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Neutron and x-ray diffraction experiments were performed on the ternary intermetallic compound YbNiSn, formerly categorized as a ferromagnetic Kondo compound. At zero field, an increase in scattering intensity was observed on top of allowed and forbidden nuclear reflections below Tc, breaking the reflection condition of the crystal symmetry Pnma. This indicates that the magnetic structure of YbNiSn is antiferromagnetic-type, rather than the previously proposed simple collinear ferromagnetic structure. Temperature dependence of the scattering intensity of the 011 reflection confirmed the magnetic ordering at 5.77(2) K. No incommensurate satellite reflection was observed at 2.5 K. By applying external magnetic field of 1 T along the a axis, the magnetic intensity at the nuclear-forbidden 001 position was suppressed, while a slight enhancement at the nuclear-allowed 002 position was observed. This suggests a spin-flip transition under the external magnetic field along the a axis in YbNiSn. The proposed magnetic structures at zero field and 1 T correspond to the magnetic space groups of Pn'm'a and Pnm'a', respectively. The piezomagnetic effect and the switch between the two magnetic space groups by the external stress, which could be detected by the anomalous Hall effect, are proposed.

Using small angle neutron scattering, we have investigated higher-order peaks in the skyrmion-lattice phase of Cu$_2$OSeO$_3$, in which two different skyrmion lattices, SkX1 and SkX2, are known to form. For each skyrmion-lattice phase, we observed two sets of symmetrically inequivalent peaks at the higher-order-reflection positions with the indices $(110)$ and $(200)$. Under the condition where the SkX1 and SkX2 coexist, we confirmed the absence of the scattering at $\mathbf{Q}$ positions combining reflections from the two phases, indicating a significantly weak double-scattering component. Detailed analysis of the peak profile, as well as the temperature and magnetic-field dependence of the peak intensity, also supports the intrinsic higher-order modulation rather than the parasitic double scattering. The two higher-order modulations show contrasting magnetic-field dependence; the former $(110)$ increases as the field is increased, whereas the latter $(200)$ decreases. This indicates that, in Cu$_2$OSeO$_3$, skyrmions are weakly distorted, and the distortion is field-dependent in a way that the dominant higher-order modulation switches from $(110)$ to $(200)$ under field. Monte Carlo simulations under sweeping external magnetic field qualitatively reproduce the observed magnetic-field dependence, and suggests that the higher-order modulations correspond to the superlattices of weak swirlings appearing in the middle of the original triangular-latticed skyrmions., Comment: 13 pages, 14 figures

Magnetic properties of the quasicrystal approximant Au$_{65}$Ga$_{21}$Tb$_{14}$ were investigated by the magnetization and the neutron diffraction experiments. The temperature dependences of the magnetic susceptibility and the magnetization curve indicate dominant ferromagnetic interactions, while the whirling antiferromagnetic order was found from the neutron diffraction experiments. In the antiferromagnetic phase, the magnetic moments are aligned almost perpendicular to a pseudo five-fold symmetry axis, which should correspond to the easy-axis direction of a Tb atom. The magnetic properties similar to those of Au$_{72}$Al$_{14}$Tb$_{14}$ in spite of the difference in the electron-per-atom ratio suggest the robustness of the easy-axis anisotropy against the chemical substitution of the nonmagnetic atoms., Comment: 6 pages, 3 figures, 2 tables

The ruthenium halide $\alpha$-RuCl$_{3}$ is a promising candidate for a Kitaev spin liquid. However, the microscopic model describing $\alpha$-RuCl$_{3}$ is still debated partly because of a lack of analogue materials for $\alpha$-RuCl$_{3}$, which prevents tracking of electronic properties as functions of controlled interaction parameters. Here, we report a successful synthesis of RuBr$_{3}$. The material RuBr$_{3}$~possesses BiI$_3$-type structure (space group: $R\overline{3}$) where Ru$^{3+}$ form an ideal honeycomb lattice. Although RuBr$_{3}$ has a negative Weiss temperature, it undergoes a zigzag antiferromagnetic transition at $T_\mathrm{N}=34$ K, as does $\alpha$-RuCl$_{3}$. Our analyses indicate that the Kitaev and non-Kitaev interactions can be modified in ruthenium trihalides by changing the ligand sites, which provides a new platform for exploring Kitaev spin liquids.

Magnetic properties of the pyrovanadate CaCoV$_2$O$_7$ have been studied by means of the bulk magnetization and neutron powder diffraction measurements. Magnetic susceptibility in the paramagnetic phase shows Curie-Weiss behavior with negative Weiss temperature $\Theta \simeq -22.5$ K, indicating dominant antiferromagnetic interactions. At $T_{\rm N} = 3.44$ K, CaCoV$_2$O$_7$ shows antiferromagnetic order, accompanied by a weak net ferromagnetic moment of $\sim 0.05$~$\mu_{\rm B}/{\rm Co}^{2+}$. Neutron powder diffraction confirms the formation of antiferromagnetic order below $T_{\rm N}$. It was further confirmed from the magnetic structure determination that the two Co$^{2+}$ ions in the adjacent edge-sharing octahedra have almost parallel (ferromagnetic) spin arrangement, indicative of a formation of a ferromagnetic spin dimer. The antiferromagnetic order is, in turn, stabilized by sizable inter-dimer antiferromagnetic interactions.

The magnetic susceptibility of the 1/1 approximants to icosahedral quasicrystals in a series of Cd85-xMgxTb15 (x = 5, 10, 15, 20) alloys was investigated in detail. The occurrence of antiferromagnetic to spin-glass-like transition was noticed by increasing Mg. Transmission electron microscopy analysis evidenced a correlation between the magnetic transition and suppression of the monoclinic superlattice ordering with respect to the orientation of the Cd4 tetrahedron at T > 100 K. The possible origins of this phenomenon were discussed in detail. The occurrence of the antiferromagnetic to spin-glass -like magnetic transition is associated with the combination of chemical disorder due to a randomized substitution of Cd with Mg and the orientational disorder of the Cd4 tetrahedra., Comment: 9 pages, 9 figures

A systematic investigation has been performed to elucidate effects of Rare-Earth (RE) type and local atomic configuration on magnetic properties of icosahedral quasicrystal (iQC) and their cubic approximants (2/1 and 1/1 ACs) in the ternary Cd-Mg-RE (RE = Gd, Tb, Dy, Ho, Er, and Tm) systems. At low temperatures, iQC and 2/1 ACs exhibit spin-glass-like freezing for RE = Gd, Tb, Dy, and Ho, while Er and Tm systems do not show freezing behaviour down to the base temperature ~ 2 K. The 1/1 ACs exhibit either spin-glass-like freezing or antiferromagnetic (AFM) ordering depending on their constituent Mg content. The Tf values show increasing trend from iQC to 2/1 and 1/1 ACs. In contrast, the absolute values of Weiss temperature for iQCs are larger than those in 2/1 and 1/1 ACs, indicating that the total AFM interactions between the neighboring spins are larger in aperiodic, rather than periodic systems. Competing spin interactions originating from the long-range Ruderman-Kittel-Kasuya-Yoshida mechanism along with chemical disorder of Cd/Mg ions presumably account for the observed spin-glass-like behavior in Cd-Mg-RE iQCs and ACs., Comment: 12 pages, 8 Figures, 2 Tables

We have investigated the effect of Ge-substitution to the magnetic ordering in the B20 itinerant chiral magnet MnSi prepared by melting and annealing under ambient pressure. From metallurgical survey, the solubility limit of Ge was found to be $x=0.144(5)$ with annealing temperature $T_\mathrm{an} = 1073$ K. Magnetization measurements on MnSi$_{1-x}$Ge$_x$ samples show that the helical ordering temperature $T_{\mathrm{c}}$ increases rapidly in the low-$x$ range, whereas it becomes saturated at higher concentration $x>~0.1$. The Ge substitution also increases both the saturation magnetization $M_\mathrm{s}$ and the critical field to the fully polarized state $H_\mathrm{c2}$. In contrast to the saturation behavior of $T_\mathrm{c}$, those parameters increase linearly up to the highest Ge concentration investigated. In the temperature-magnetic field phase diagram, we found enlargement of the skyrmion phase region for large $x$ samples. We, furthermore, observed the non-linear behavior of helical modulation vector $k$ as a function of Ge concentration, which can be described qualitatively using the mean field approximation., Comment: 9 pages, 10 figures

In an ideal classical pyrochlore antiferromagnet without perturbations, an infinite degeneracy at a ground state leads to absence of a magnetic order and spin-glass transition. Here we present Na$_3$Mn(CO$_3$)$_2$Cl as a new candidate compound where classical spins are coupled antiferromagnetically on the pyrochlore lattice, and report its structural and magnetic properties.The temperature dependences of the magnetic susceptibility and heat capacity, and the magnetization curve are consistent with those of an $S$ = 5/2 pyrochlore lattice antiferromagnet with nearest-neighbor interactions of 2 K. Neither an apparent signature of a spin-glass transition nor a magnetic order is detected in magnetization and heat capacity measurements, or powder neutron diffraction experiments. On the other hand, an antiferromagnetic short-range order from the nearest neighbors is evidenced by the $Q$-dependence of the diffuse scattering which develops around 0.85 \AA$^{-1}$. A high degeneracy near the ground state in Na$_3$Mn(CO$_3$)$_2$Cl is supported by the magnetic entropy estimated as almost 4 J K$^{-2}$ mol$^{-1}$ at 0.5 K., Comment: 9 pages, 7 figures, accepted to PRB

A tiny adiabatic-demagnetization refrigerator (T-ADR) has been developed for a commercial superconducting quantum interference device magnetometer [Magnetic Property Measurement System (MPMS) from Quantum Design]. The whole T-ADR system is fit in a cylindrical space of the diameter $8.5$ mm and the length $250$ mm, and can be inserted into the narrow sample tube of MPMS. A sorption pump is self-contained in T-ADR, and hence no complex gas handling system is necessary. With the single crystalline Gd$_3$Ga$_5$O$_{12}$ garnet ($\sim 2$ grams) used as a magnetic refrigerant, the routinely achievable lowest temperature is $\sim 0.56$ K. The lower detection limit for a magnetization anomaly is $\sim 1 \times 10^{-7}$ emu, estimated from fluctuation of the measured magnetization. The background level is $\sim 5 \times 10^{-5}$ emu below 2 K at $H = 100$ Oe, which is largely attributable to a contaminating paramagnetic signal from the magnetic refrigerant., Comment: 8 pages, 8 figures, accepted for publication in Rev. Sci. Inst

Small angle neutron inelastic scattering measurement has been performed to study the magnon dispersion relation in the field-induced-ferromagnetic phase of the noncentrosymmetric binary compound MnSi. For the magnons propagating parallel or anti-parallel to the external magnetic field, we experimentally confirmed that the dispersion relation is asymmetrically shifted along the magnetic field direction. This magnon dispersion shift is attributed to the relativistic Dzyaloshinskii-Moriya interaction, which is finite in noncentrosymmetric magnets, such as MnSi. The shift direction is found to be switchable by reversing the external magnetic field direction., Comment: 6 pages, 4 figures, accepted for publication in Phys. Rev. B

Small angle neutron scattering measurements have been performed to study the thermodynamic stability of skyrmion-lattice phases in Cu$_2$OSeO$_3$. We found that the two distinct skyrmion-lattice phases [SkX(1) and SkX(2) phases] can be stabilized through different thermal histories; by cooling from the paramagnetic phase under finite magnetic field, the SkX(2) phase is selected. On the other hand, the 30$^{\circ}$-rotated SkX(1) phase becomes dominant by heating the sample from the ordered conical phase under finite field. This difference in stabilization is surprisingly similar to the irreversibility observed in spin glasses. The zero-field cooling results in the co-existence of the two phases. It is further found that once one of the skyrmion-lattice phases is formed, it is hardly destabilized. This indicates unusual thermal stability of the two skyrmion-lattice phases originating from an unexpectedly large energy barrier between them., Comment: 9 pages, 10 figures

Mechanical alloying method has been employed to prepare the Ba-Fe-As-P precursors, necessary for the Ba-(As,P) flux growth of the single crystalline BaFe$_2$(As$_{1-x}$P$_x$)$_2$. By alloying constituent elementals mechanically, the Ba-(As,P) precursors are successfully formed at the room temperature within one hour, significantly reducing preparation time. Using the mechanically alloyed precursors, we have grown single crystals of BaFe$_2$(As$_{1-x}$P$_x$)$_2$ with the sizes up to 5~mm $\times$ 5~mm $\times$ 0.1~mm., Comment: 9 pages, 3 figures, 1 table

We performed magnetic susceptibility and neutron powder diffraction experiments on the ternary compound Pr5Ru3Al2. It belongs to the noncentrosymmetric and nonmirrorsymmetric cubic I213 space group. The previously reported ferromagnetic transition at 24 K was not detected in our improved quality samples. Instead, magnetic ordering was observed in the DC magnetic susceptibility at 3.8 K. Neutron powder diffraction further indicates that an incommensurate magnetic structure is established below 3.8 K, with the magnetic modulation vector (0.066, 0.066, 0.066) (r.l.u.). Using the magnetic representation analysis, we propose the block helical structure as a candidate for the incommensurate magnetic structure., Comment: 11 pages, 5 figures

Long-range non-collinear all-in/all-out magnetic order has been directly observed for the first time in real space in the pyrochlore Cd$_2$Os$_2$O$_7$ using resonant magnetic microdiffraction at the Os L$_3$ edge. Two different antiferromagnetic domains related by time-reversal symmetry could be distinguished and have been mapped within the same single crystal. The two types of domains are akin to magnetic twins and were expected - yet unobserved so far - in the all-in/all-out model. Even though the magnetic domains are antiferromagnetic, we show that their distribution can be controlled using a magnetic field-cooling procedure., Comment: Main text: 11 pages, 4 figures ; Supplementary materials: 9 pages, 5 figures

Structural phase transition accompanying with quadrupolar ordering in DyB4 with Shastry-Sutherland type geometrical frustration has been studied by X-ray diffraction. Previous study [D. Okuyama et al.: J. Phys. Soc. Jpn. 74 (2005) 2434.] using resonant X-ray scattering revealed short-range ordering of the Ozx-type quadrupolar moments and the c-plane component of the magnetic moments in addition to long-range ordering of the c-axis component of the magnetic moments. The present report focuses on the lattice distortion below the quadrupolar ordering temperature at TN2=12.7 K. The (0 0 l=integer) fundamental lattice reflection splits into four peaks along the h and k directions and the (h=even 0 0) reflection becomes broad along the l direction. This indicates that a structural transition from tetragonal to monoclinic takes place below TN2 together with the ordering of the quadrupolar moments., Comment: 3 pages, 4 figures, the Proceedings of ASR-WYP-2005

We have examined whether the Co ions crystallographically substitute on the Ti sites in rutile and anatase Ti_{1-x}$Co$_{x}$O$_{2-delta}$ thin films that exhibit room-temperature ferromagnetism. Intensities of the x-ray Bragg reflection from the films were measured around the $K$-absorption-edge of Co. If the Co ions randomly substitute on the Ti sites, the intensity should exhibit an anomaly due to the anomalous dispersion of the atomic scattering factor of Co. However, none of the anatase and rutile samples did exhibit an anomaly, unambiguously showing that the Co ions in Ti$_{1-x}$Co$_{x}$O$_{2-delta}$ are not exactly located at the Ti sites of TiO$_2$. The absence of the anomaly is probably caused by a significant deformation of the local structure around Co due to the oxygen vacancy. We have applied the same method to paramagnetic Zn$_{1-x}$Co$_{x}$O thin films and obtained direct evidence that the Co ions are indeed substituted on the Zn sites., Comment: 5 pages, 4 figures, accepted in PRB

We have observed geometrical frustration of quadrupolar and magnetic moments in dysprosium tetraboride, DyB4, where the rare-earth sites form a Shastry-Sutherland lattice. Resonant x-ray scattering at the LIII absorption edge of Dy was utilized. Analysis of the energy, polarization, temperature, and azimuthal-angle dependences of the E1 resonance of the (1 0 0) forbidden reflection show that the magnetic and quadrupolar components within the frustrated c plane have a short-range correlation, suggesting that the moments are fluctuating. By contrast, the basic antiferromagnetic component along the c axis has a long-range order., Comment: 5 pages, 4 figures, submitted to Physical Review Letter

Resonant x-ray scattering (RXS) experiment has been performed for the (3 0 1.5) superlattice reflection in the antiferroquadrupolar and antiferromagnetic phase of DyB2C2. Azimuthal-angle dependence of the resonance enhanced intensities for both dipolar (E1) and quadrupolar (E2) resonant processes has been measured precisely with polarization analysis. Every scattering channel exhibits distinctive azimuthal dependence, differently from the symmetric reflection at (0 0 0.5) which was studied previously. We have analyzed the results using a theory developed by Lovesey et al., which directly connects atomic tensors with the cross-section of RXS. The fitting results indicate that the azimuthal dependences can be explained well by the atomic tensors up to rank 2. Rank 3 and rank 4 tensors are reflected in the data very little. In addition, The coupling scheme among the 4f quadrupolar moment, 5d ortitals, and the lattice has been determined from the interference among the Thomson scattering from the lattice distortion and the resonant scatterings of E1 and E2 processes. It has also been established from the RXS of the (3 0 1.5) reflection that the canting of the 4f quadrupolar moments exists up to T_Q. We also discuss a possible wavefunction of the ground state from the point-charge model calculation., Comment: 9 pages, 10 figures