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Magnetoelectric mutual control in multiferroics, which is the electric control of magnetization, or reciprocally the magnetic control of polarization has attracted much attention because of its possible applications to spintronic devices, multi-bit memories, and so on. While the required working temperature for the practical application is much higher than room temperature, which ensures stable functionality at room temperature, the reported working temperatures were at most around room temperature. Here, we demonstrated magnetic control of ferroelectric polarization at 432 K in ferroelectric and ferroelastic Tb$_2$(MoO$_4$)$_3$, in which the polarity of ferroelectric polarization is coupled to the orthorhombic strain below the transition temperature 432 K. The paramagnetic but strongly magnetoelastic Tb$^{3+}$ magnetic moments enable the magnetic control of ferroelectric and ferroelastic domains; the ferroelectric polarization is controlled depending on whether the magnetic field is applied along [110] or [$\bar{1}$10]. This result may pave a new avenue for designing high-temperature multiferroics., Comment: 13 pages, 7 figures

Strongly correlated spin systems can be driven to quantum critical points via various routes. In particular, gapped quantum antiferromagnets can undergo phase transitions into a magnetically ordered state with applied pressure or magnetic field, acting as tuning parameters. These transitions are characterized by $z=1$ or $z=2$ dynamical critical exponents, determined by the linear and quadratic low-energy dispersion of spin excitations, respectively. Employing high-frequency susceptibility and ultrasound techniques, we demonstrate that the tetragonal easy-plane quantum antiferromagnet NiCl$_{2}\cdot$4SC(NH$_2$)$_2$ (aka DTN) undergoes a spin-gap closure transition at about $4.2$ kbar, resulting in a pressure-induced magnetic ordering. The studies are complemented by high-pressure-electron spin-resonance measurements confirming the proposed scenario. Powder neutron diffraction measurements revealed that no lattice distortion occurs at this pressure and the high spin symmetry is preserved, establishing DTN as a perfect platform to investigate $z=1$ quantum critical phenomena. The experimental observations are supported by DMRG calculations, allowing us to quantitatively describe the pressure-driven evolution of critical fields and spin-Hamiltonian parameters in DTN., Comment: Main text: 9 pages, 7 figures. Supplemental Material: 8 pages, 6 figures

High-field phase diagram of a chiral-lattice antiferromagnet Sr(TiO)Cu4(PO4)4 is studied by means of the ultrasound, dielectric, and magnetocaloric-effect measurements. These experimental techniques reveal two new phase transitions at high fields, which have not been resolved by the previous magnetization experiments. Specifically, the c66 acoustic mode shows drastic changes with hysteresis with applied fields along the c axis, indicating a strong magneto-elastic coupling. Combined with the cluster mean-field theory, we discuss the origins of these phase transitions. By considering the chiral-twist effect of Cu4O12 cupola units, which is inherent to the chiral crystal structure, the phase diagram is reasonably reproduced. The agreement between the experiment and theory suggests that this material is a unique quasi two-dimensional spin system with competing exchange interactions and chirality, leading to the rich phase diagram., Comment: 12 pages, 11 figures, 1 table

In this study, we have performed the magnetocaloric effect and the specific heat measurements of chromium spinel oxide HgCr$_2$O$_4$, wherein the magnetic Cr$^{3+}$ ions form a highly frustrated pyrochlore lattice with significant spin-lattice coupling. In addition to the known magnetic-field-induced phases, our thermodynamic measurements detect a novel quantum phase just before the saturation of the magnetization, which has not been expected from the classical theories of the pyrochlore lattice antiferromagnet with spin-lattice coupling. Based on recent theoretical model calculation, we discuss the possibility of a spin nematic state appearing for this quantum phase., Comment: 14 pages, 4 figures

Nematic orders emerge nearly universally in iron-based superconductors, but elucidating their origins is challenging because of intimate couplings between orbital and magnetic fluctuations. The iron-based ladder material BaFe2S3, which superconducts under pressure, exhibits antiferromagnetic order below TN ~ 117K and a weak resistivity anomaly at T* ~ 180K, whose nature remains elusive. Here we report angle-resolved magnetoresistance (MR) and elastoresistance (ER) measurements in BaFe2S3, which reveal distinct changes at T*. We find that MR anisotropy and ER nematic response are both suppressed near T*, implying that an orbital order promoting isotropic electronic states is stabilized at T*. Such an isotropic state below T* competes with the antiferromagnetic order, which is evidenced by the nonmonotonic temperature dependence of nematic fluctuations. In contrast to the cooperative nematic orders in spin and orbital channels in iron pnictides, the present competing orders can provide a new platform to identify the separate roles of orbital and magnetic fluctuations., Comment: 7 pages 5 figures, to be published in Phys. Rev. Res

Magnetic-field effect on the magnetic and electric properties in a chiral polar ordered corundum Ni$_2$InSbO$_6$ has been investigated. Single-crystal soft x-ray and neutron diffraction measurements confirm long-wavelength magnetic modulation. The modulation direction tends to align along the magnetic field applied perpendicular to the polar axis, suggesting that the nearly proper-screw type helicoid should be formed below 77\,K. The application of a high magnetic field causes a metamagnetic transition. In a magnetic field applied perpendicular to the polar axis, a helix-to-canted antiferromagnetic transition takes place through the intermediate soliton lattice type state. On the other hand, a magnetic field applied along the polar axis induces a first-order metamagnetic transition. These metamagnetic transitions accompany a change in the electric polarization along the polar axis.

The wavefuntion of conduction electrons moving in the background of a non-coplanar spin structure can gain a quantal phase - Berry phase - as if the electrons were moving in a strong fictitious magnetic field. Such an emergent magnetic field effect is approximately proportional to the solid angle subtended by the spin moments on three neighbouring spin sites, termed the scalar spin chirality. The entire spin chirality of the crystal, unless macroscopically canceled, causes the geometrical Hall effect of real-space Berry-phase origin, whereas the intrinsic anomalous Hall effect (AHE) in a conventional metallic ferromagnet is of the momentum-space Berry-phase origin induced by relativistic spin-orbit coupling (SOC). Here, we report the ordering phenomena of the spin-trimer scalar spin chirality and the consequent large geometrical Hall effect in the breathing kagom\'e lattice compound Dy$_3$Ru$_4$Al$_{12}$, where the Dy$^{3+}$ moments form non-coplanar spin trimers with local spin chirality. Using neutron diffraction, we show that the local spin chirality of the spin trimers as well as its ferroic/antiferroic orders can be switched by an external magnetic field, accompanying large changes in the geometrical Hall effect. Our finding reveals that systems composed of tunable spin trimers can be a fertile field to explore large emergent electromagnetic responses arising from real-space topological magnetic orders., Comment: 15 pages, 12 figures

In this study, we conducted various magnetotransport measurements on Fe$_{1+y}$Te$_{1-x}$Se$_{x}$ single crystals from which excess iron was sufficiently removed. Our results revealed that crossover from the incoherent to the coherent electronic state and opening of the pseudogap occur at high temperatures ($\approx$ 150 K for $x$ = 0.2). This is accompanied by a more substantial pseudogap and the emergence of a phase with a multi-band nature at lower temperatures (below $\approx$ 50 K for $x$ = 0.2) before superconductivity sets in. A comparison of these results with those of the as-grown (non-superconducting) samples implies that the coherent state accompanied by the pseudogap is needed for the occurrence of superconductivity in this system., Comment: 9 pages, 7 figures

We report our combined experimental and theoretical study of magnetoelectric properties of an antiferromagnet Sr(TiO)Cu$_4$(PO$_4$)$_4$, in comparison with the isostructurals Ba(TiO)Cu$_4$(PO$_4$)$_4$ and Pb(TiO)Cu$_4$(PO$_4$)$_4$. The family of compounds commonly possesses a low-symmetric magnetic unit called the square cupola, which is a source of magnetoelectric responses associated with the magnetic multipoles activated under simultaneous breaking of spatial inversion and time reversal symmetries. Measuring the full magnetization curves and the magnetic-field profiles of dielectric constant for Sr(TiO)Cu$_4$(PO$_4$)$_4$ and comparing them with the theoretical analyses by the cluster mean-field theory, we find that the effective $S=1/2$ spin model, which was used for the previous studies for Ba(TiO)Cu$_4$(PO$_4$)$_4$ and Pb(TiO)Cu$_4$(PO$_4$)$_4$, well explains the experimental results by tuning the model parameters. Furthermore, elaborating the phase diagram of the model, we find that the square cupolas could host a variety of magnetic multipoles, i.e., monopole, toroidal moment, and quadrupole tensor, depending on the parameters that could be modulated by deformations of the magnetic square cupolas. Our results not only provide a microscopic understanding of the series of the square cupola compounds, but also stimulate further exploration of the magnetoelectric behavior arising from cluster multipoles harboring in low-symmetric magnetic units., Comment: 13 pages, 12 figures

We perform a combined experimental and theoretical study of a magnetic-field ($B$) induced evolution of magnetic and ferroelectric properties in an antiferromagnetic material Pb(TiO)Cu$_4$(PO$_4$)$_4$, whose structure is characterized by a staggered array of Cu$_4$O$_{12}$ magnetic units with convex geometry known as square cupola. Our experiments show a $B$-induced phase transition from a previously reported low-$B$ linear magnetoelectric phase to a new high-$B$ magnetoelectric phase, which accompanies a 90$^\circ$ flop of electric polarization and gigantic magnetodielectric effect. Moreover, we observe a $B$-induced sign reversal of ferroelectric polarization in the high-$B$ phase. Our model and first-principles calculations reveal that the observed complex magnetoelectric behavior is well explained in terms of a $B$-dependent electric polarization generated in each Cu$_4$O$_{12}$ unit by the so-called exchange striction mechanism. The present study demonstrates that the materials design based on the magnetic structural unit with convex geometry deserves to be explored for developing strong magnetoelectric couplings., Comment: 13 pages, 9 figures

To investigate the relationship between the pseudogap and superconductivity, we measured both the in-plane ($\rho_{ab}$) and out-of-plane ($\rho_c$) resistivity for oxygen-controlled Bi$_{2}$Sr$_{2}$CaCu$_{2}$O$_{8+\delta}$ single crystals subject to magnetic fields (parallel to the $c$ axis) of up to 17.5 T. The onset temperature for the superconductive fluctuation, $T_{scf}$, is determined by the large positive in-plane magnetoresistance (MR) and negative out-of-plane MR observed near $T_c$, whereas the pseudogap opening temperature $T^*$ is determined by the semiconductive upturn of the zero-field $\rho_c$. $T_{scf}$ was found to scale roughly as $T_c$, with a decreasing temperature interval between them upon doping. On the other hand, $T^*$ starts out much higher than $T_{scf}$ but decreases monotonically upon doping; finally, at a heavily overdoped state, it is not observed above $T_{scf}$. These results imply that the pseudogap is not a simple precursor of superconductivity, but that further study is needed to determine whether or not $T^*$ exists below $T_{scf}$ in the heavily overdoped state., Comment: 17 pages, 7 figures, to appear in JPSJ

We have investigated spin-wave excitations in a four-sublattice (4SL) magnetic ground state of a frustrated magnet CuFeO2, in which `electromagnon' (electric-field-active magnon) excitation has been discovered by recent terahertz time-domain spectroscopy [Seki et al. Phys. Rev. Lett. 105 097207 (2010)]. In previous study, we have identified two spin-wave branches in the 4SL phase by means of inelastic neutron scattering measurements under applied uniaxial pressure. [T. Nakajima et al. J. Phys. Soc. Jpn. 80 014714 (2011) ] In the present study, we have performed high-energy-resolution inelastic neutron scattering measurements in the 4SL phase, resolving fine structures of the lower-energy spin-wave branch near the zone center. Taking account of the spin-driven lattice distortions in the 4SL phase, we have developed a model Hamiltonian to describe the spin-wave excitations. The determined Hamiltonian parameters have successfully reproduced the spin-wave dispersion relations and intensity maps obtained in the inelastic neutron scattering measurements. The results of the spin-wave analysis have also revealed physical pictures of the magnon and electromagnon modes in the 4SL phase, suggesting that collinear and noncollinear characters of the two spin-wave modes are the keys to understand the dynamical coupling between the spins and electric dipole moments in this system., Comment: 8 pages, 6 figures

We report the experimental and the analytical results of electron spin resonance (ESR) and magnetization in high magnetic fields up to about 68 T of the quasi two-dimensional triangular lattice antiferromagnet NiGa$_2$S$_4$. From the temperature evolution of the ESR absorption linewidth, we find a distinct disturbing of the development of the spin correlation by $Z_2$-vortices between 23 K and 8.5 K. Below $T_{\rm{v}}=8.5$ K, spin-wave calculations based on a 57$^{\circ}$ spiral spin order well explains the frequency dependence of the ESR resonance fields and high field magnetization processes for $H$$\parallel$$c$ and $H$$\perp$$c$, although the magnetization for $H$$\perp$$c$ at high fields is different from the calculated one. Furthermore, we explain the field independent specific heat with $T^2$-dependence by the same spin-wave calculation, but the magnitude of the specific heat is much less than the observed one. Accordingly, these results suggest the occurrence of a $Z_2$ vortex-induced topological transition at $T_{\rm{v}}$ and may indicate quantum effects beyond the descriptions based on the above classical spin models.