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Transition metal dichalcogenides with superperiodic lattice distortions have been widely investigated as the platform of ultrafast structural phase manipulations. Here we performed ultrafast electron diffraction on room-temperature TaTe$_2$, which exhibits peculiar double zigzag chain pattern of Ta atoms. From the time-dependent electron diffraction pattern, we revealed a photoinduced change in the crystal structure occurring within <0.5 ps, though there is no corresponding high-temperature equilibrium phase. We further clarified the slower response (~1.5 ps) reflecting the lattice thermalization. Our result suggests the unusual ultrafast crystal structure dynamics specific to the non-equilibrium transient process in TaTe$_2$., Comment: The paer is accepted in Applied Physics Express.(Open Access)

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., Comment: 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

Cu2OSeO3 is known as a unique example of insulating multiferroic compounds with skyrmion spin texture, which is characterized by the chiral cubic crystal structure at ambient pressure. Recently, it has been reported that this compound shows pressure-induced structural transition with large enhancement of magnetic ordering temperature Tc. In the present study, we have investigated the detailed crystal structure in the high pressure phase, by combining the synchrotron X-ray diffraction experiment with the diamond anvil cell and the analysis based on the genetic algorithm. Our results suggest that the original pyrochlore Cu network is sustained even after the structural transition, while the orientation of SeO3 molecule as well as the position of oxygen in the middle of Cu tetrahedra are significantly modified. The latter features may be the key for the reported enhancement of Tc and associated stabilization of skyrmion phase at room temperature., Comment: 13 pages, 4 figures, 1 table

Topologically nontrivial materials host protected edge states associated with the bulk band inversion through the bulk-edge correspondence. Manipulating such edge states is highly desired for developing new functions and devices practically using their dissipation-less nature and spin-momentum locking. Here we introduce a transition-metal dichalcogenide VTe$_2$, that hosts a charge density wave (CDW) coupled with the band inversion involving V3$d$ and Te5$p$ orbitals. Spin- and angle-resolved photoemission spectroscopy with first-principles calculations reveal the huge anisotropic modification of the bulk electronic structure by the CDW formation, accompanying the selective disappearance of Dirac-type spin-polarized topological surface states that exist in the normal state. Thorough three dimensional investigation of bulk states indicates that the corresponding band inversion at the Brillouin zone boundary dissolves upon CDW formation, by transforming into anomalous flat bands. Our finding provides a new insight to the topological manipulation of matters by utilizing CDWs' flexible characters to external stimuli., Comment: 46 pages, 6 main figures, 12 supplementary figures

Controlling acoustic phonons, the carriers of sound and heat, has been attracting great attention toward the manipulation of sonic and thermal properties in nanometric devices. In particular, the photo-acoustic effect using ultrafast optical pulses has a promising potential to optically manipulate phonons in picoseconds time regime. However, its mechanism has been so far mostly based on the commonplace thermoelastic expansion in isotropic media, limiting the spectrum of potential applications. We investigate a conceptually new mechanism of photo-acoustic effect involving the structural instability, by utilizing a transition-metal dichalcogenide VTe$_2$ with the ribbon-type charge-density-wave (CDW). Ultrafast electron microscope imaging and diffraction measurements reveal the generation and propagation of unusual acoustic waves in the nanometric thin plate associated with the optically induced instantaneous charge-density-wave dissolution. Our results highlight the capability of photo-induced structural instability as a source of coherent acoustic waves., Comment: 6 pages, 5 figures

Field-dependent magnetic structure of a layered Dirac material EuMnBi$_2$ was investigated in detail by the single crystal neutron diffraction and the resonant x-ray magnetic diffraction techniques. On the basis of the reflection conditions in the antiferromagnetic phase at zero field, the Eu moments were found to be ordered ferromagnetically within the $ab$ plane and stacked antiferromagnetically along the $c$ axis in the sequence of up-up-down-down. Upon the spin-flop transition under the magnetic field parallel to the $c$ axis, the Eu moments are reoriented from the $c$ to the $a$ or $b$ directions forming two kinds of spin-flop domains, whereas the antiferromagnetic structure of the Mn sublattice remains intact as revealed by the quantitative analysis of the change in the neutron diffraction intensities. The present study provides a concrete basis to discuss the dominant role of the Eu sublattice on the enhanced two-dimensionality of the Dirac fermion transport in EuMnBi$_2$., Comment: 16 pages, 5 figures, accepted in PRB

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

We report spin-split Landau levels of quasi-two-dimensional Dirac fermions in a layered antiferromagnet EuMnBi$_2$, as revealed by interlayer resistivity measurements in a tilted magnetic field up to $\sim$35 T. The amplitude of Shubnikov-de Haas (SdH) oscillation in interlayer resistivity is strongly modulated by changing the tilt angle of the field, i.e., the Zeeman-to-cyclotron energy ratio. The effective $g$ factor estimated from the tilt angle, where the SdH oscillation exhibits a phase inversion, differs by approximately 50% between two antiferromagnetic phases. This observation signifies a marked impact of the magnetic order of Eu sublattice on the Dirac-like band structure. The origin may be sought in strong exchange coupling with the local Eu moments, as verified by the first-principles calculation., Comment: 13 pages, 4 figures, submitted

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

For the innovation of spintronic technologies, Dirac materials, in which the low-energy excitation is described as relativistic Dirac fermions, are one of the most promising systems, because of the fascinating magnetotransport associated with the extremely high mobility. To incorporate Dirac fermions into spintronic applications, their quantum transport phenomena are desired to be manipulated to a large extent by magnetic order in a solid. We here report a bulk half-integer quantum Hall effect in a layered antiferromagnet EuMnBi$_2$, in which field-controllable Eu magnetic order significantly suppresses the interlayer coupling between the Bi layers with Dirac fermions. In addition to the high mobility more than 10,000 cm$^2$/Vs, Landau level splittings presumably due to the lifting of spin and valley degeneracy are noticeable even in a bulk magnet. These results will pave a route to the engineering of magnetically functionalized Dirac materials., Comment: 26 pages, 4 figures, 1 table

Ferroelectrics with spontaneous electric polarization play an essential role in today's device engineering, such as capacitors and memories. Their physical properties are further enriched by suppressing the long-range polar order, as is exemplified by quantum paraelectrics with giant piezoelectric and dielectric responses at low temperatures. Likewise in metals, a polar lattice distortion has been theoretically predicted to give rise to various unusual physical properties. So far, however, a "ferroelectric"-like transition in metals has seldom been controlled and hence its possible impacts on transport phenomena remain unexplored. Here we report the discovery of anomalous enhancement of thermopower near the critical region between the polar and nonpolar metallic phases in 1T'-Mo$_{1-x}$Nb$_{x}$Te$_2$ with a chemically tunable polar transition. It is unveiled from the first-principles calculations and magnetotransport measurements that charge transport with strongly energy-dependent scattering rate critically evolves towards the boundary to the nonpolar phase, resulting in large cryogenic thermopower. Such a significant influence of the structural instability on transport phenomena might arise from the fluctuating or heterogeneous polar metallic states, which would pave a novel route to improving thermoelectric efficiency., Comment: 26 pages, 4 figures

The relation between the polar structural instability and superconductivity in a Weyl semimetal candidate MoTe2 has been clarified by finely controlled physical and chemical pressure. The physical pressure as well as the chemical pressure, i.e., the Se substitution for Te, enhances the superconducting transition temperature Tc at around the critical pressure where the polar structure transition disappears. From the heat capacity and thermopower measurements, we ascribe the significant enhancement of Tc at the critical pressure to a subtle modification of the phonon dispersion or the semimetallic band structure upon the polar-to-nonpolar transition. On the other hand, the physical pressure, which strongly reduces the interlayer distance, is more effective on the suppression of the polar structural transition and the enhancement of Tc as compared with the chemical pressure, which emphasizes the importance of the interlayer coupling on the structural and superconducting instability in MoTe2., Comment: 5 pages, 4 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., Comment: 23 pages, 10 figures

We investigate the surface electronic structures of polar 1T'-MoTe2, the Weyl semimetal candidate realized through the nonpolar-polar structural phase transition, by utilizing the laser angle-resolved photoemission spectroscopy (ARPES) combined with first-principles calculations. Two kinds of domains with different surface band dispersions are observed from a single-crystalline sample. The spin-resolved measurements further reveal that the spin polarizations of the surface and the bulk-derived states show the different domain-dependences, indicating the opposite bulk polarity. For both domains, some segment-like band features resembling the Fermi arcs are clearly observed. The patterns of the arcs present the marked contrast between the two domains, respectively agreeing well with the slab calculation of (0 0 1) and (0 0 -1) surfaces. The present result strongly suggests that the Fermi arc connects the identical pair of Weyl nodes on one side of the polar crystal surface, whereas it connects between the different pairs of Weyl nodes on the other side., Comment: 13 pages, 4 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

There is still no general consensus on how one can describe the out-of-equilibrium phenomena in matter induced by an ultrashort light pulse. We investigate the pulse-induced dynamics in a layered Dirac semimetal SrMnBi2 by pump-and-probe photoemission spectroscopy. At ~<1 ps, the electronic recovery slowed upon increasing the pump power. Such a bottleneck-type slowing is expected in a two-temperature model (TTM) scheme, although opposite trends have been observed to date in graphite and in cuprates. Subsequently, an unconventional power-law cooling took place at ~100 ps, indicating that spatial heat diffusion is still ill defined at ~100 ps. We identify that the successive dynamics before the emergence of heat diffusion is a canonical realization of a TTM scheme. Criteria for the applicability of the scheme is also provided.

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

Effects of electron doping on the BiS$_2$-based superconductors Sr$_{1-x}$La$_x$FBiS$_2$ ($0\le x\le 0.6$) have been investigated using the systematically synthesized polycrystals. The pristine compound is a band insulator with the BiS$_2$ layer, which accommodates electron carriers through the La substitution for Sr, as evidenced by the change in x-ray absorption spectra reflecting the occupancy of Bi 6$p$ orbitals. With increasing the carrier density, the resistivity progressively decreases and a bad metallic state appears for $x\ge0.45$, where bulk superconductivity manifests itself below approximately 3 K. The value of $T_{\rm c}$ gradually increases with decreasing $x$ from 0.6 to 0.45 and immediately decreases down to zero at the critical concentration of $x\sim 0.4$, resulting in an insulator-superconductor transition highly sensitive to the carrier density. Thermodynamic measurements furthermore have revealed the possible enhancement of the superconducting coupling strength as the insulating phase is approached. The obtained superconducting phase diagram is markedly different from the broad dome-shaped superconducting phase previously reported for $R$O$_{1-x}$F$_x$BiS$_2$ ($R$: rare-earth ion), suggesting a strong influence of the blocking layer on the superconductivity. Instead all these features are similar to those observed in Li-intercalated ZrNCl superconductor, except for the critical electron concentration of as low as 6% in the latter compound. For the present superconductor, notably, the existence of hole-type carriers has been indicated in the normal state from the Hall effect measurements. The Sr$_{1-x}$La$_x$FBiS$_2$ system providing the phase diagram for the rigid-band doping in the BiS$_2$ layer would be another prototypical example of superconductivity derived from a doped layered band insulator, hosting both hole-like and electron-like Fermi surfaces., Comment: 19 pages, 8 figures, accepted for publication in J. Phys. Soc. Jpn

The chirality, i.e. left or right handedness, is an important notion in a broad range of science. In condensed matter, this occurs not only in molecular or crystal forms but also in magnetic structures. A magnetic skyrmion, a topologically-stable spin vortex structure, as observed in chiral-lattice helimagnets is one such example; the spin swirling direction (skyrmion helicity) should be closely related to the underlying lattice chirality via the relativistic spin-orbit coupling (SOC). Here, we report on the correlation between skyrmion helicity and crystal chirality as observed by Lorentz transmission electron microscopy (TEM) and convergent-beam electron diffraction (CBED) on the composition-spread alloys of helimagnets Mn1-xFexGe over a broad range (x = 0.3 - 1.0) of the composition. The skyrmion lattice constant or the skyrmion size shows non-monotonous variation with the composition x, accompanying a divergent behavior around x = 0.8, where the correlation between magnetic helicity and crystal chirality is reversed. The underlying mechanism is a continuous x-variation of the SOC strength accompanying sign reversal in the metallic alloys. This may offer a promising way to tune the skyrmion size and helicity., Comment: 15 pages, 4 figures, 1 table

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., Comment: 5 pages, 4 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 $q \parallel <001>$ 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 $q \parallel <110>$ to $q \parallel <001>$ 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., Comment: 5 pages, 4 figures, published as a Rapid Communication in Phys. Rev. B

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., Comment: 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., Comment: 13 pages, 5 figures

We have investigated the thermal Hall effect of magnons for various ferromagnetic insulators. For pyrochlore ferromagnetic insulators Lu$_2$V$_2$O$_7$, Ho$_2$V$_2$O$_7$, and In$_2$Mn$_2$O$_7$, finite thermal Hall conductivities have been observed below the Curie temperature $T_C$ . From the temperature and magnetic field dependences, it is concluded that magnons are responsible for the thermal Hall effect. The Hall effect of magnons can be well explained by the theory based on the Berry curvature in momentum space induced by the Dzyaloshinskii-Moriya (DM) interaction. The analysis has been extended to the transition metal (TM) oxides with perovskite structure. The thermal Hall signal was absent or far smaller in La$_2$NiMnO$_6$ and YTiO$_3$, which have the distorted perovskite structure with four TM ions in the unit cell. On the other hand, a finite thermal Hall response is discernible below $T_C$ in another ferromagentic perovskite oxide BiMnO$_3$, which shows orbital ordering with a larger unit cell. The presence or absence of the thermal Hall effect in insulating pyrochlore and perovskite systems reflect the geometric and topological aspect of DM-induced magnon Hall effect., Comment: 26 pages, 14 figures; v2: accepted version

A helical spin texture is of great current interest for a host of novel spin-dependent transport phenomena. We report a rich variety of nontrivial, helimagnetic phases in the simple cubic perovskite SrFeO3 under magnetic fields up to 42 T. Magnetic and resistivity measurements revealed that the proper-screw spin phase proposed for SrFeO3 can be subdivided into at least five kinds of ordered phases. Near the multicritical point, an unconventional anomalous Hall effect was found to show up and was interpreted as due to a possible long-period noncoplanar spin texture with scalar spin chirality., Comment: 5 pages, 5 figures, Physical Review B in press

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., Comment: 8 pages, 5 figures, 2 tables

Transport and magnetic properties have been systematically investigated for SmMnAsO_{1-x} with controlled electron-doping. As the electron band-filling is increased with the increase of oxygen deficiency (x), the resistivity monotonically decreases and the transition from Mott-insulator to metal occurs between x=0.17 and 0.2. Seebeck coefficient at room temperature abruptly changes around the critical doping level from a large value (\sim -300 \mu V/K) to a small one (\sim -50 \mu V/K) both with negative sign. In the metallic compounds with x=0.2 and x=0.3, Mn spins order antiferromagnetically around 30 K, and the Hall coefficient with the negative sign shows a reduction in magnitude upon the magnetic transition, indicating the change in the multiple Fermi surfaces. Gigantic positive magnetoresistance effect is observed in a wide range of temperature, reaching up to 60 % at 2 K for the x=0.3 compound. The effect is attributed to the field-induced change of the complex Fermi surfaces in this multi-orbital correlated electron system., Comment: 8 pages, 9 figures

Magnetic and dielectric properties with varying magnitude and direction of magnetic field H have been investigated for a triangular lattice helimagnet MnI2. The in-plane electric polarization P emerges in the proper screw magnetic ground state below 3.5 K, showing the rearrangement of six possible multiferroic domains as controlled by the in-plane H. With every 60-degree rotation of H around the [001]-axis, discontinuous 120-degree flop of P-vector is observed as a result of the flop of magnetic modulation vector q. With increasing the in-plane H above 3 T, however, the stable q-direction changes from q||<1-10> to q||<110>, leading to a change of P-flop patterns under rotating H. At the critical field region (~3 T), due to the phase competition and resultant enhanced q-flexibility, P-vector smoothly rotates clockwise twice while H-vector rotates counter-clockwise once., Comment: 4 pages, 3 figures. Accepted in Physical Review Letters

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 ($0^\circ<\theta<90^\circ$) by external magnetic fields, we identify the maximal magnetochromism around $\theta\approx45^\circ$. On the contrary, there is no remarkable signature of the electromagnon in the proper screw and spin-collinear (ferrimagnetic) phases, clearly indicating the important role of the conical spin order to produce the magnetically-controllable electromagnons. The possible origin of this electromagnon is argued in terms of the exchange-striction mechanism., Comment: 19 pages including 7 figures; Accepted for publication in Phys. Rev. B

Single crystals of electron-doped SrMnO3 with a cubic perovskite structure have been systematically investigated as the most canonical (orbital-degenerate) double-exchange system, whose ground states have been still theoretically controversial. With only 1-2% electron doping by Ce substitution for Sr, a G-type antiferromagnetic metal with a tiny spin canting in a cubic lattice shows up as the ground state, where the Jahn-Teller polarons with heavy mass are likely to form. Further electron doping above 4%, however, replaces this isotropic metal with an insulator with tetragonal lattice distortion, accompanied by a quasi-one-dimensional 3z^2-r^2 orbital ordering with the C-type antiferromagnetism. The self-organization of such dilute polarons may reflect the critical role of the cooperative Jahn-Teller effect that is most effective in the originally cubic system., Comment: 5 pages, 4 figures

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., Comment: 5 pages, 5 figures

We have investigated electrically-active magnetic excitations (electromagnons) in perovskite manganites with the $E$-type (up-up-down-down) spin structure by terahertz spectroscopy. Eu$_{1-x}$Y$_x$MnO$_3$ (0.1$\le x\le$1) and Y$_{1-y}$Lu$_y$MnO$_3$ (0$\le y\le$1) without magnetic $f$-moments, which host collinear sinusoidal, $A$-type, cycloidal, and $E$-type spin orders, are used to examine the systematics of possible electromagnons. Three-peak structures (23, 35, 45 cm$^{-1}$) of magnetic origin show up in the $E$-type phase with little composition ($y$) dependence of frequencies, making a contrast with the electromagnons observed in the cycloidal-spin ($x\le0.8$) phases. One of these electromagnon is ascribed to the zone-edge magnon mode based on the calculated magnon dispersions., Comment: 5 pages, 4 figures

Complete magnetoelectric (ME) phase diagrams of orthorhombic $R$MnO$_{3}$ with and without magnetic moments on the $R$ ions have been established. Three kinds of multiferroic ground states, the $ab$-cycloidal, the $bc$-cycloidal, and the collinear $E$-type phases, have been identified by the distinct ME responses. The electric polarization of the $E$-type phase dominated by the symmetric spin exchange ($bm{S}_{i} cdot bm{S}_{j}$) is more than 10 times as large as that of the $bc$-cycloidal phase dominated by the antisymmetric one ($bm{S}_{i} times bm{S}_{j}$), and the ME response is enhanced near the bicritical phase boundary between these multiferroic phases of different origins. These findings will provide an important clue for the development of the magnetically induced multiferroics., Comment: 5 pages, 3 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., Comment: 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., Comment: 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,...)., Comment: 24 pages, 8 figures, Phys. Rev. B in press

We have measured magnetic susceptibility and resistivity of Sr$_{1-x}$Y$_x$CoO$_{3-\delta}$ ($x=$ 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$_{3-\delta}$ 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 $\mu_B$/Co at 10 K, which implies that the observed ferromagnetism is a bulk effect. We attribute this ferromagnetism to a peculiar Sr/Y ordering., Comment: 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., Comment: submitted to PRB