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We performed inelastic neutron scattering experiments on single-crystal samples of the honeycomb lattice magnet, ilmenite NiTiO3. Below the Neel temperature of 22 K, spin wave excitations with a band energy of 3.7 meV were observed. The neutron energy spectra were well-reproduced by modeling the system as a ferromagnetic honeycomb lattice with antiferromagnetic interlayer coupling, using linear spin wave theory. Similar to another ilmenite CoTiO3, a crossing structure was observed at the K point, suggesting the resence of Dirac magnons in NiTiO3. Further calculations suggested the formation of Dirac nodal line.

Altermagnetism is a newly discovered magnetic class named after the alternating spin polarizations in both real and reciprocal spaces. Like the spin-splitting of electronic bands, the magnon bands in altermagnets are predicted to exhibit alternating chiral splitting. In this work, by performing inelastic neutron scattering on $\alpha$-MnTe, we directly verified the chiral splitting in altermagnetic magnon dispersions. The lifted degeneracy of chirality is further explained by a symmetric-exchange origin. In addition, the $g$-wave magnetism was identified in MnTe., Comment: 6 pages, 3 figures. To appear in Phys. Rev. Lett. This is the initial manuscript that was submitted to Phys. Rev. Lett

We performed inelastic neutron scattering experiments on single crystal samples of a linear magnetoelectric material Mn$_{3}$Ta$_{2}$O$_{8}$, which exhibits a collinear antiferromagnetic order, to reveal the spin dynamics. Numerous modes observed in the neutron spectra were reasonably reproduced by linear spin-wave theory on the basis of the spin Hamiltonian including eight Heisenberg interactions and an easy-plane type single-ion anisotropy. The presence of strong frustration was found in the identified spin Hamiltonian., Comment: 8 pages, 4 figures

A new multiplex-type inelastic neutron scattering spectrometer, HOrizontally Defocusing Analyzer Concurrent data Acquisition spectrometer (HODACA), was recently developed and built at the C1-1 cold neutron beam port in JRR-3. The spectrometer is suitable for dynamics measurements in the energy range of $-1$ meV $\lesssim \hbar \omega \lesssim$ 7 meV, catering to a broad array of research fields in physics and material science. HODACA combines 24 detectors and 132 pieces of analyzer crystals and has an estimated measurement efficiency that is 70 times greater than the existing conventional triple-axis spectrometer at the C1-1 beam port. The concept, design, specification, and results of commissioning experiments are described., Comment: 11 pages, 16 figures

This paper reports the first experimental observation of phonons and their softening on single crystalline LaPt$_2$Si$_2$ via inelastic neutron scattering. From the temperature dependence of the phonon frequency in close proximity to the charge-density wave (CDW) $q$-vector, we obtain a CDW transition temperature of T$_{CDW}$ = 230 K and a critical exponent $\beta$ = 0.28 $\pm$ 0.03. This value is suggestive of a non-conventional critical behavior for the CDW phase transition in LaPt$_2$Si$_2$, compatible with a scenario of CDW discommensuration (DC). The DC would be caused by the existence of two CDWs in this material, propagating separately in the non equivalent (Si1-Pt2-Si1) and (Pt1-Si2-Pt1) layers respectively, with transition temperatures T$_{CDW-1}$ = 230 K and T$_{CDW-2}$ = 110 K. A strong $q$-dependence of the electron-phonon coupling has been identified as the driving mechanism for the CDW transition at T$_{CDW-1}$ = 230 K while a CDW with 3-dimensional character, and Fermi surface quasi-nesting as a driving mechanism, is suggested for the transition at T$_{CDW-2}$ = 110 K. Our results clarify some aspects of the CDW transition in LaPt$_2$Si$_2$, which have been so far misinterpreted by both theoretical predictions and experimental observations, and give direct insight into its actual temperature dependence.

We performed inelastic neutron scattering (INS) experiments to measure spin dynamics on a polycrystalline sample of a spin tube candidate CsCrF$_{4}$. The compound exhibits a successive phase transition from a paramagnetic phase through an intermediate temperature (IT) phase of a 120$^{\circ}$ structure to a low temperature (LT) phase of another 120$^{\circ}$ structure. Elaborate comparison between observed and calculated neutron spectra in LT phase reveals that the spin Hamiltonian is identified as antiferromagnetic spin tubes including perturbative terms of intertube interaction, Dzyaloshinskii-Moriya interaction, and single ion anisotropy. A phase diagram for the ground state is classically calculated. A set of parameters in the spin Hamiltonian obtained from the INS spectra measured in LT phase is quite close to a boundary to the phase of the 120$^{\circ}$ structure of IT phase. The INS spectra measured in IT phase is, surprisingly, the same as those in LT phase in the level of powder averaged spectra, even though the magnetic structures in IT and LT phases are different. Identical dynamical structures compatible with two different static structures are observed. No difference in the observed spectra indicates no change of the spin Hamiltonian with the temperature, suggesting that the origin of the successive phase transition being order-by-disorder mechanism.

We performed an inelastic neutron scattering experiment on a polycrystalline sample of a helimagnet Ni$_2$InSbO$_6$ to construct the spin Hamiltonian. Well-defined spin-wave excitation with a band energy of 20 meV was observed below $T_{N} = 76$ K. Using the linear spin-wave theory, the spectrum was reasonably reproduced with honeycomb spin layers coupled along the stacking axis (the $c$ axis). The proposed spin model reproduces the soliton lattice induced by a magnetic field applied perpendicular to the $c$ axis., Comment: 8 pages, 5 figures

A triplon refers to a fictitious particle that carries angular momentum $S = 1$ corresponding to the elementary excitation in a broad class of quantum dimerized spin systems. Such systems without magnetic order have long been studied as a testing ground for quantum properties of spins. Although triplons have been found to play a central role in thermal and magnetic properties in dimerized magnets with singlet correlation, a spin angular momentum flow carried by triplons, a triplon current, has not been detected yet. Here we report spin Seebeck effects induced by a triplon current: triplon spin Seebeck effect, using a spin-Peierls system CuGeO$_3$. The result shows that the heating-driven triplon transport induces spin current whose sign is positive, opposite to the spin-wave cases in magnets. The triplon spin Seebeck effect persists far below the spin-Peierls transition temperature, being consistent with a theoretical calculation for triplon spin Seebeck effects.

The kagome lattice is a fertile platform to explore topological excitations with both Fermi-Dirac and Bose-Einstein statistics. While relativistic Dirac Fermions and flat-bands have been discovered in the electronic structure of kagome metals, the spin excitations have received less attention. Here we report inelastic neutron scattering studies of the prototypical kagome magnetic metal FeSn. The spectra display well-defined spin waves extending up to 120 meV. Above this energy, the spin waves become progressively broadened, reflecting interactions with the Stoner continuum. Using linear spin wave theory, we determine an effective spin Hamiltonian that reproduces the measured dispersion. This analysis indicates that the Dirac magnon at the K-point remarkably occurs on the brink of a region where well-defined spin waves become unobservable. Our results emphasize the influential role of itinerant carriers on the topological spin excitations of metallic kagome magnets., Comment: 6 pages, 4 figures

Dimensionality is a critical factor in determining the properties of solids and is an apparent built-in character of the crystal structure. However, it can be an emergent and tunable property in geometrically frustrated spin systems. Here, we study the spin dynamics of the tetrahedral cluster antiferromagnet, pharmacosiderite, via muon spin resonance and neutron scattering. We find that the spin correlation exhibits a two-dimensional characteristic despite the isotropic connectivity of tetrahedral clusters made of spin 5/2 Fe3+ ions in the three-dimensional cubic crystal, which we ascribe to two-dimensionalisation by geometrical frustration based on spin wave calculations. Moreover, we suggest that even one-dimensionalisation occurs in the decoupled layers, generating low-energy and one-dimensional excitation modes, causing large spin fluctuation in the classical spin system. Pharmacosiderite facilitates studying the emergence of low-dimensionality and manipulating anisotropic responses arising from the dimensionality using an external magnetic field., Comment: 22 pages, 22 figures

We measured the temperature dependences of the static magnetization and the spin excitation in a square-lattice multiferroics Ba$_2$MnGe$_2$O$_7$. An anisotropy gap of the observed low energy mode is scaled by electric polarization rather than a power of sublattice moment. Spin nematic interaction in effective spin Hamiltonian, which is equivalent to interaction of electric polarization, is responsible for the easy-axis anisotropy. The nontrivial behavior of the anisotropy gap can be rationalized as change of the hybridized $d$-$p$ orbital with temperature, leading to the temperature dependence of the spin nematic interaction., Comment: Main article: 12 pages, 4 figures. Supplementary material: 12 pages, 7 figures

We have investigated the low-temperature magnetism of sodium superoxide (NaO$_{2}$), in which spin, orbital, and lattice degrees of freedom are closely entangled. The magnetic susceptibility shows anomalies at $T_{1}=220$ K and $T_{2}=190$ K, which correspond well to the structural phase transition temperatures, and a sudden decrease below $T_{3}=34$ K. At 4.2 K, the magnetization shows a clear stepwise anomaly around 30 T with a large hysteresis. In addition, the muon spin relaxation experiments indicate no magnetic phase transition down to $T=0.3$ K. The inelastic neutron scattering spectrum exhibits magnetic excitation with a finite energy gap. These results confirm that the ground state of NaO$_{2}$ is a spin-singlet state. To understand this ground state in NaO$_{2}$, we performed Raman scattering experiments. All the Raman-active libration modes expected for the marcasite phase below $T_{2}$ are observed. Furthermore, we find that several new peaks appear below $T_{3}$. This directly evidences the low crystal symmetry, namely, the presence of the phase transition at $T_{3}$. We conclude the singlet-ground state of NaO$_{2}$ due to the spin-Peierls instability., Comment: 6 pages, 3 figures

Finding new materials with antiferromagnetic (AFM) Kitaev interaction is an urgent issue to broaden and enrich the quantum magnetism research significantly. By carrying out inelastic neutron scattering experiments and subsequent analysis, we conclude that Na$_3$Co$_2$SbO$_6$ and Na$_2$Co$_2$TeO$_6$ are new honeycomb cobalt-based AFM Kitaev systems. The spin-orbit excitons at 20-28~meV in both compounds strongly supports the idea that Co$^{2+}$ ions of both compounds have a spin-orbital entangled $J_\rm{eff}=1/2$ state. Furthermore, we found that a generalized Kitaev-Heisenberg Hamiltonian can well describe the spin-wave excitations of both compounds with additional 3rd nearest-neighbor interaction. Our best-fit parameters show large AFM Kitaev terms and off-diagonal symmetric anisotropy terms of a similar magnitude in both compounds. We should stress that our parameters' optimized magnetic structures are consistent with the magnetic structures reported from neutron diffraction studies. Moreover, there is also the magnon-damping effect at the higher energy part of the spin waves, as usually observed in other Kitaev magnets. We demonstrate that Na$_3$Co$_2$SbO$_6$ and Na$_2$Co$_2$TeO$_6$ are the first experimental realization of AFM Kitaev magnets based on the systematic studies of the spin waves and analysis., Comment: 28 pages, 10 figures, Journal of Physics: Condensed Matter

Spin-orbit coupled honeycomb magnets with the Kitaev interaction have received a lot of attention due to their potential of hosting exotic quantum states including quantum spin liquids. Thus far, the most studied Kitaev systems are 4d/5d-based honeycomb magnets. Recent theoretical studies predicted that 3d-based honeycomb magnets, including Na2Co2TeO6 (NCTO), could also be a potential Kitaev system. Here, we have used a combination of heat capacity, magnetization, electron spin resonance measurements alongside inelastic neutron scattering (INS) to study NCTO's quantum magnetism, and we have found a field-induced spin disordered state in an applied magnetic field range of 7.5 T < B (vertical to b-axis) < 10.5 T. The INS spectra were also simulated to tentatively extract the exchange interactions. As a 3d-magnet with a field-induced disordered state on an effective spin-1/2 honeycomb lattice, NCTO expands the Kitaev model to 3d compounds, promoting further interests on the spin-orbital effect in quantum magnets., Comment: 19 pages and 5 figures for main text. 16 pages and 6 figures for Supplemental Material

The effect of chemical substitution on the ground state of the geometrically frustrated antiferromagnet CsCrF$_4$ has been investigated through a neutron powder diffraction experiment. Magnetic Fe-substituted CsCr$_{0.94}$Fe$_{0.06}$F$_{4}$ and nonmagnetic Al-substituted CsCr$_{0.98}$Al$_{0.02}$F$_{4}$ samples are measured, and magnetic Bragg peaks are clearly observed in both samples. Magnetic structure analysis revealed a 120$^{\circ}$ structure having a magnetic propagation vector $\mathbf{k}_{\rm mag}=(0,0,1/2)$ in CsCr$_{0.94}$Fe$_{0.06}$F$_{4}$. For CsCr$_{0.98}$Al$_{0.02}$F$_{4}$, a quasi-120$^{\circ}$ structure having $\mathbf{k}_{\rm mag}=(1/2,0,1/2)$ is formed. It is notable that the identified magnetic structure in CsCr$_{0.94}$Fe$_{0.06}$F$_{4}$ belongs to a different phase of ground states from those in CsCr$_{0.98}$Al$_{0.02}$F$_{4}$ and the parent CsCrF$_{4}$. These results suggest that the Fe-substitution strongly influences the ground state of CsCrF$_{4}$.

The magnetic excitations in CoPS$_3$, a two-dimensional van der Waals (vdW) antiferromagnet with spin $S=3/2$ on a honeycomb lattice, has been measured using powder inelastic neutron scattering. Clear dispersive spin waves are observed with a large spin gap of ~13 meV. The magnon spectra were fitted using an $XXZ$-type $J_1-J_2-J_3$ Heisenberg Hamiltonian with a single-ion anisotropy assuming no magnetic exchange between the honeycomb layers. The best-fit parameters show ferromagnetic exchange $J_1=-2.08$ meV and $J_2=-0.26$ meV for the nearest and second-nearest neighbors and a sizeable antiferromagnetic exchange $J_3=4.21$ meV for the third-nearest neighbor with the strong easy-axis anisotropy $K=-2.06$ meV. The suitable fitting could only be achieved by the anisotropic $XXZ$-type Hamiltonian, in which the exchange interaction for the out-of-plane component is smaller than that for the in-plane one by a ratio $\alpha=J_z/J_x=0.6$. Moreover, the absence of spin-orbit exciton around 30 meV indicates that Co$^{2+}$ ions in CoPS$_3$ have a $S=3/2$ state rather than a spin-orbital entangled $J_\rm{eff}=1/2$ ground state. Our result directly shows that CoPS$_3$ is an experimental realization of the $XXZ$ model with a honeycomb lattice in 2D vdW magnets., Comment: 17 pages, 5 figures

We performed inelastic neutron scattering measurements on a polycrystalline sample of a classical kagome antiferromagnet NaBa$_{2}$Mn$_{3}$F$_{11}$ to investigate the possibility of a dispersionless zero-energy excitation associated with rotation of spins along the chains. The observed spectra indeed exhibit such an excitation with strong intensity at low energy, as well as dispersive excitations with weak intensity at high energy. Combining the measurements with calculations from linear spin-wave theory reveals that NaBa$_{2}$Mn$_{3}$F$_{11}$ is a good realization of the classical kagome antiferromagnet which exhibits a dispersionless mode lifted by the magnetic dipole-dipole interaction.

Chemical doping is one of the most important strategies for tuning electrical properties of semiconductors, particularly thermoelectric materials. Generally, the main role of chemical doping lies in optimizing the carrier concentration, but there can potentially be other important effects. Here, we show that chemical doping plays multiple roles for both electron and phonon transport properties in half-Heusler thermoelectric materials. With ZrNiSn-based half-Heusler materials as an example, we use high-quality single and polycrystalline crystals, various probes, including electrical transport measurements, inelastic neutron scattering measurement, and first-principles calculations, to investigate the underlying electron-phonon interaction. We find that chemical doping brings strong screening effects to ionized impurities, grain boundary, and polar optical phonon scattering, but has negligible influence on lattice thermal conductivity. Furthermore, it is possible to establish a carrier scattering phase diagram, which can be used to select reasonable strategies for optimization of the thermoelectric performance., Comment: 21 pages, 5 figures

Investigating exotic magnetic materials with spintronic techniques is effective at advancing magnetism as well as spintronics. In this work, we report unusual field-induced suppression of the spin-Seebeck effect (SSE) in a quasi one-dimensional frustrated spin-$\frac{1}{2}$ magnet LiCuVO$_4$, known to exhibit spin-nematic correlation in a wide range of external magnetic field $B$. The suppression takes place above $|B| > 2$ T in spite of the $B$-linear isothermal magnetization curves in the same $B$ range. The result can be attributed to the growth of the spin-nematic correlation while increasing $B$. The correlation stabilizes magnon pairs carrying spin-2, thereby suppressing the interfacial spin injection of SSE by preventing the spin-1 exchange between single magnons and conduction electrons at the interface. This interpretation is supported by integrating thermodynamic measurements and theoretical analysis on the SSE., Comment: accepted for publication in Phys. Rev. Lett

Investigation of materials that exhibit quantum phase transition provides valuable insights into fundamental problems in physics. We present neutron scattering under pressure in a triangular-lattice antiferromagnet which has a quantum disorder in the low-pressure phase and a noncollinear structure in the high-pressure phase. The neutron spectrum continuously evolves through the critical pressure; a single mode in the disordered state becomes soft with the pressure, and it splits into gapless and gapped modes in the ordered phase. Extended spin-wave theory reveals that the longitudinal and transverse fluctuations of spins are hybridized in the modes because of the noncollinearity, and novel magnetic excitations are formed. We report a new hybridization of the phase and amplitude fluctuations of the order parameter in a spontaneously symmetry-broken state., Comment: Supplementary material comes first and main text is followed. 12 pages, 3 figures and 1 table for supplementary material. 13 pages and 4 figures for main text

Low-energy incommensurate (IC) magnetic fluctuations in the multiband superconductor Sr$_2$RuO$_4$ is investigated by high-resolution inelastic neutron scattering measurements and random phase approximation (RPA) calculations. Below $T_\text{c}$, the substantial spin gap is observed at $\mathbf{Q}_\text{IC}=(0.3, 0.3, L)$ where the quasi-one-dimensional $\alpha$ and $\beta$ sheets consisting of the Fermi surfaces are in good nesting conditions. $L$ modulated intensity of the low-energy IC magnetic fluctuations and our RPA calculations indicate that the superconducting gaps regarding the $\alpha$ and $\beta$ sheets have the horizontal line nodes., Comment: 13 pages, 4 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 use inelastic neutron scattering to study the low-energy spin excitations of 112-type iron pnictide Ca$_{0.82}$La$_{0.18}$Fe$_{0.96}$Ni$_{0.04}$As$_{2}$ with bulk superconductivity below $T_c=22$ K. A two-dimensional spin resonance mode is found around $E=$ 11 meV, where the resonance energy is almost temperature independent and linearly scales with $T_c$ along with other iron-based superconductors. Polarized neutron analysis reveals the resonance is nearly isotropic in spin space without any $L$ modulations. Due to the unique monoclinic structure with additional zigzag arsenic chains, the As $4p$ orbitals contribute to a three-dimensional hole pocket around $\Gamma$ point and an extra electron pocket at $X$ point. Our results suggest that the energy and momentum distribution of spin resonance does not directly response to the $k_z$ dependence of fermiology, and the spin resonance intrinsically is a spin-1 mode from singlet-triplet excitations of the Cooper pairs in the case of weak spin-orbital coupling., Comment: 9 pages, 8 figures, with supplementary materials

We have studied the ground state of the classical Kagome antiferromagnet NaBa$_{2}$Mn$_{3}$F$_{11}$. Strong magnetic Bragg peaks observed in the $d$-spacing shorter than 6.0 \AA\ were indexed by the propagation vectors of $\boldsymbol{k}_{0} = (0,0,0)$. Additional peaks with weak intensities in the range of the $d$-spacing longer than 8.0 \AA\ were indexed by the incommensurate vectors of $\boldsymbol{k}_{1}=(0.3209(2),0.3209(2),0)$ and $\boldsymbol{k}_{2}=(0.3338(4),0.3338(4),0)$. Magnetic structure analysis exhibits that the 120$^{\circ}$ structure with the {\it tail-chase} geometry having $\boldsymbol{k}_0$ is modulated by the incommensurate vectors. The classical calculation of the Kagome Heisenberg antiferromagnet having the antiferromagnetic 2nd-neighbor interaction, the ground state of which is degenerated 120$^{\circ}$ structures with $\boldsymbol{k}_0$, reveals that the magnetic dipole-dipole (MDD) interaction including up to the 4th neighbor terms selects the tail-chase structure. The observed modulation of the tail-chase structure is indicated to be due to a small perturbation such as the long-range MDD interaction or the interlayer interaction.

We developed control and visualization programs, YUI and HANA, for High- Resolution Chopper spectrometer (HRC) installed at BL12 in MLF, J-PARC. YUI is a comprehensive program to control DAQ-middleware, the accessories, and sample environment devices. HANA is a program for the data transformation and visualization of inelastic neutron scattering spectra. In this paper, we describe the basic system structures and unique functions of these programs from the viewpoint of users., Comment: 9 pages, 4 figures

We carried out inelastic neutron scattering experiments on a buckled honeycomb lattice antiferromagnet Ba$_{2}$NiTeO$_{6}$ exhibiting a stripe structure at a low temperature. Magnetic excitations are observed in the energy range of $\hbar \omega \lesssim 10$ meV having an anisotropy gap of 2 meV at 2 K. We perform spin-wave calculations to identify the spin model. The obtained microscopic parameters are consistent with the location of the stripe structure in the classical phase diagram. Furthermore, the Weiss temperature independently estimated from a bulk magnetic susceptibility is consistent with the microscopic parameters. The results reveal that a competition between the NN and NNN interactions that together with a relatively large single ion magnetic anisotropy stabilize the stripe magnetic structure., Comment: 6 pages, 5 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

Nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) of Cu have been measured in a coupled spin dimers and chains compound Cu2Fe2Ge4O13. Cu NQR has also been measured in an isostructural material Cu2Sc2Ge4O13 including only spin dimers. Comparison of the temperature dependence of the 63Cu nuclear spin-lattice relaxation rate between the two compounds reveals that the Fe chains in Cu2Fe2Ge4O13 do not change a spin gap energy of the Cu dimers from that in Cu2Sc2Ge4O13, contributing additionally to the relaxation rate at the Cu site. A modestly large internal field of 3.39 T was observed at the Cu site in the antiferromagnetic state of Cu2Fe2Ge4O13 at 4.2 K, which is partly because of quantum reduction of the ordered moment of a Cu atom. The internal field and the ordered moment of Cu are noncollinear due to large anisotropy of the hyperfine interaction at the Cu site. A model analysis of the internal field based on the fourfold planar coordination of Cu suggests that a 3d hole of the Cu2+ ion is mainly in the d(x2-y2) orbital state., Comment: 10 pages, 11 figures, replaced with the published version

We study field induced quantum phase in weakly-coupled ferromagnetic frustrated chain LiCuVO$_4$ by neutron diffraction technique. A new incommensurate magnetic peak is observed at $H \ge 8.5$ T. The field dependent propagation vector is identified with the spin density wave correlation in the theoretically predicted magnetic quadrupole order. Quantum fluctuation, geometrical frustration, and interchain interaction induce the exotic spin density wave long-range order in the insulating magnet.