn$_6$ establish that the CDW is suppressed by substitution of Sc by larger Lu or Y. Single crystal x-ray diffraction reveals that compressible Sn-Sn bonds accommodate the larger rare earth atoms within loosely packed $R$-Sn-Sn chains without significantly expanding the lattice. We propose that Sc provides the extra room in these chains crucial to CDW formation in ScV$_6$Sn$_6$. Our rattling chain model explains why both physical pressure and substitution by larger rare earths hinder CDW formation despite opposite impacts on lattice size. We emphasize the cooperative effect of pressure and rare earth size by demonstrating that pressure further suppresses the CDW in a Lu-doped ScV$_6$Sn$_6$ crystal. Our model not only addresses why a CDW only forms in the $R$V$_6$Sn$_6$ materials with tiny Sc, it also advances to our understanding of why unusual CDWs form in the kagome metals., Comment: 28 pages, 9 figures, crystallographic information files for LuV6Sn6 and YV6Sn6 along with supplemental materials in ancillary files

We study the ground state and spin excitations in Ba3MnSb2O9, an easy-plane S = 5/2 triangular lattice antiferromagnet. By combining single-crystal neutron scattering, electric spin resonance (ESR), and spin wave calculations, we determine the frustrated quasi-two-dimensional spin Hamiltonian parameters describing the material. While the material has a slight monoclinic structural distortion, which could allow for isosceles-triangular exchanges and biaxial anisotropy by symmetry, we observe no deviation from the behavior expected for spin waves in the in-plane 120o state. Even the easy-plane anisotropy is so small that it can only be detected by ESR in our study. In conjunction with the quasi-two-dimensionality, our study establishes that Ba3MnSb2O9 is a nearly ideal triangular lattice antiferromagnet with the quasi-classical spin S = 5/2, which suggests that it has the potential for an experimental study of Z- or Z2-vortex excitations.

We present a new lite python-based program, CrysFieldExplorer, for fast optimizing crystal electric field (CEF) parameters to fit experimental data. The main novelty of CrysFieldExplorer is the development of a unique loss function, referred to as the Spectrum-Characteristic Loss ($L_{\text{Spectrum}}$), which is defined based on the characteristic polynomial of the Hamiltonian matrix. Particle Swarm Optimization and Covariance matrix adaptation evolution strategy are used to find the minimum of the total loss function. We demonstrate that CrysFieldExplorer can performs direct fitting of CEF parameters to any experimental data such as neutron spectrum, susceptibility, magnetizations etc. CrysFieldExplorer can handle a large amount of none-zero CEF parameters and reveal multiple local and global minimum solutions. Detailed crystal field theory, description of the loss function, implementation and limit of the program are discussed within context of two examples.

Mixed halide chemistry has recently been utilized to tune the intrinsic magnetic properties of transition-metal halides $-$ one of the largest families of magnetic van der Waals materials. Prior studies have shown that the strength of exchange interactions, hence the critical temperature, can be tuned smoothly with halide composition for a given ground-state. Here we show that the ground-state itself can be altered by a small change of halide composition leading to a quantum phase transition in FeCl$_{3-x}$Br$_x$. Specifically, we find a three-fold jump in the N\'{e}el temperature and a sign change in the Weiss temperature at $x= 0.08$ corresponding to only $3\%$ bromine doping. Using neutron scattering, we reveal a change of the ground-state from spiral order in FeCl$_3$ to A-type antiferromagnetic order in FeBr$_3$. Using first-principles calculations, we show that a delicate balance between nearest and next-nearest neighbor interactions is responsible for such a transition. These results support the proximity of FeCl$_3$ to a spiral spin liquid state, in which competing interactions and nearly degenerate magnetic $k$-vectors may cause large changes in response to small perturbations., Comment: 6 pages, 4 figures

Single crystals of a Shastry-Sutherland magnetic semiconductor, BaNd2ZnS5, were synthesized through a high-temperature solution growth technique. Physical properties were characterized by powder and single crystal x-ray diffraction, temperature- and field-dependent magnetization, and temperature-dependent specific heat measurements. BaNd2ZnS5 orders antiferromagnetically at 2.9 K, with magnetic moments primarily aligned within the ab-plane. Magnetic isothermal measurements show metamagnetic transitions at ~ 15 kOe for the [110] direction and ~ 21 kOe for the [100] direction. Estimated magnetic entropy suggests a double ground state for each Nd ion., Comment: 5 figures

A 2-Q antiferromagnetic order of the ferromagnetic dimers was found below TN = 2.9 K in the Shastry-Sutherland lattice BaNd2ZnS5 by single crystal neutron diffraction. The magnetic order can be understood by the orthogonal arrangement of local Ising Nd spins, identified by polarized neutrons. A field was applied along [1 -1 0] to probe the observed metamagnetic transition in the magnetization measurement. The field decouples two magnetic sublattices corresponding to the propagation vectors q1= (0.5, 0.5, 0) and q2= (-0.5, 0.5, 0), respectively. Each sublattice shows a stripe order with a Neel-type arrangement in each single layer. The stripe order with q1 remains nearly intact up to 6 T, while the other one with q2 is suppressed at a critical field Hc ~1.7 T, indicating a partial disorder. The Hc varies with temperature and is manifested in the H-T phase diagram constructed by measuring the magnetization in BaNd2ZnS5., Comment: 25 pages, 6 figures

AMn6Bi5 materials (A = Na, K, Rb and Cs) consisting of unique Mn-cluster chains emerge as a new family of superconductors with the suppression of their antiferromagnetic (AFM) order under high pressures. Here, we report transverse incommensurate spin density waves (SDWs) for the Mn atoms with a propagating direction along the chain axes as a ground state for KMn6Bi5 by single crystal neutron diffraction. The SDWs have a refined amplitude of ~2.46 Bohr magnetons for the Mn atoms in the pentagons and ~0.29 Bohr magnetons with a large standard deviation for Mn atoms in the center between the pentagons. AFM dominate both the nearest-neighbor Mn-Mn interactions within the pentagon and next-nearest-neighbor Mn-Mn interactions out of the pentagon (along the propagating wave). The SDWs exhibit both local and itinerant characteristics probably formed by a cooperative interaction between local magnetic exchange and conduction electrons. A significant magnetoelastic effect during the AFM transition, especially along the chain direction, has been demonstrated by temperature-dependent x-ray powder diffraction. Single crystal x-ray diffraction below the AFM transition revealed satellite peaks originating from charge density waves along the chain direction with a q-vector twice as large as the SDW one, pointing to a strong real space coupling between them. Our work not only manifests a fascinating interplay among spin, charge, lattice and one dimensionality to trigger intertwined orders in KMn6Bi5 but also provides important piece of information for the magnetic structure of the parent compound to understand the mechanism of superconductivity in this new family.

As the first intrinsic antiferromagnetic (AFM) topological insulator (TI), MnBi$_2$Te$_4$ has provided a material platform to realize various emergent phenomena arising from the interplay of magnetism and band topology. Here by investigating (Mn$_{1-x}$Pb$_x$)Bi$_2$Te$_4$ $(0\leq x \leq 0.82)$ single crystals via the x-ray, electrical transport, magnetometry and neutron measurements, chemical analysis, external pressure, and first-principles calculations, we reveal the magnetic dilution effect on the magnetism and band topology in MnBi$_2$Te$_4$. With increasing $x$, both lattice parameters $a$ and $c$ expand linearly by around 2\%. All samples undergo the paramagnetic to A-type antiferromagnetic transition with the N$\acute{e}$el temperature decreasing lineally from 24 K at $x=0$ to 2 K at $x=0.82$. Our neutron data refinement of the $x=0.37$ sample indicates that the ordered moment is 4.3(1)$\mu_B$/Mn at 4.85 K and the amount of the Mn$_{\rm{Bi}}$ antisites is negligible within the error bars. Isothermal magnetization data reveal a slight decrease of the interlayer plane-plane antiferromagnetic exchange interaction and a monotonic decrease of the magnetic anisotropy, due to diluting magnetic ions and enlarging the unit cell. For $x=0.37$, the application of external pressures enhances the interlayer antiferromagnetic coupling, boosting the N$\acute{e}$el temperature at a rate of 1.4 K/GPa and the saturation field at a rate of 1.8 T/GPa. Furthermore, our first-principles calculations reveal that the band inversion in the two end materials, MnBi$_2$Te$_4$ and PbBi$_2$Te$_4$, occurs at the $\Gamma$ and $Z$ point, respectively, while two gapless points appear at $x = $ 0.44 and $x = $ 0.66, suggesting possible topological phase transitions with doping., Comment: 10 pages, 7 figures

Materials hosting kagome lattices have drawn interest for the diverse magnetic and electronic states generated by geometric frustration. In the $A$V$_3$Sb$_5$ compounds ($A$ = K, Rb, Cs), stacked vanadium kagome layers give rise to unusual charge density waves (CDW) and superconductivity. Here we report single-crystal growth and characterization of ScV$_6$Sn$_6$, a hexagonal HfFe$_6$Ge$_6$-type compound that shares this structural motif. We identify a first-order phase transition at 92 K. Single crystal X-ray and neutron diffraction reveal a charge density wave modulation of the atomic lattice below this temperature. This is a distinctly different structural mode than that observed in the $A$V$_3$Sb$_5$ compounds, but both modes have been anticipated in kagome metals. The diverse HfFe$_6$Ge$_6$ family offers more opportunities to tune ScV$_6$Sn$_6$ and explore density wave order in kagome lattice materials., Comment: 5 pages, 3 figures. Email corresponding authors for .cif files

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

Eu-based compounds often exhibit unusual magnetism, which is critical for nontrivial topological properties seen in materials such as EuCd2As2. We investigate the structure and physical properties of EuZn2As2 through measurements of the electrical resistivity, Hall effect, magnetization, and neutron diffraction. Our data show that EuZn2As2 orders antiferromagnetically with an A-type spin configuration below TN = 19 K. Surprisingly, there is strong evidence for dominant ferromagnetic fluctuations above TN, as reflected by positive Curie-Weiss temperature and extremely large negative magnetoresistance (MR) between TN and Tfl {\guillemotright} 200 K. Furthermore, the angle dependence of the MRab indicates field-induced spin reorientation from the ab-plane to a direction approximately 45{\deg} from the ab plane. Compared to EuCd2As2, the doubled TN and Tfl make EuZn2As2 a better platform for exploring topological properties in both magnetic fluctuation (TN < T < Tfl) and ordered (T < TN) regimes., Comment: 17 pages, 4 figures

Understanding phonons in $\alpha$-RuCl$_3$ is critical to analyze the controversy around the observation of the half-integer thermal quantum Hall effect. While many studies have focused on the magnetic excitations in $\alpha$-RuCl$_3$, its vibrational excitation spectrum has remained relatively unexplored. We investigate the phonon structure of $\alpha$-RuCl$_3$ via inelastic neutron scattering experiments and density functional theory calculations. Our results show excellent agreement between experiment and first principles calculations. After validating our theoretical model, we extrapolate the low energy phonon properties. We find that the phonons in $\alpha$-RuCl$_3$ that either propagate or vibrate in the out-of-plane direction have significantly reduced velocities, and therefore have the potential to dominate the observability of the elusive half integer plateaus in the thermal Hall conductance. In addition, we use low-energy interlayer phonons to resolve the low temperature stacking structure of our large crystal of $\alpha$-RuCl$_3$, which we find to be consistent with that of the $R\bar{3}$ space group, in agreement with neutron diffraction., Comment: The first two authors contributed equally

Van der Waals magnet VI$_3$ demonstrates intriguing magnetic properties that render it great for use in various applications. However, its microscopic magnetic structure has not been determined yet. Here, we report neutron diffraction and susceptibility measurements in VI$_3$ that revealed a ferromagnetic order with the moment direction tilted from the $c$-axis by ~36{\deg} at 4 K. A spin reorientation accompanied by a structure distortion within the honeycomb plane is observed at a temperature of ~27 K, before the magnetic order completely disappears at $T_C$ = 50 K. The refined magnetic moment of ~1.3 $\mu_B$ at 4 K is considerably lower than the fully ordered spin moment of 2 $\mu_B$/ V$^{3+}$, suggesting the presence of a considerable orbital moment antiparallel to the spin moment and strong spin-orbit coupling in VI$_3$. This results in strong magnetoelastic interactions that make the magnetic properties of VI$_3$ easily tunable via strain and pressure., Comment: 8 pages, 4 figures

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., Comment: 26 pages, 6 figures, 3 tables

New surprises continue to be revealed about La$_2$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 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 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., Comment: 12 pages, 10 figures; accepted version

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. Although our initial measurements on FeSn indeed reveal well-defined spin waves extending well above 140 meV coexisting with a flat excitation at 170 meV, subsequent experiments on CoSn indicate that the flat mode actually arises mostly from hydrocarbon scattering of the CYTOP-M commonly used to glue the samples to aluminum holder. Therefore, our results established the evolution of spin excitations in FeSn and CoSn, and identified an anomalous flat mode that has been overlooked by the neutron scattering community for the past 20 years.

$A$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., Comment: 8 pages, 7 figures, accepted by Phys. Rev. B

A toroidal dipole moment appears independent of the electric and magnetic dipole moment in the multipole expansion of electrodynamics. It arises naturally from vortex-like arrangements of spins. Observing and controlling spontaneous long-range orders of toroidal moments are highly promising for spintronics but remain challenging. Here we demonstrate that a vortex-like spin configuration with a staggered arrangement of toroidal moments, a ferritoroidal state, is realized in a chiral triangular-lattice magnet BaCoSiO4. Upon applying a magnetic field, we observe multi-stair toroidal transitions correlating directly with metamagnetic transitions. We establish a first-principles microscopic Hamiltonian that explains both the formation of toroidal states and the metamagnetic toroidal transition as a combined effect of the magnetic frustration and the Dzyaloshinskii-Moriya interactions allowed by the crystallographic chirality in BaCoSiO4.

Quantum effects fundamentally engender exotic physical phenomena in macroscopic systems, which advance next-generation technological applications. Rotational tunneling that represents the quantum phenomenon of the librational motion of molecules is ubiquitous in hydrogen-contained materials. However, its direct manifestation in realizing macroscopic physical properties is elusive. Here we report an observation of reentrant ferroelectricity under low pressure that is mediated by the rotational tunneling of ammonium ions in molecule-based (NH$_4$)$_2$FeCl$_5 \cdot$H$_2$O. Applying a small pressure leads to a transition from spin-driven ferroelectricity to paraelectricity coinciding with the stabilization of a collinear magnetic phase. Such a transition is attributed to the hydrogen bond fluctuations via the rotational tunneling of ammonium groups as supported by theoretical calculations. Higher pressure lifts the quantum fluctuations and leads to a reentrant ferroelectric phase concomitant with another incommensurate magnetic phase. These results demonstrate that the rotational tunneling emerges as a new route to control magnetic-related properties in soft magnets, opening avenues for designing multi-functional materials and realizing potential quantum control., Comment: 4 figures. Supplemental Material available on request

Two-dimensional van der Waals MnBi$_{2n}$Te$_{3n+1}$ (n = 1, 2, 3, 4) compounds have been recently found to be intrinsic magnetic topological insulators rendering quantum anomalous Hall effect and diverse topological states. Here, we summarize and compare the crystal and magnetic structures of this family, and discuss the effects of chemical composition on their magnetism. We found that a considerable fraction of Bi occupies at the Mn sites in MnBi$_{2n}$Te$_{3n+1}$ (n = 1, 2, 3, 4) while Mn is no detectable at the non-magnetic atomic sites within the resolution of neutron diffraction experiments. The occupancy of Mn monotonically decreases with the increase of n. The polarized neutron diffraction on the representative MnBi$_{4}$Te$_{7}$ reveals that its magnetization density is exclusively accumulated at the Mn site, in good agreement with the results from the unpolarized neutron diffraction. The defects of Bi at the Mn site naturally explain the continuously reduced saturated magnetic moments from n = 1 to n = 4. The experimentally estimated critical exponents of all the compounds generally suggest a three-dimensional character of magnetism. Our work provides material-specified structural parameters that may be useful for band structure calculations to understand the observed topological surface states and for designing quantum magnetic materials through chemical doping., Comment: 5 figures, typos corrected

We use neutron scattering to investigate spin excitations in Sr(Co$_{1-x}$Ni$_{x})_2$As$_2$, which has a $c$-axis incommensurate helical structure of the two-dimensional (2D) in-plane ferromagnetic (FM) ordered layers for $0.013\leq x \leq 0.25$. By comparing the wave vector and energy dependent spin excitations in helical ordered Sr(Co$_{0.9}$Ni$_{0.1}$)$_2$As$_2$ and paramagnetic SrCo$_2$As$_2$, we find that Ni-doping, while increasing lattice disorder in Sr(Co$_{1-x}$Ni$_{x})_2$As$_2$, enhances quasi-2D FM spin fluctuations. However, our band structure calculations within the combined density functional theory and dynamic mean field theory (DFT+DMFT) failed to generate a correct incommensurate wave vector for the observed helical order from nested Fermi surfaces. Since transport measurements reveal increased in-plane and $c$-axis electrical resistivity with increasing Ni-doping and associated lattice disorder, we conclude that the helical magnetic order in Sr(Co$_{1-x}$Ni$_{x})_2$As$_2$ may arise from a quantum order-by-disorder mechanism through the itinerant electron mediated Ruderman-Kittel-Kasuya-Yosida (RKKY) interactions.

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$_9$H$_{18}$N$_2$CuBr$_4$. Single-crystal heat capacity and neutron diffraction measurements reveal that the N$\rm \acute{e}$el-ordered phase breaks down beyond a critical pressure of $P_{\rm c}$$\sim$1.0 GPa through a continuous quantum phase transition. Estimates of the critical exponents suggest that this transition may fall outside the traditional Landau paradigm. The inelastic neutron scattering spectra at 1.3 GPa are characterized by two well-separated gapped modes, including one continuum-like and another resolution-limited excitation in distinct scattering channels, which further indicates an exotic quantum-disordered phase above $P_{\rm c}$., Comment: The revised version includes 10 pages and 5 figures in the main text. To appear in Nature Communications. Any comments are welcome

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.

Magnetic topological semimetals have attracted intense attention recently since these materials carry a great promise for potential applications in novel spintronic devices. Here, we report an intimate interplay between lattice, Eu magnetic order and topological semimetallic behavior in Eu$_{1-x}$Sr$_{x}$MnSb$_{2}$ driven by nonmagnetic Sr doping on magnetic Eu site. Different types of Eu spin reorientations are controllable by the Sr concentration, temperature or magnetic field, and coupled to the quantum transport properties of Dirac fermions generated by the 2D Sb layers. Our study opens a new pathway to achieving exotic magnetic order and topological semimetallic state via controlling spin reorientation. The effective strategy of substituting rare-earth site by nonmagnetic element demonstrated here may be applicable to the AMnCh$_{2}$ (A=rare-earth elements; Ch=Bi/Sb) family and a wide variation of other layered compounds involving spatially separated rare-earth and transition metal layers., Comment: 25 pages, 4 figures, 2 tables, plus supplementary materials

The fine control of magnetism and electronic structure is crucial since the interplay between magnetism and band topology can lead to various novel magnetic topological states including axion insulators, magnetic Weyl semimetals and Chern insulators etc. Through crystal growth, transport, thermodynamic, neutron diffraction measurements, we show that with Sb-doping, the newly-discovered intrinsic antiferromagnetic topological insulator MnBi4Te7 evolves from antiferro-magnetic to ferromagnetic and then ferrimagnetic. We attribute this to the formation of Mn(Bi,Sb) antisites upon doping, which result in additional Mn sublattices that modify the delicate interlayer magnetic interactions and cause the dominant Mn sublattice to go from antiferromagnetic to ferro-magnetic. We further investigate the effect of antisites on the band topology using the first-principles calculations. Without considering antisites, the series evolves from antiferromagnetic topological insulator (x = 0) to ferromagnetic axion insulators. In the exaggerated case of 16.7% of periodic antisites, the band topology is modified and type-I magnetic Weyl semimetal phase can be realized at intermediate dopings. Therefore, this doping series provides a fruitful platform with continuously tunable magnetism and topology for investigating emergent phenomena, including quantum anomalous Hall effect, Fermi arc states, etc., Comment: Defect analysis and magnetotransport data are added. 6 figs and 2 tables in total

Iron diantimonide is a material with the highest known thermoelectric power. By combining scanning transmission electron microscope study with electronic transport neutron, X-ray scattering and first principle calculation we identify atomic defects that control colossal thermopower magnitude and nanoprecipitate clusters with Sb vacancy ordering which induce additional phonon scattering and substantially reduce thermal conductivity. Defects are found to cause rather weak but important monoclinic distortion of the unit cell Pnnm to Pm. The absence of Sb along [010] for high defect concentration forms conducting path due to Fe d orbital overlap. The connection between atomic defect anisotropy and colossal thermopower in FeSb2 paves the way for the understanding and tailoring of giant thermopower in related materials.

We report a comprehensive inelastic neutron scattering study of the hybrid molecule-based multiferroic compound (ND4)2FeCl5D2O in the zero-field incommensurate cycloidal phase and the high-field quasi-collinear 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 change of polarization direction, the underlying multiferroic mechanism was proposed to switch from the spin-current model induced via the inverse Dzyalloshinskii-Moriya interaction to the p-d hybridization model. We perform a detailed analysis of the inelastic neutron data of (ND4)2FeCl5D2O using linear spin-wave theory to quantify magnetic interaction strengths and investigate 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 an 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 (ND4)2FeCl5D2O are much more robust than the electric polarization in response to delicate reorganizations of the electronic degrees of freedom in an applied magnetic field., Comment: 18 pages, 4 main figures, 1 Table

The crystalline and magnetic structures of Ca$_2$Ru$_{1-x}$Fe$_x$O$_4$ (x=0.02, 0.05, 0.08 and 0.12) have been studied using neutron and X-ray diffraction. The Fe-doping reduces the Ru-O bond length in both apical and planar directions. The smaller Ru(Fe)O$_6$ octahedron leads to its reduced distortion. The $Pbca$ space group is maintained in all the Fe-dopings, so is the octahedral flattening. Warming has a similar effect on the lattice to that of the Fe-doping in releasing the distorted octahedra but precipitates an abrupt octahedral elongation near the N$\acute{e}$el temperature. Two competing antiferromagnetic orders, $A$- and $B$-centered phases have been observed. The Fe-doping-relaxed crystal structure prefers the latter to the former. As the doping increases, the $B$-centered phase continuously grows at the cost of the $A$-centered one and eventually replaces it at x=0.12. The absence of the two-dimensional antiferromagnetic critical fluctuations above the magnetic transition temperature and the three-dimensional magnetic correlation below the transition, together with the anomalous lattice response, point to an important role of orbital degree of freedom in driving the magnetic phase competition.

Triangular lattice of rare-earth ions with interacting effective spin-$1/2$ local moments is an ideal platform to explore the physics of quantum spin liquids (QSLs) in the presence of strong spin-orbit coupling, crystal electric fields, and geometrical frustration. The Yb delafossites, NaYbCh$_2$ (Ch=O, S, Se) with Yb ions forming a perfect triangular lattice, have been suggested to be candidates for QSLs. Previous thermodynamics, nuclear magnetic resonance, and muon spin rotation measurements on NaYbCh$_2$ have supported the suggestion of the QSL ground states. The key signature of a QSL, the spin excitation continuum, arising from the spin quantum number fractionalization, has not been observed. Here we perform both elastic and inelastic neutron scattering measurements as well as detailed thermodynamic measurements on high-quality single-crystalline NaYbSe$_2$ samples to confirm the absence of long-range magnetic order down to 40 mK, and further reveal a clear signature of magnetic excitation continuum extending from 0.1 to 2.5 meV. The comparison between the structure of the magnetic excitation spectra and the theoretical expectation from the spinon continuum suggests that the ground state of NaYbSe$_2$ is a QSL with a spinon Fermi surface., Comment: 18 pages, 6 figures

The Dzyaloshinskii-Moriya (DM) interaction is present in the transition metal dichalcogenides (TMDC) magnets of form $M_{1/3}T$S$_{2}$ ($M$ $=$ 3d transition metal, $T$ $\in$ {Nb, Ta}), given that the intercalants $M$ form $\sqrt{3}\times\sqrt{3}$ superlattices within the structure of the parent materials $T$S$_2$ and break the centrosymmetry. Competition between the DM and ferromagnetic exchange interactions in these systems has been shown to stabilize a topological defect known as a chiral soliton in select intercalated TMDCs, initiating interest both in terms of fundamental physics and the potential for technological applications. In the current article, we report on our study of the materials V$_{1/3}$TaS$_2$ and V$_{1/3}$NbS$_2$, using a combination of x-ray powder diffraction, magnetization and single crystal neutron diffraction. Historically identified as ferromagnets, our diffraction results instead reveal that vanadium spins in these compounds are arranged into an A-type antiferromagnetic configuration at low temperatures. Refined moments are 1.37(6)$\mu_{B}$ and 1.50(9)$\mu_{B}$ for V$_{1/3}$TaS$_2$ and V$_{1/3}$NbS$_2$, respectively. Transition temperatures $T_{c}$~$=$~32K for V$_{1/3}$TaS$_{2}$ and 50K for V$_{1/3}$NbS$_{2}$ are obtained from the magnetization and neutron diffraction results. We attribute the small net magnetization observed in the low-temperature phases to a subtle ($\sim$2$^{\circ}$) canting of XY-spins in the out-of-plane direction. These new results are indicative of dominant antiferromagnetic exchange interactions between the vanadium moments in adjacent ab-planes, likely eliminating the possibility of identifying stable chiral solitons in the current materials., Comment: 10 pages, 6 figures

By combining single crystal x-ray and neutron diffraction, and the magnetodielectric measurements on single crystal Fe4Nb2O9, we present the magnetic structure and the symmetry-allowed magnetoelectric coupling in Fe4Nb2O9. It undergoes an antiferromagnetic transition at TN=93 K, followed by a displacive transition at TS=70 K. The temperature-dependent dielectric constant of Fe4Nb2O9 is strongly anisotropic with the first anomaly at 93 K due to the exchange striction as a result of the long range spin order, and the second one at 70 K emanating from the structural phase transition primarily driven by the O atomic displacements. Magneticfield induced magnetoelectric coupling was observed in single crystal Fe4Nb2O9 and is compatible with the solved magnetic structure that is characteristic of antiferromagnetically arranged ferromagnetic chains in the honeycomb plane. We propose that such magnetic symmetry should be immune to external magnetic fields to some extent favored by the freedom of rotation of moments in the honeycomb plane, laying out a promising system to control the magnetoelectric properties by magnetic fields.

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.

Neutron scattering experiments have been performed to elucidate magnetic properties of the quasicrystal approximant Au$_{70}$Si$_{17}$Tb$_{13}$, consisting of icosahedral spin clusters in a body-centered-cubic lattice. Bulk magnetic measurements performed on the single crystalline sample unambiguously confirm long-range ordering at $T_{\rm C} = 11.6 \pm 1$ K. In contrast to the simple ferromagnetic response in the bulk measurements, single crystal neutron diffraction confirms a formation of intriguing non-collinear and non-coplanar magnetic order. The magnetic moment direction was found to be nearly tangential to the icosahedral cluster surface in the local mirror plane, which is quite similar to that recently found in the antiferromagnetic quasicrystal approximant Au$_{72}$Al$_{14}$Tb$_{14}$. Inelastic neutron scattering on the powdered sample exhibits a very broad peak centered at $\hbar \omega \simeq 4$ meV. The observed inelastic spectrum was explained by the crystalline-electric-field model taking account of the chemical disorder at the fractional Au/Si sites. The resulting averaged anisotropy axis for the crystalline-electric-field ground state is consistent with the ordered moment direction determined in the magnetic structure analysis, confirming that the non-coplanar magnetic order is stabilized by the local uniaxial anisotropy., Comment: 14 pages, 10 figures, 3 tables

The interplay between topology and magnetism is essential for realizing novel topological states including the axion insulator, the magnetic Weyl semimetal, etc. An intrinsically ferromagnetic topological material with only the topological bands at the charge neutrality energy has so far remained elusive. By rationally designing the natural heterostructure consisting of [MnBi2Te4] septuple layers and [Bi2Te3] quintuple layers, we report MnBi8Te13 as the first intrinsic ferromagnetic topological material with clean low-energy band structure. Based on the thermodynamic, transport and neutron diffraction measurements, our data show that despite the adjacent [MnBi2Te4] being 44.1 {\AA} apart, MnBi8Te13 manifests long-range ferromagnetism below 10.5 K with strong coupling between magnetism and charge carriers. Our first-principles calculations and angle-resolved photoemission spectroscopy measurements further demonstrate that MnBi8Te13 is an intrinsic ferromagnetic axion state. Therefore, MnBi8Te13 serves as an ideal system to investigate rich emergent phenomena, including the quantized anomalous Hall effect and quantized topological magnetoelectric effect., Comment: 6 figs

Using single crystal neutron diffraction, we present a systematic investigation of the crystal structure and magnetism of van der Waals topological insulators MnBi$_2$Te$_4$ and MnBi$_4$Te$_7$, where rich topological quantum states have been recently predicted and observed. Structural refinements reveal that considerable Bi atoms occupied on the Mn sites in both materials, distinct from the previously reported antisite disorder. We show unambiguously that MnBi$_{2}$Te$_{4}$ orders antiferromagnetically below 24 K featured by a magnetic symmetry $R_I$-${3c}$ while MnBi$_{4}$Te$_{7}$ is antiferromagnetic below 13 K with a magnetic space group $P_c$-${3c1}$. They both present antiferromagnetically coupled ferromagnetic layers with spins along the $c$-axis. We put forward a stacking rule for the crystal structure of an infinitely adaptive series MnBi$_{2n}$Te$_{3n+1}$ (n$\geq$1) with the building unit of [Bi$_2$Te$_3$]. A comparison of magnetic properties between MnBi$_{2}$Te$_{4}$ and MnBi$_{4}$Te$_{7}$, together with the recent density-functional theory calculations, enables us to draw that a two-dimensional magnetism limit might be realized in the derivatives. Our work may promote the theoretical studies of topological magnetic states in the series of MnBi$_{2n}$Te$_{3n+1}$., Comment: typos corrected in table I

Here we report a new quasi-one-dimensional $S$ = 1 chain compound NiTe$_{2}$O$_{5}$. From the comprehensive study of the structure and magnetic properties on high quality single crystalline NiTe$_{2}$O$_{5}$, it's revealed that NiTe$_{2}$O$_{5}$ undergoes a transition into an intriguing long-range antiferromagnetic order at $T_{\rm N}=30.5 {\rm K}$, in which longitudinal magnetic moments along the chain direction are ferromagnetically ordered, while their transverse components have an alternating ferromagnetic-antiferromagnetic coupling. Even though the temperature dependence of magnetic susceptibility represents an archetypal anisotropic antiferromagnetic order, we found that critical behavior of unconventional nature with $\alpha'\sim0.25$ and $\beta\sim0.18$ is accompanied by the temperature evolution of the antiferromagnetic order parameter.

We report neutron diffraction studies of FeS single crystals obtained from Rb$_x$Fe$_{2-y}$S$_2$ single crystals via a hydrothermal method. While no $\sqrt {5}\times \sqrt {5}$ iron vacancy order or block antiferromagnetic order typical of Rb$_x$Fe$_{2-y}$S$_2$ is found in our samples, we observe $C$-type short range antiferromagnetic order with moments pointed along the $c$-axis hosted by a new phase of FeS with an expanded inter-layer spacing. The N\'{e}el temperature for this magnetic order is determined to be 165 K. Our finding of a variant FeS structure hosting this $C$-type antiferromagnetic order demonstrates that the known FeS phase synthesized in this method is in the vicinity of a magnetically ordered ground state, providing insights into understanding a variety of phenomena observed in FeS and the related FeSe$_{1-x}$S$_x$ iron chalcogenide system., Comment: 7 pages, 6 figures