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A compact energy-recovery linac (cERL) has been un-der construction at KEK since 2009 to develop key technologies for the energy-recovery linac. The cERL began operating in 2013 to create a high-current beam with a low-emittance beam with stable continuous wave (CW) superconducting cavities. Owing to the development of critical components, such as the DC gun, superconducting cavities, and the design of ideal beam transport optics, we have successfully established approximately 1 mA stable CW operation with a small beam emittance and extremely small beam loss. This study presents the details of our key technologies and experimental results for achieving 100% energy recovery operation with extremely small beam loss during a stable, approximately 1 mA CW beam operation., Comment: 11 pages, 16 figures

We successfully synthesized a verdazyl-based complex, ($p$-Py-V-$p$-CN)$_2$[Cu(hfac)$_2$]. Molecular orbital calculations reveal that three types of antiferromagnetic (AF) interactions are involved in the formation of a spin-1/2 distorted octagonal lattice composed of the verdazyl radical and Cu spins. The magnetic properties of the compound exhibited contributions from AF correlations and a phase transition to an AF ordered state at approximately $T_{\rm{N}}$ = 2.5 K. Below $T_{\rm{N}}$, we observed a $T^2$ dependence of the specific heat, indicating dominant two-dimensional AF correlations within the octagonal lattice. The magnetization curve in the low-temperature region exhibited a low-field linear increase, subsequent bending at 1/3 magnetization, and high-field nonlinear increase. We reproduced the observed unique magnetic behavior through the numerical analysis based on the octagonal lattice. These results demonstrate that the present compound exhibits magnetic properties characteristic of octagonal lattice topology., Comment: 7 pages, 4 figures. arXiv admin note: text overlap with arXiv:2310.14569

We report on spin Hall magnetoresistance (SMR) in bilayers composed of Pt and magnetic insulator MgFe$_{2}$O$_{4}$ (MFO) with spinel structure. The Pt thickness dependence of the SMR reveals that annealing of the MFO surface before depositing the Pt layer is crucial for a large SMR with better interface quality. We also found that oxygen pressure during the MFO growth hardly affects the SMR while it influences on magnetic property of the MFO film. Our findings provide important clues to further understanding the spin transport at interfaces containing magnetic insulators, facilitating development of low power consumption devices., Comment: 4 figures, 1 table

We successfully synthesized ($p$-Py-V)[Cu(hfac)$_2$], a verdazyl-based complex. Molecular orbital calculations revealed five types of intermolecular interactions between the radical spins and two types of intramolecular interactions between the radical and the Cu spins, resulting in a spin-1/2 distorted honeycomb-based lattice. Additionally, competing ferromagnetic and antiferromagnetic (AF) interactions induce frustration. The magnetization curve displayed a multistage increase, including a zero-field energy gap. Considering the stronger AF interactions that form dimers and tetramers, the magnetic susceptibility and magnetization curves were qualitatively explained. These findings demonstrated that the quantum state, based on the dominant AF interactions, was stabilized due to the effects of frustration in the lattice. Hence, the exchange interactions forming two-dimensional couplings decoupled, reducing energy loss caused by frustration and leading to frustration-induced dimensional reduction., Comment: 6 pages, 5 figures

This study presents the experimental realization of a spin-1/2 zigzag-square lattice in a verdazyl-based complex, namely ($m$-Py-V-2,6-F$_2$)$[$Cu(hfac)$_2]$. Molecular orbital calculations suggest the presence of five types of frustrated exchange couplings. Our observations reveal an incremental increase in the magnetization curve beyond a critical field, signifying a phase transition from the antiferromagnetic ordered state to a quantum state characterized by a 1/2 plateau. This intriguing behavior arises from the effective stabilization of a zigzag chain by the external fields. These results provide evidence for field-induced dimensional reduction in a zigzag-square lattice attributed to the effects of frustration., Comment: 5 pages, 4 figures

We developed a metallic pressure cell made of nickel-chromium-aluminum (NiCrAl) for use with a non-destructive pulse magnet and a magnetic susceptibility measurement apparatus with a proximity detector oscillator (PDO) in pulsed magnetic fields of up to 51 T under pressures of up to 2.1 GPa. Both the sample and sensor coil of the PDO were placed in the cell so that the magnetic signal from NiCrAl would not overlay the intrinsic magnetic susceptibility of the sample. A systematic investigation of the Joule heating originating from metallic parts of the pressure cell revealed that the temperature at the sample position remains at almost 1.4 K until approximately 80 $\%$ of the maximum applied magnetic field ($H_{\rm max}$) in the field-ascending process (e.g., 40 T for $H_{\rm max}$ of 51 T). The effectiveness of our apparatus was demonstrated, by investigating the pressure dependence of the magnetization process of the triangular-lattice antiferromagnet Ba$_3$CoSb$_2$O$_9$., Comment: 7pages, 5 figures

We study spin Hall magnetoresistance (SMR) in Pt/ferrimagnetic insulator Y$_{3}$Fe$_{5}$O$_{12}$ (YIG) bilayers by focusing on crystallinity, magnetization, and interface roughness by controlling post-annealing temperatures. The SMR in the Pt/YIG grown on Si substrate is comparable to that grown on widely used Gd$_{3}$Ga$_{5}$O$_{12}$ substrate, indicating that the large SMR can be achieved irrespective to the crystallinity. We deduced the spin mixing conductance from the Pt thickness dependence of the SMR to find the high interface quality of the optimized Pt/YIG grown on Si in terms of spin current. We also clarified that the SMR correlates well with the magnetization, the interface roughness, and carrier density. These findings highlight that optimizing YIG properties is a key to control of magnetization by spin current, leading to the development of low power consumption spintronic device based on the magnetic insulator.

We report on the highly efficient spin-orbit torque (SOT) generation in epitaxial SrIrO$_{3}$(SIO), which is grown on an orthorhombic DyScO$_{3}$(110) substrate. By conducting harmonic Hall measurement in Co$_{20}$Fe$_{60}$B$_{20}$ (CoFeB)/SIO bilayers, we characterize two kinds of the SOTs, i.e., dampinglike (DL) and fieldlike ones to find that the former is much larger than the latter. By comparison with the Pt control sample with the same CoFeB thickness, the observed DL SOT efficiency $\xi$$_{DL}$ of SIO ($\sim$0.32) is three times higher than that of Pt ($\sim$0.093). The $\xi$$_{DL}$ is nearly constant as a function of the CoFeB thickness, suggesting that the SIO plays a crucial role in the large SOT generation. These results on the CoFeB/SIO bilayers highlight that the epitaxial SIO is promising for low-current and reliable spin-orbit torque-controlled devices., Comment: arXiv admin note: text overlap with arXiv:2305.17887

We report on efficient spin current generation at room temperature in rutile type WO$_{2}$ grown on Al$_{2}$O$_{3}$(0001) substrate. The optimal WO$_{2}$ film has (010)-oriented monoclinically distorted rutile structure with metallic conductivity due to 5$\it{d}$$^2$ electrons, as characterized by x-ray diffraction, electronic transport, and x-ray photoelectron spectroscopy. By conducting harmonic Hall measurement in Ni$_{81}$Fe$_{19}$/WO$_{2}$ bilayer, we estimate two symmetries of the spin-orbit torque (SOT), i.e., dampinglike (DL) and fieldlike ones to find that the former is larger than the latter. By comparison with the Ni$_{81}$Fe$_{19}$/W control sample, the observed DL SOT efficiency $\xi$$_{DL}$ of WO$_{2}$ (+0.174) is about two thirds of that of W (-0.281) in magnitude, with a striking difference in their signs. The magnitude of the $\xi$$_{DL}$ of WO$_{2}$ exhibits comparable value to those of widely reported Pt and Ta, and Ir oxide IrO$_{2}$. The positive sign of the $\xi$$_{DL}$ of WO$_{2}$ can be explained by the preceding theoretical study based on the 4$\it{d}$ oxides. These results highlight that the epitaxial WO$_{2}$ offers a great opportunity of rutile oxides with spintronic functionalities, leading to future spin-orbit torque-controlled devices., Comment: 14 pages, 4 figures

Complexity of quantum phases of matter is often understood by the underlying gauge structures, as was recognized by the $\mathbb{Z}_2$ and U(1) gauge theory description of spin liquid in frustrated magnets. Anomalous Hall effect of conducting electrons can intrisically arise from U(1) gauges expressing the spatial modulation of ferromagnetic moments or from SU(2) gauges representing the spin-orbit coupling effect. Similarly, in insulating ferro and antiferromagnets, the magnon excitations can contribute to anomalous transports by feeling the U(1) and SU(2) gauges arising from the features of ordered moments or interactions. In this work, we report the emergent higher rank SU(3) gauge structure in the magnon transport based on the thermal conductivity measurements of MnSc$_2$S$_4$ in an applied field up to 14\,T. The thermal Hall coefficient takes a substantial value when the material enters a three-sublattice antiferromagnetic skyrmion phase, which is confirmed by the large-scale spin wave theory. The excited magnons are dressed with SU(3) gauge field, which is a mixture of three species of U(1) gauge fields originating from the slowly varying magnetic moments on these sublattices., Comment: 16 pages, 12 figures

We investigate the ground-state phase diagram of a spin-1/2 honeycomb-lattice antiferromagnetic (AF) Heisenberg model with three exchange interactions, $J_{\rm A}$, $J_{\rm B}$, and $J_{\rm C}$ that is realized in a distorted honeycomb-lattice antiferromagnet ${\rm Cu_2 (pymca)_3 (ClO_4)}$. We remeasured the magnetic susceptibility of its polycrystalline sample with special care, and determined the exchange parameters of this material through the comparison with numerical results based on a quantum Monte Carlo (QMC) method. The QMC method also provides a ground-state phase diagram in the $J_{\rm A}/J_{\rm C}$-$J_{\rm B}/J_{\rm C}$ plane. The phase diagram consists of a small N${\rm \acute{e}}$el phase and a gapped quantum paramagnetic phase surrounding the N${\rm \acute{e}}$el phase. The latter includes six regimes of hexagonal-singlet-type states and dimer-singlet-type states alternatingly without boundaries closing the spin gap. We further calculate the equal-time spin structure factor in each phase using the QMC method. The computed spin dynamics by the exact diagonalization method exhibits continuums near and in the AF phase. Characteristic four energy band structures in the state with strong hexagonal-singlet-type correlations are informative to clarify the ground-state of ${\rm Cu_2 (pymca)_3 (ClO_4)}$ by future neutron scattering measurements., Comment: 10 pages, 7 figures

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

We report a metal-insulator transition (MIT) in the half-filled multiorbital antiferromagnet (AF) BaMn$_2$Bi$_2$ that is tunable by a magnetic field perpendicular to the AF sublattices. Instead of an Anderson-Mott mechanism usually expected in strongly correlated systems, we find by scaling analyses that the MIT is driven by an Anderson localization. Electrical and thermoelectrical transport measurements in combination with electronic band calculations reveal a strong orbital-dependent correlation effect, where both weakly and strongly correlated $3d$-derived bands coexist with decoupled charge excitations. Weakly correlated holelike carriers in the $d_{xy}$-derived band dominate the transport properties and exhibit the Anderson localization, whereas other $3d$ bands show clear Mott-like behaviors with their spins ordered into AF sublattices. The tuning role played by the perpendicular magnetic field supports a strong spin-spin coupling between itinerant holelike carriers and the AF fluctuations, which is in sharp contrast to their weak charge coupling.

The 5d transition-metal oxides have been an intriguing platform to demonstrate efficient charge to spin current conversion due to a unique electronic structure dominated by strong spin-orbit coupling. Here, we report on stacking-order effect of spin-orbit torque (SOT), spin-Hall magnetoresistance, and magnetic anisotropy in bilayer Ni$_{81}$Fe$_{19}$-5d iridium oxide, IrO$_2$. While all the IrO$_2$ and Pt control samples exhibit large dampinglike-SOT generation stemming from the efficient charge to spin current conversion, the magnitude of the SOT is larger in the IrO$_2$ (Pt)-bottom sample than in the IrO$_2$ (Pt)-top one. The fieldlike-SOT has even more significant stack order effect, resulting in an opposite sign in the IrO$_2$ samples in contrast to the same sign in the Pt samples. Furthermore, we observe that the magnetic anisotropy energy density and the anomalous Hall effect are increased in the IrO$_2$ (Pt)-bottom sample, suggesting enhanced interfacial perpendicular magnetic anisotropy. Our findings highlight the significant influence of the stack order on spin transport and magnetotransport properties of Ir oxide/ferromagnet systems, providing useful information on design of SOT devices including 5d transition-metal oxides.

The 5d transition-metal oxides have a unique electronic structure dominated by strong spin-orbit coupling and hence they can be an intriguing platform to explore spin-current physics. Here, we report on room-temperature generation of spin-orbit torque (SOT) from a conductive 5d iridium oxide, IrO2. By measuring second-harmonic Hall resistance of Ni81Fe19/IrO2 bilayers, we find both dampinglike and fieldlike SOTs. The former is larger than the latter, enabling easier control of magnetization. We also observe that the dampinglike SOT efficiency has a significant dependence on IrO2 thickness, which is well described by the drift-diffusion model based on the bulk spin Hall effect. We deduce the effective spin Hall angle of +0.093 +- 0.003 and the spin-diffusion length of 1.7 +- 0.2 nm. By comparison with control samples Pt and Ir, we show that the effective spin Hall angle of IrO2 is comparable to that of Pt and seven times higher than that of Ir. The fieldlike SOT efficiency has a negative sign without appreciable dependence on the thickness, in contrast to the dampinglike SOT. This suggests that the fieldlike SOT likely stems from the interface. These experimental findings suggest that the uniqueness of the electronic structure of 5d transition-metal oxides is crucial for highly efficient charge to spin-current conversion.

Ground-state phase diagrams and magnetization curves of a spin-1 Heisenberg diamond cluster with two different coupling constants and uniaxial single-ion anisotropy are investigated in a presence of the external magnetic field with the help of exact diagonalization methods. It is shown that the spin-1 Heisenberg diamond cluster exhibits several remarkable quantum ground states, which are manifested in zero- and low-temperature magnetization curves as intermediate plateaus at one-quarter, one-half and three-quarters of the saturation magnetization. It is found that the width of the fractional magnetization plateaus depends basically on a relative strength of the coupling constants as well as uniaxial single-ion anisotropy, which may substantially shrink or even cause full breakdown of some intermediate magnetization plateaus. It is evidenced that a relatively weak uniaxial single-ion anisotropy of the easy-axis type considerably improves a theoretical fit of low-temperature magnetization curves of the tetranuclear nickel complex [Ni4(CO3)2(aetpy)8](ClO4)4 in a low-field region without spoiling the previous fit based on the fully isotropic Heisenberg model in a high-field region., Comment: 4 pages, 4 figures, presented at Physics of magnetism conference

Magnetic and magnetocaloric properties of a spin-1 Heisenberg diamond cluster with two different coupling constants are investigated with the help of an exact diagonalization based on the Kambe's method, which employs a local conservation of composite spins formed by spin-1 entities located in opposite corners of a diamond spin cluster. It is shown that the spin-1 Heisenberg diamond cluster exhibits several intriguing quantum ground states, which are manifested in low-temperature magnetization curves as intermediate plateaus at 1/4, 1/2 and 3/4 of the saturation magnetization. Besides, the spin-1 Heisenberg diamond cluster may also exhibit an enhanced magnetocaloric effect, which may be relevant for a low-temperature refrigeration achieved through the adiabatic demagnetization. It is evidenced that the spin-1 Heisenberg diamond cluster with the antiferromagnetic coupling constants J1/kB = 41.4 K and J2/kB = 9.2 K satisfactorily reproduces a low-temperature magnetization curve recorded for the tetranuclear nickel complex [Ni4(CO3)2(aetpy)8](ClO4)4 (aetpy = 2-aminoethyl-pyridine) including a size and position of intermediate plateaus detected at 1/2 and 3/4 of the saturation magnetization. A microscopic nature of fractional magnetization plateaus observed experimentally is clarified and interpreted in terms of valence-bond crystal with either a single or double valence bond. It is suggested that this frustrated magnetic molecule can provide a prospective cryogenic coolant with the maximal isothermal entropy change - Delta S = 10.6 J/(K.kg) in a temperature range below 2.3 K., Comment: 17 pages, 10 figures

A very large negative magnetoresistance (LNMR) is observed in the insulating regime of the antiferromagnet BaMn$_2$Bi$_2$ when a magnetic field is applied perpendicular to the direction of the sublattice magnetization. High perpendicular magnetic field eventually suppresses the insulating behavior and allows BaMn$_2$Bi$_2$ to re-enter a metallic state. This effect is seemingly unrelated to any field induced magnetic phase transition, as measurements of magnetic susceptibility and specific heat did not find any anomaly as a function of magnetic fields at temperatures above $2\,\mathrm{K}$. The LNMR appears in both current-in-plane and current-out-of-plane settings, and Hall effects suggest that its origin lies in an extreme sensitivity of conduction processes of holelike carriers to the infinitesimal field-induced canting of the sublattice magnetization. The LNMR-induced metallic state may thus be associated with the breaking of the antiferromagnetic parity-time symmetry by perpendicular magnetic fields and/or the intricate multi-orbital electronic structure of BaMn$_2$Bi$_2$.

A high-intensity proton beam exposure with 181 MeV energy has been conducted at Brookhaven Linac Isotope Producer facility on various material specimens for accelerator targetry applications, including titanium alloys as a beam window material. The radiation damage level of the analyzed capsule was 0.25 dpa at beam center region with an irradiation temperature around 120 degree C. Tensile tests showed increased hardness and a large decrease in ductility for the dual alpha+beta-phase Ti-6Al-4V Grade-5 and Grade-23 extra low interstitial alloys, with the near alpha-phase Ti-3Al-2.5V Grade-9 alloy still exhibiting uniform elongation of a few % after irradiation. Transmission Electron Microscope analyses on Ti-6Al-4V indicated clear evidence of a high-density of defect clusters with size less than 2 nm in each alpha-phase grain. The beta-phase grains did not contain any visible defects such as loops or black dots, while the diffraction patterns clearly indicated omega-phase precipitation in an advanced formation stage. The radiation-induced omega-phase transformation in the beta-phase could lead to greater loss of ductility in Ti-6Al-4V alloys in comparison with Ti-3Al-2.5V alloy with less beta-phase., Comment: 23 pages, 9 figures, In Press

We report the discovery of a novel giant magnetoresistance (GMR) phenomenon in a family of BaMn$_{2}$Pn$_{2}$ antiferromagnets (Pn stands for P, As, Sb, and Bi) with a parity-time symmetry. The resistivities of these materials are reduced by $60$ times in magnetic fields ($\vec{H}$'s), thus yielding the GMR of about $-98\%$. The GMR changes systematically along with the Pn elements, hinting that its origin is the spin orbit coupling (SOC) and/or $d$-$p$ orbital hybridization. A positive MR component emerging on top of the negative GMR at low temperatures suggests an orbital-sensitive magnetotransport as $\vec{H}$ suppresses the conduction of the electron-like carriers in the $d$-like band but enhances those of hole-like ones in the $d$-$p$ hybridized band. The anisotropy of the GMR reveals that the electrical conductivity is extremely sensitive to the minute changes in the direction of the antiferromagnetic moments induced by the parity-time breaking $\vec{H}$, which seems to be associated with a magnetoelectric effect in the dynamic regime of conduction electrons. We attribute the observed GMR to the non-trivial low energy band of BMPn's, which is governed by the parity-time symmetry and an magnetic hexadecapole ordering., Comment: 5 figures

We report on the experimental results of magnetic susceptibility, specific heat, electron spin resonance (ESR), and high-field magnetization measurements on a polycrystalline sample of the spin-$1/2$ distorted honeycomb-lattice antiferromagnet Cu$_2$(pymca)$_3$(ClO$_4$). Magnetic susceptibility shows a broad peak at about 25~K, which is typical of a low dimensional antiferromagnet, and no long range magnetic order is observed down to 0.6~K in the specific heat measurements. Magnetization curve up to 70~T at 1.4~K shows triple stepwise jumps. Assuming three different exchange bonds $J_{\rm A}$, $J_{\rm B}$ and $J_{\rm C}$ from the structure, the calculated magnetization curve reproduces the observed one when $J_{\rm A}/k_{\rm B} = 43.7~{\rm K}$, $J_{\rm B}/J_{\rm A} = 1$ and $J_{\rm C}/J_{\rm A} = 0.2$ except the magnetization near 70~T, where the observed magnetization indicates another step while the calculated magnetization becomes saturated. The relationship between magnetization plateaus and exchange bonds is discussed based on the numerical calculations., Comment: 5 pages, 5 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

Structure with orbital degeneracy is unstable toward spontaneous distortion. Such orbital correlation usually has a much higher energy scale than spins, and therefore, magnetic transition takes place at a much lower temperature, almost independently from orbital ordering. However, when the energy scales of orbitals and spins meet, there is a possibility of spin-orbital entanglement that would stabilize novel ground state such as spin-orbital liquid and random singlet state. Here we review on such a novel spin-orbital magnetism found in the hexagonal perovskite oxide Ba$_3$CuSb$_2$O$_9$, which hosts a self-organized honeycomblike short-range order of a strong Jahn-Teller ion Cu$^{2+}$. Comprehensive structural and magnetic measurements have revealed that the system has neither magnetic nor Jahn-Teller transition down to the lowest temperatures, and Cu spins and orbitals retain the hexagonal symmetry and paramagnetic state. Various macroscopic and microscopic measurements all indicate that spins and orbitals remain fluctuating down to low temperatures without freezing, forming a spin-orbital entangled liquid state., Comment: 33 pages, 17 figures, 1 table, to appear in Journal of Physics: Condensed Matter (topical review)

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

We report experimental and theoretical evidence that Rb$_2$Cu$_2$Mo$_3$O$_{12}$ has a nonmagnetic tetramer ground state of a two-leg ladder comprising antiferromagnetically coupled frustrated spin-$1/2$ chains and exhibits a Haldane spin gap of emergent spin-1 pairs. Three spin excitations split from the spin-1 triplet by a Dzyaloshinskii-Moriya interaction are identified in inelastic neutron-scattering and electron spin resonance spectra. A tiny magnetic field generates ferroelectricity without closing the spin gap, indicating a novel class of ferroelectricity induced by a vector spin chirality order., Comment: main text (6 pages, 5 figures) + supplemental material (10 pages, 8 figures), to appear in Phys. Rev. B (R)

We successfully synthesize single crystals of the verdazyl radical $\alpha$-2,3,5-Cl$_3$-V. $Ab$ $initio$ molecular orbital calculations indicate that the two dominant antiferromagnetic interactions, $J_{\rm{1}}$ and $J_{\rm{2}}$ ($\alpha =J_{\rm{2}}/J_{\rm{1}}\simeq 0.56$), form an $S$ = 1/2 distorted square lattice. We explain the magnetic properties based on the $S$ = 1/2 square lattice Heisenberg antiferromagnet using the quantum Monte Carlo method, and examine the effects of the lattice distortion and the interplane interaction contribution. In the low-temperature regions below 6.4 K, we observe anisotropic magnetic behavior accompanied by a phase transition to a magnetically ordered state. The electron spin resonance signals exhibit anisotropic behavior in the temperature dependence of the resonance field and the linewidth. We explain the frequency dependence of the resonance fields in the ordered phase using a mean-field approximation with out-of-plane easy-axis anisotropy, which causes a spin-flop phase transition at approximately 0.4 T for the field perpendicular to the plane. Furthermore, the anisotropic dipole field provides supporting information regarding the presence of the easy-axis anisotropy. These results demonstrate that the lattice distortion, anisotropy, and interplane interaction of this model are sufficiently small that they do not affect the intrinsic behavior of the $S$ = 1 / 2 square lattice Heisenberg antiferromagnet., Comment: 12 pages, 9 figures

Magnetic structure of the multiferroic Ca$_{2}$CoSi$_{2}$O$_{7}$ was determined by neutron diffraction techniques. Combination of the polycrystalline and single-crystal samples experiments revealed a collinear antiferromagnetic structure with the easy axis along $<$100$>$ directions. The dielectric state was discussed in the framework of the spin-dependent $d$-$p$ hybridization mechanism, leading to the realization of the antiferroelectric structure. The origin of the magnetic anisotropy was discussed in comparison with the isostructural Ba$_{2}$CoGe$_{2}$O$_{7}$., Comment: 5 pages, 5 figures

Exotic spin-multipolar ordering in spin transition metal insulators has so far eluded unambiguous experimental observation. A less studied, but perhaps more feasible fingerprint of multipole character emerges in the excitation spectrum in the form of quadrupolar transitions. Such multipolar excitations are desirable as they can be manipulated with the use of light or electric field and can be captured by means of conventional experimental techniques. Here we study single crystals of multiferroic Sr$_2$CoGe$_2$O$_7$, and show that due to its nearly isotropic nature a purely quadrupolar bimagnon mode appears in the electron spin resonance (ESR) spectra. This non-magnetic spin-excitation couples to the electric field of the light and becomes observable for a specific experimental configuration, in full agreement with a theoretical analysis of the selection rules., Comment: 19 pages, 13 figures, , accepted for publication in Phys. Rev. B

We have discovered a novel candidate for a spin liquid state in a ruthenium oxide composed of dimers of $S = $ 3/2 spins of Ru$^{5+}$,Ba$_3$ZnRu$_2$O$_9$. This compound lacks a long range order down to 37 mK, which is a temperature 5000-times lower than the magnetic interaction scale of around 200 K. Partial substitution for Zn can continuously vary the magnetic ground state from an antiferromagnetic order to a spin-gapped state through the liquid state. This indicates that the spin-liquid state emerges from a delicate balance of inter- and intra-dimer interactions, and the spin state of the dimer plays a vital role. This unique feature should realize a new type of quantum magnetism., Comment: 5 pages, 4 figures

Magnetoelectric properties are studied by a combined experimental and theoretical study of a quasi-two-dimensional material composed of square cupolas, Ba(TiO)Cu$_4$(PO$_4$)$_4$. The magnetization is measured up to above the saturation field, and several anomalies are observed depending on the field directions. We propose a $S$=1/2 spin model with Dzyaloshinskii-Moriya interactions, which well reproduces the full magnetization curves. Elaborating the phase diagram of the model, we show that the anomalies are explained by magnetoelectric phase transitions. Our theory also accounts for the scaling of the dielectric anomaly observed in experiments. The results elucidate the crucial role of the in-plane component of Dzyaloshinskii-Moriya interactions, which is induced by the noncoplanar buckling of square cupola. We also predict a `hidden' phase and another magnetoelectric response both of which appear in nonzero magnetic field., Comment: 5 pages, 5 figures

A compound with very weakly interacting chains, MnCl$_3$(bpy), has attracted a great deal of attention as a possible $S=2$ Haldane chain. However, long-range magnetic order of the chains prevents the Haldane gap from developing below 11.5~K. Based on a four-sublattice model, a description of the antiferromagnetic resonance (AFMR) spectrum up to frequencies of 1.5~THz and magnetic fields up to 50~T indicates that the interchain coupling is indeed quite small but that the Dzaloshinskii-Moriya interaction produced by broken inversion symmetry is substantial (0.12~meV). In addition, the antiferromagnetic, nearest-neighbor interaction within each chain (3.3~meV) is significantly stronger than previously reported. The excitation spectrum of this $S=2$ compound is well-described by a $1/S$ expansion about the classical limit., Comment: 4 figures