SrV0.3Fe0.7O2.8: A Vacancy-Ordered Fe-Based Perovskite Exhibiting Room-Temperature Magnetoresistance.

We report room-temperature (RT) magnetoresistance (MR) in a novel Fe-based perovskite, SrV0.3Fe0.7O2.8. This compound contains ordered oxygen vacancies in every fifth primitive perovskite (111)p plane, leading to a layered structure consisting of triple-octahedral and double-tetrahedral layers. Along with the oxygen vacancies, the transition-metal ions are also ordered: the octahedral sites are occupied by 100% of Fe ions, while the tetrahedral sites are occupied by 25% of Fe ions and 75% of V ions. As a result, SrV0.3Fe0.7O2.8 forms a magnetically striped lattice in which the octahedral layers with 100% of magnetic Fe ions are separated by the diluted magnetic layer. The compound exhibits weak ferromagnetism and shows a large negative MR (-5% at 3 T) at RT, despite the small saturation moment (0.4 µB/Fe atom). Thus, this type of layered compound is promising for further large MR by an increase of magnetization through chemical substitution.

Synthesis of Hydride-Doped Perovskite Stannate with Visible Light Absorption Capability.

Narrow-gap semiconductors with visible light absorption capability have attracted attention as photofunctional materials. H--doped BaSn0.7Y0.3O3-δ containing Sn(II) species was recently reported to absorb visible light up to 600 nm, which represents the first demonstration of oxyhydride-based visible-light-absorbers. In the present study, a more detailed investigation was made to obtain information on the synthesis and properties of H--doped perovskite-type stannate with respect to the A-site cation of the material and the preparation conditions. H--doped ASn0.7Y0.3O3-δ (A = Ba, Ba0.5Sr0.5, and Sr) obtained by the reaction of ASn0.7Y0.3O3-δ precursors with CaH2 at 773 K under vacuum conditions was shown to have almost the same bandgap (ca. 2.1 eV), regardless of the A-site cation. Physicochemical measurements and theoretical calculations revealed that the identical bandgaps of H--doped ASn0.7Y0.3O3-δ are due to the simultaneous shift of the midgap states composed of Sn2+ with the conduction band minimum. Experimental results also indicated that the appropriate preparation conditions with respect to Y3+-substitution and the temperature for the synthesis of the ASn0.7Y0.3O3-δ precursors were essential to obtain H--doped products that have a low density of defects.

Enhanced Magnetic Interaction by Face-Shared Hydride Anions in 6H-BaCrO2H.

Studies on magnetic oxyhydrides have been almost limited to perovskite-based lattices with corner-sharing octahedra with a M-H-M (M: transition metal) angle of θ ∼ 180°. Using a high-pressure method, we prepared BaCrO2H with a 6H-type hexagonal perovskite structure with corner- and face-sharing octahedra, offering a unique opportunity to investigate magnetic interactions based on a θ ∼ 90° case. Neutron diffraction for BaCrO2H revealed an antiferromagnetic (AFM) order at TN ∼ 375 K, which is higher than ∼240 K in BaCrO3-xFx. The relatively high TN of BaCrO2H can be explained by the preferred occupancy of H- at the face-sharing site that provides AFM superexchange in addition to AFM direct exchange interactions. First-principles calculations on BaCrO2H in comparison with BaCrO2F and BaMnO3 further reveal that the direct Cr-Cr interaction is significantly enhanced by shortening the Cr-Cr distance due to the covalent nature of H-. This study provides a useful strategy for the extensive control of magnetic interactions by exploiting the difference in the covalency of multiple anions.

Triplon current generation in solids.

A triplon refers to a fictitious particle that carries angular momentum S=1 corresponding to the elementary excitation in a broad class of quantum dimerized spin systems. Such systems without magnetic order have long been studied as a testing ground for quantum properties of spins. Although triplons have been found to play a central role in thermal and magnetic properties in dimerized magnets with singlet correlation, a spin angular momentum flow carried by triplons, a triplon current, has not been detected yet. Here we report spin Seebeck effects induced by a triplon current: triplon spin Seebeck effect, using a spin-Peierls system CuGeO3. The result shows that the heating-driven triplon transport induces spin current whose sign is positive, opposite to the spin-wave cases in magnets. The triplon spin Seebeck effect persists far below the spin-Peierls transition temperature, being consistent with a theoretical calculation for triplon spin Seebeck effects.

Impact of the Lattice on Magnetic Properties and Possible Spin Nematicity in the S=1 Triangular Antiferromagnet NiGa_{2}S_{4}.

NiGa_{2}S_{4} is a triangular lattice S=1 system with strong two dimensionality of the lattice, actively discussed as a candidate to host spin-nematic order brought about by strong quadrupole coupling. Using Raman scattering spectroscopy we identify a phonon of E_{g} symmetry which can modulate magnetic exchange J_{1} and produce quadrupole coupling. Additionally, our Raman scattering results demonstrate a loss of local inversion symmetry on cooling, which we associate with sulfur vacancies. This will lead to disordered Dzyaloshinskii-Moriya interactions, which can prevent long-range magnetic order. Using magnetic Raman scattering response we identify 160 K as a temperature of an upturn of magnetic correlations. The temperature range below 160 K, but above 50 K where antiferromagnetic correlations start to increase, is a candidate for spin-nematic regime.

Realization of interlayer ferromagnetic interaction in MnSb2Te4 toward the magnetic Weyl semimetal state.

Magnetic properties of MnSb2Te4 were examined through magnetic susceptibility, specific-heat, and neutron-diffraction measurements. As opposed to isostructural MnBi2Te4 with the antiferromagnetic ground state, MnSb2Te4 develops a spontaneous magnetization below 25 K. From our first-principles calculations on the material in a ferromagnetic state, the state could be interpreted as a type-II Weyl semimetal state with broken time-reversal symmetry. Detailed structural refinements using x-ray-diffraction and neutron-diffraction data reveal the presence of site mixing between Mn and Sb sites, leading to the ferrimagnetic ground state. With theoretical calculations, we found that the presence of site mixing plays an important role for the interlayer Mn-Mn ferromagnetic interactions.

Spin Fluctuations from Hertz to Terahertz on a Triangular Lattice.

The temporal magnetic correlations of the triangular-lattice antiferromagnet NiGa_{2}S_{4} are examined through 13 decades (10^{-13}-1 sec) using ultrahigh-resolution inelastic neutron scattering, muon spin relaxation, and ac and nonlinear susceptibility measurements. Unlike the short-ranged spatial correlations, the temperature dependence of the temporal correlations show distinct anomalies. The spin fluctuation rate decreases precipitously upon cooling towards T^{*}=8.5 K, but fluctuations on the microsecond time scale then persist in an anomalous dynamical regime for 4 K

Pressure-induced superconductivity in the iron-based ladder material BaFe2S3.

All the iron-based superconductors identified so far share a square lattice composed of Fe atoms as a common feature, despite having different crystal structures. In copper-based materials, the superconducting phase emerges not only in square-lattice structures but also in ladder structures. Yet iron-based superconductors without a square-lattice motif have not been found, despite being actively sought out. Here, we report the discovery of pressure-induced superconductivity in the iron-based spin-ladder material BaFe2S3, a Mott insulator with striped-type magnetic ordering below ∼120 K. On the application of pressure this compound exhibits a metal-insulator transition at about 11 GPa, followed by the appearance of superconductivity below Tc = 14 K, right after the onset of the metallic phase. Our findings indicate that iron-based ladder compounds represent promising material platforms, in particular for studying the fundamentals of iron-based superconductivity.

Two-dimensional magnetism and spin-size effect in the S = 1 triangular antiferromagnet NiGa(2)S(4).

The triangular antiferromagnet is one of the most fundamental systems of geometrically frustrated magnets. NiGa(2)S(4) is a layered chalcogenide compound with an equilateral triangular lattice, and it is a prime candidate for an S = 1 triangular antiferromagnet. Here we focus on low temperature magnetism in NiGa(2)S(4), where quasi-static spins develop a spin-wave-like mode without forming any long-range ordering. We have studied low temperature magnetism of both polycrystalline samples and single crystals of Ni(1 - x)A(x)Ga(2)S(4) (A = Mn, Fe, Co, and Zn). A scaling law with a single energy scale of the Weiss temperature is found as an impurity effect and a hydrostatic pressure effect, providing evidence that it is in-plane interactions in the two-dimensional NiS(2) plane that drive the critical slowing down to the viscous spin liquid state at T(*) = 8.5 K and the spin-wave-like excitations of NiGa(2)S(4) that emerge below T ∼ 3 K. Furthermore, we find spin-size dependent impurity effects in the temperature dependence of the specific heat of Ni(1 - x)A(x)Ga(2)S(4). Even with a high impurity content, Zn(2+) (S = 0) and Fe(2+) (S = 2) substituted systems with weak XY anisotropy and integral spins retain the quadratic temperature dependence of the magnetic specific heat like pure NiGa(2)S(4). A spin glass-like phase, on the other hand, emerges at low temperatures with the substitution of magnetic impurities with half-odd integer spins: Ising Co(2+) (S = (3/2)) and weak XY Mn(2+) S = (5/2)) spins. This indicates that an integer size of spins is important for stabilizing the two-dimensional spin-wave-like behavior, and the unconventional spin state of NiGa(2)S(4) at low temperatures is distinct from a canonical spin glass.

Incommensurate magnetism in FeAs strips: neutron scattering from CaFe(4)As(3).

Magnetism in the orthorhombic metal CaFe(4)As(3) was examined through neutron diffraction for powder and single crystalline samples. Incommensurate [q(m) ≈ (0.37-0.39) × b*] and predominantly longitudinally (|| b) modulated order develops through a 2nd order phase transition at TN = 89.63(6) K with a 3D Heisenberg-like critical exponent ß = 0.365(6). A 1st order transition at T2 = 25.6(9) K is associated with the development of a transverse component, locking q(m) to 0.375(2)b*, and increasing the moments from 2.1(1) to 2.2(3) µ B for Fe2+ and from 1.3(3) to 2.4(4) µB for Fe+. The ab initio Fermi surface is consistent with a nesting instability in cross-linked FeAs strips.

Separation between low-energy hole dynamics and spin dynamics in a frustrated magnet.

An angle-resolved photoemission spectroscopy (ARPES) study is reported on a Mott insulator NiGa2S4 in which Ni2+ (S=1) ions form a triangular lattice and the Ni spins do not order even in its ground state. The first ARPES study on the two-dimensional spin-disordered system shows that low-energy hole dynamics at high temperatures is characterized by wave vectors Q(E) which are different from wave vectors Q(M) dominating low-energy spin excitations at low temperatures. The unexpected difference between Q(E) and Q(M) is deeply related to charge fluctuation across the Mott gap in the frustrated lattice and is a key issue to understand the spin-disordered ground states in Mott insulators.

Spin dependent impurity effects on the 2D frustrated magnetism of NiGa2S4.

Impurity effects on the triangular antiferromagnets Ni1-xMxGa2S4 (M=Mn, Fe, Co and Zn) are studied. The 2D frozen spin-disordered state of NiGa2S4 is stable against the substitution of Zn2+ (S=0) and Heisenberg Fe2+ (S=2) spins, and exhibits a T2-dependent magnetic specific heat, scaled by the Weiss temperature. In contrast, the substitutions with Co2+ (S=3/2) spin with Ising-like anisotropy and Heisenberg Mn2+ (S=5/2) spin induce a conventional spin glass phase below 1 K. From these comparisons, it is suggested that the integer size of the Heisenberg spins is important to stabilize the 2D coherent behavior observed in the frozen spin-disordered state.

Spin disorder on a triangular lattice.

As liquids crystallize into solids on cooling, spins in magnets generally form periodic order. However, three decades ago, it was theoretically proposed that spins on a triangular lattice form a liquidlike disordered state at low temperatures. Whether or not a spin liquid is stabilized by geometrical frustration has remained an active point of inquiry ever since. Our thermodynamic and neutron measurements on NiGa2S4, a rare example of a two-dimensional triangular lattice antiferromagnet, demonstrate that geometrical frustration stabilizes a low-temperature spin-disordered state with coherence beyond the two-spin correlation length. Spin liquid formation may be an origin of such behavior.