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We describe the existence of local distortion discovered in the synchrotron x-ray single-crystal structure analysis of layered ditelluride 1T-MTe2 (M = V, Nb, Ta). In 1T-TaTe2, the double zigzag chain structure of Ta is deformed at about 170 K, and heptamer molecules are formed periodically at low temperatures. We found that some of the Ta atoms that compose the double zigzag chain structure appearing at high temperatures are locally displaced, resulting in local dimerization. This tendency weakens when Ta is replaced by V or Nb. Our results indicate that the local distortion persistently survives in these ditellurides, where the electronic degrees of freedom, including orbitals, are weakened. We further discuss the origin of local distortion in these ditellurides, which is different from many usual material systems where molecular formation occurs at low temperatures., 11 pages, 4 figures, 18 tables, To be published in Phys. Rev. B

A new layered perovskite-type oxide Ba$_2$RhO$_4$ was synthesized by a high-pressure technique with the support of convex-hull calculations. The crystal and electronic structure were studied by both experimental and computational tools. Structural refinements for powder x-ray diffraction data showed that Ba$_2$RhO$_4$ crystallizes in a K$_2$NiF$_4$-type structure, isostructural to Sr$_2$RuO$_4$ and Ba$_2$IrO$_4$. Magnetic, resistivity, and specific heat measurements for polycrystalline samples of Ba$_2$RhO$_4$ indicate that the system can be characterized as a correlated metal. Despite the close similarity to its Sr$_2$RuO$_4$ counterpart in the electronic specific heat coefficient and the Wilson ratio, Ba$_2$RhO$_4$ shows no signature of superconductivity down to 0.16 K. Whereas the Fermi surface topology has reminiscent pieces of Sr$_2$RuO$_4$, an electron-like e$_g$-($d_{x^2-y^2}$) band descends below the Fermi level, making of this compound unique also as a metallic counterpart of the spin-orbit-coupled Mott insulator Ba$_2$IrO$_4$., Comment: 8 pages, 6 figures

We have experimentally studied a magnetopiezoelectric effect predicted recently for magnetic metals with low crystal symmetries. In EuMnBi2 with antiferromagnetic Mn moments at 77 K, dynamic displacements emerge along the $a$ direction upon application of ac electric fields in the $c$ direction, and increase in proportion to the applied electric fields. Such displacements are not observed along the $c$ direction of EuMnBi2 or EuZnBi2 with nonmagnetic Zn ions. As temperature increases from 77 K, the displacement signals decrease and disappear at about 200 K, above which electric conduction changes from coherent to incoherent. These results demonstrate the emergence of the magnetopiezoelectric effect in a magnetic metal lacking inversion and time-reversal symmetries.

Helimagnetic materials are identified as promising for novel spintronic applications. Since helical spin order is manifested as a compromise of competing magnetic exchange interactions, its emergence is limited by unique constraints imposed by the crystalline lattice and the interaction geometries, as exemplified by the multiferroic perovskite manganites with large orthorhombic distortion. Here we show that a simple cubic perovskite SrCoO$_3$ with room-temperature ferromagnetism has the potential to host helimagnetic order upon isotropic lattice expansion. Increasing the Ba content $x$ in Sr$_{1-x}$Ba$_x$CoO$_3$ continuously expands the cubic lattice, eventually suppressing the ferromagnetic order near $x$=0.4, where helimagnetic correlations are observed as incommensurate diffuse magnetic scattering by neutron diffraction measurements. The emergence of helimagnetism is semi-quantitatively reproduced by first-principles calculations, leading to the conjecture that a simple cubic lattice with strong $d$-$p$ hybridisation can exhibit a variety of novel magnetic phases originating from competing exchange interactions., Comment: 14 pages, 4 figures, To appear in Phys. Rev. Materials

The skyrmion crystal (SkX) characterized by a multiple-q helical spin modulation has been reported as a unique topological state that competes with the single-q helimagnetic order in non-centrosymmetric materials. Here we report the discovery of a rich variety of multiple-q helimagnetic spin structures in the centrosymmetric cubic perovskite SrFeO3. On the basis of neutron diffraction measurements, we have identified two types of robust multiple-q topological spin structures that appear in the absence of external magnetic fields: an anisotropic double-q spin spiral and an isotropic quadruple-q spiral hosting a three-dimensional lattice of hedgehog singularities. The present system not only diversifies the family of SkX host materials, but furthermore provides an experimental missing link between centrosymmetric lattices and topological helimagnetic order. It also offers perspectives for integration of SkXs into oxide electronic devices.

The GdFeO$_{3}$-type perovskite CaCoO$_{3}$ has been successfully synthesized by high-pressure oxygen annealing for the oxygen deficient perovskite. A detailed structural analysis based on synchrotron X-ray diffraction data and a thermogravimetric analysis show that the valence of Co is +4 and the sample is free from oxygen deficiency. This compound shows an antiferromagnetic ordering at 95 K, which has presumably helical spin arrangement, with keeping the incoherent metallic state down to the lowest temperature. This work demonstrates that the Co$^{4+}$-perovskite oxides exhibit a variety of magnetic phases by the band-width control through the lattice distortion., Comment: 5 pages, 5 figures

We investigate a large variation in a diagonal component of the linear magnetoelectric (ME) susceptibility in a polar ferrimagnet Mn2Mo3O8 while changing the magnetic-ion site from orbital-quenched Mn2+ to Fe2+ with strong uniaxial anisotropy. In Mn2Mo3O8, the linear ME susceptibility is dominated by the non-relativistic exchange striction mechanism, showing a positive value at low temperature and a critical behavior toward negative divergence around the transition temperature. This negative peak value becomes four times larger when 50% of Mn2+ ions are replaced with Fe2+ ion, highlighting the beneficial perspective of the compositionally-tunable ME effect. As the doped Fe increases in fraction, gradual negative shift of the ME coefficient is observed around the lowest temperature, which manifests relativistic single-site origin of the ME susceptibility. Further doping with x >= 75% in (Mn1-xFex)2Mo3O8, the ME coefficient becomes negative in the entire temperature region. Such a composition dependence can be explained in terms of the chemical preference for the two types of magnetic sites of Mn/Fe ions. The present study demonstrates the large tunability of ME effect by substituting the magnetic ion with the primary structural/magnetic characters kept intact., 23 pages, 10 figures

Magnetic excitations are investigated for a hexagonal polar magnet Fe2Mo3O8 by terahertz spectroscopy. We observed magnon modes including an electric-field active magnon, electromagnon, in the collinear antiferromagnetic phase with spins parallel to the c axis. We unravel the nature of these excitations by investigating the correlation between the evolution of the mode profile and the magnetic transition from antiferromagnetic to ferrimagnetic order induced by magnetic field or Zn-doping. We propose that the observed electromagnon mode involves the collective precession of the spins with oscillating in-plane electric polarization through the mechanism of the linear magnetoelectric effect., Comment: 16 pages, 4 figures

Using resonant soft x-ray scattering as a function of both temperature and magnetic field, we reveal a large number of almost degenerate magnetic orders in SrCo6O11. The Ising-like spins in this frustrated material in fact exhibit a so-called magnetic devil's staircase. It is demonstrated how a magnetic field induces transitions between different microscopic spin configurations, which is responsible for the magnetoresistance of SrCo6O11. This material therefore constitutes a unique combination of a magnetic devil's staircase and spin valve effects, yielding a novel type of magnetoresistance system., Comment: 5 pages, 5 figures

The change in the electronic structure of layered Cu$_{x}$IrTe$_{2}$ has been characterized by transport and spectroscopic measurements, combined with first-principles calculations. The Cu-intercalation suppresses the monoclinic distortion, giving rise to the stabilization of the trigonal phase with superconductivity. Thermopower and Hall resistivity measurements suggest the multiband nature with hole and electron carriers for this system, which is masked by the predominance of the hole carriers enhanced by the interlayer hybridization in the trigonal phase. Rather than the instability of Ir $d$ band, a subtle balance between the interlayer and intralayer Te-Te hybridizations is proposed as a main factor dominating the structural transition and the superconductivity., 5 pages, 4 figures

Dielectric properties were investigated under various magnitudes and directions of magnetic field (H) for a chiral magnetic insulator Cu2OSeO3. We found that the skyrmion crystal induces electric polarization (P) along either in-plane or out-of-plane direction of the spin vortices depending on the applied H-direction. The observed H-dependence of P in ferrimagnetic, helimagnetic, and skyrmion crystal state can be consistently described by the d-p hybridization model, highlighting an important role of relativistic spin-orbit interaction in the magnetoelectric coupling in Cu2OSeO3. Our analysis suggests that each skyrmion particle can locally carry electric dipole or quadrupole, which implies that the dynamics of skyrmions are controllable by the external electric field., 5 pages, 4 figures

The skyrmion is a topologically stable spin texture, in which the spin direction wraps a sphere. The topological nature gives rise to emergent electromagnetic phenomena such as topological Hall effect. Recently, the crystallization of nanoscale skyrmions was observed in chiral helimagnets with use of the neutron diffraction and Lorentz transmission electron microscopy. The skyrmions are quite mobile under electric current density as low as $\sim$ 10$^6$ A/m$^2$, and, in some cases, stable up to near room temperature. These features suggest that the skyrmions may work as a magnetic stable-variable similar to the bubble memory but equipped with topological functionalities. Here, we investigate the low-energy excitations of the skyrmion crystal in a helimagnetic insulator Cu$_2$OSeO$_3$ in terms of microwave response. We have observed two distinct excitations of the skyrmion with different polarization characteristics; the counter-clockwise circulating mode at 1 GHz and the breathing mode at 1.5 GHz. These modes may play a crucial role in the low energy dynamics of skyrmions and hence in their manipulation via external stimuli., 13 pages, 5 figures

Small angle neutron scattering experiments were performed on a bulk single crystal of chiral-lattice multiferroic insulator Cu$_2$OSeO$_3$. In the absence of an external magnetic field, helical spin order with magnetic modulation vector $q \parallel $ was identified. When a magnetic field is applied, a triple-$q$ magnetic structure emerges normal to the field in the A-phase just below the magnetic ordering temperature $T_c$, which suggests the formation of a triangular lattice of skyrmions. Notably, the favorable $q$-direction in the A-phase changes from $q \parallel $ to $q \parallel $ upon approaching $T_c$. Near the phase boundary between these two states, the external magnetic field induces a 30$^\circ$-rotation of the skyrmion lattice. This suggests a delicate balance between the magnetic anisotropy and the spin texture near $T_c$, such that even a small perturbation significantly affects the ordering pattern of the skyrmions., 5 pages, 4 figures, published as a Rapid Communication in Phys. Rev. B

Magnetically-driven ferroelectric atomic displacements of the order of 10$^{-3} Angstrom have been observed in orthorhombic (perovskite like) YMnO$_3$ by a single-crystal synchrotron x-ray diffraction. The refined polar structure shows the characteristic bond alternation driven by the exchange striction in staggered Mn-O-Mn arrays with $\uparrow\uparrow\downarrow\downarrow$ type ordering, giving rise to a spontaneous polarization along a-axis. First-principles calculations based on the Berry phase method as well as on the experimentally refined crystal structure can reproduce the observed polarization value., 8 pages, 5 figures, 2 tables

Effects of temperature (6--225 K) and magnetic field (0--7 T) on the low-energy (1.2--5 meV) electrodynamics of the electromagnon, the magnetic resonance driven by the light electric field, have been investigated for a hexaferrite magnet Ba$_2$Mg$_2$Fe$_{12}$O$_{22}$ by using terahertz time-domain spectroscopy. We find the gigantic terahertz magnetochromism via electromagnons; the magnetochromic change, as defined by the difference of the absorption intensity with and without magnetic field, exceeds 500% even at 0.6 T. The results arise from the fact that the spectral intensity of the electromagnon critically depends on the magnetic structure. With changing the conical spin structures in terms of the conical angle $\theta$ from the proper screw ($\theta=0^\circ$) to the ferrimagnetic ($\theta=90^\circ$) through the conical spin-ordered phases ($0^\circ, Comment: 19 pages including 7 figures; Accepted for publication in Phys. Rev. B

Magnetoelectric properties were investigated for an S=1/2 chain antiferromagnet CuCl2, which turns out to be the first example of non-chalcogen based spiral-spin induced multiferroics. Upon the onset of helimagnetic order propagating along the b-axis under zero magnetic field (H), we found emergence of ferroelectric polarization along the c-axis. Application of H along the b-axis leads to spin-flop transition coupled with drastic suppression of ferroelectricity, and rotation of H around the b-axis induces the rotation of spin-spiral plane and associated polarization direction. These behaviors are explained well within the framework of the inverse Dzyaloshinskii-Moriya model, suggesting the robustness of this magnetoelectric coupling mechanism even under the strong quantum fluctuation., 5 pages, 5 figures

A two-staged, uniaxial magnetoresistive effect has been discovered in SrCo6O11 having a layered hexagonal structure. Conduction electrons and localized Ising spins are in different sublattices but their interpenetration makes the conduction electrons sensitively pick up the stepwise field-dependence of magnetization. The stepwise field-dependence suggests two competitive interlayer interactions between ferromagnetic Ising-spin layers, i.e., a ferromagnetic nearest-layer interaction and an antiferromagnetic next-nearest-layer interaction. This oxide offers a unique opportunity to study nontrivial interplay between conduction electrons and Ising spins, the coupling of which can be finely controlled by a magnetic field of a few Tesla., 14 pages, 4 figures, accepted for publication in Phys. Rev. Lett

The crystal structures of the NaxCoO2 phases based on three-layer NaCoO2, with x=0.32, x=0.51, x=0.60, x=0.75 and x=0.92, determined by powder neutron diffraction, are reported. The structures have triangular CoO2 layers interleaved by sodium ions, and evolve with variation in Na content in a more complex way than has been observed in the two-layer NaxCoO2 system. The highest and lowest Na containing phases studied (x=0.92 and x=0.32) are trigonal, with three CoO2 layers per cell and octahedral Na ion coordination. The intermediate compositions have monoclinic structures. The x=0.75 compound has one CoO2 layer per cell, with Na in octahedral coordination and an incommensurate superlattice. The x=0.6 and x=0.5 phases are also single-layer, but the Na is found in trigonal prismatic coordination. The magnetic behavior of the phases is similar to that observed in the two-layer system. Both the susceptibility and the electronic contribution to the specific heat are largest for x=0.6., Comment: 24 pages, 14 figures, submitted to Phys.Rev. B

Perovskite-type BiNiO$_3$ is an insulating antiferromagnet in which a charge disproportionation occurs at the Bi site. La substitution for Bi suppresses the charge disproportionation and makes the system metallic. We have measured the photoemission and x-ray absorption (XAS) spectra of Bi$_{1-x}$La$_{x}$NiO$_{3}$ to investigate how the electronic structure changes with La doping. From Ni $2p$ XAS, we observed an increase of the valence of Ni from 2+ toward 3+. Combined with the core-level photoemission study, it was found that the average valence of Bi remains $\sim 4+$ and that the Ni valence behaves as $\sim (2+x)+$, that is, La substitution results in hole doping at the Ni sites. In the valence-band photoemission spectra, we observed a Fermi cutoff for $x>0$, consistent with the metallic behavior of the La-doped compounds. The Ni $2p$ XAS, Ni $2p$ core-level photoemission, and valence-band photoemission spectra were analyzed by configuration-interaction cluster-model calculation, and the spectral line shapes were found to be consistent with the gradual Ni$^{2+} \to$ Ni$^{3+}$ valence change., 6 pages, 7 figures

Metal-insulator transitions strongly coupled with lattice were found in Bi1-xLaxNiO3. Synchrotron X-ray powder diffraction revealed that pressure (P ~ 3 GPa, T = 300 K), temperature (T ~ 340 K, x = 0.05), and La-substitution (x ~ 0.075, T = 300 K) caused the similar structural change from a triclinic (insulating) to an orthorhombic (metallic) symmetry, suggesting melting of the A-site charge disproportionation. Comparing crystal structure and physical properties with the other ANiO3 series, an electronic state of the metallic phase can be described as [A3+Ld, Ni2+L1-d], where a ligand-hole L contributes to a conductivity. We depicted a schematic P-T phase diagram of BiNiO3 including a critical point (3 GPa, 300 K) and an inhomogeneous region, which implies universality of ligand-hole dynamics in ANiO3 (A = Bi, Pr, Nd,...)., 24 pages, 8 figures, Phys. Rev. B in press

We have measured magnetic susceptibility and resistivity of Sr$_{1-x}$Y$_x$CoO$_{3-��}$ ($x=$ 0.1, 0.15, 0.2, 0.215, 0.225, 0.25, 0.3, and 0.4), and have found that Sr$_{1-x}$Y$_x$CoO$_{3-��}$ is a room temperature ferromagnet with a Curie temperature of 335 K in a narrow compositional range of 0.2 $\leq x\leq$ 0.25. This is the highest transition temperature among perovskite Co oxides. The saturation magnetization for $x=$ 0.225 is 0.25 $��_B$/Co at 10 K, which implies that the observed ferromagnetism is a bulk effect. We attribute this ferromagnetism to a peculiar Sr/Y ordering., 5 pages, 4 figures

La$_4$Cu$_3$MoO$_{12}$ is a cluster antiferromagnet where copper spin-1/2 form a network of st rongly coupled spin-trimers. The magnetic properties of this material have bee n examined using magnetic neutron scattering. At low temperatures, excitations from the ground state are observed at 7.5(3) meV and 132.5(5) meV. An additio nal peak in the neutron scattering spectrum, which appears at 125.0(5) meV on heating is ascribed to a transition between excited states. The wave-vector an d temperature-dependence of the inelastic magnetic scattering cross section is consistent with intra-trimer transitions. Magnetic neutron diffraction reveal s antiferromagnetic order below T$_N$=2.6 K that doubles the unit cell along t he {\bf a} direction. The ordered magnetic structure is described as inter-tri mer order where spin correlations within trimers are controlled by the strong intra-trimer interactions. Combining the information derived from elastic and inelastic magnetic neutron scattering with group theoretical analysis, a consi stent set of intra-trimer interactions and ordered magnetic structures are der ived. The experiment provides a simple worked example of magnetism associated with inter-atomic composite degrees of freedom in the extreme quantum limit., submitted to PRB