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Quasicrystals (QCs), first discovered in 1984, generally do not exhibit long-range magnetic order. Here, we report on long-range magnetic order in the real icosahedral quasicrystals (i QCs) Au–Ga–Gd and Au–Ga–Tb. The Au65Ga20Gd15i QC exhibits a ferromagnetic transition at TC = 23 K, manifested as a sharp anomaly in both magnetic susceptibility and specific heat measurements, along with an appearance of magnetic Bragg peak below TC. This is the first observation of long-range magnetic order in a real quasicrystal, in contrast to the spin-glass-like behaviors observed for the other magnetic quasicrystals found to date. Moreover, when Gd is replaced by Tb, i.e., for the Au65Ga20Tb15i QC, a ferromagnetic behavior is still retained with TC = 16 K. Although the sharp anomaly in the specific heat observed for the Au65Ga20Gd15i QC becomes broadened upon Tb substitution, neutron diffraction experiments clearly show marked development of magnetic Bragg peaks just below TC, indicating long-range magnetic order for the Au65Ga20Tb15i QC also. Our findings can contribute to the further investigation of exotic magnetic orders formed on real quasiperiodic lattices with unprecedented highest global symmetry, i.e., icosahedral symmetry.

A magnetic order of the quasicrystal approximant Au70Al16Tb14 was investigated via single crystalline neutron diffraction experiments. In spite of some differences in the macroscopic magnetic properties compared with Au72Al14Tb14, the whirling antiferromagnetic structure similar to Au72Al14Tb14 was found. The robustness of the magnetic structure suggests the orientation of the magnetic moment dominated by easy-axis anisotropy of Tb. In addition, the critical exponent β indicates a mean field nature of the magnetic transition.

The control of the stoichiometry of Li 1 + x Zn 2 − y Mo 3 O 8 was achieved by the solid-state-reaction. We found that the best sample that has the chemical composition Li 0.95 ( 4 ) Zn 1.92 ( 8 ) Mo 3 O 8 was obtained from the starting nominal composition with Li : Zn : Mo : O= ( 1 + w ) : ( 2.8 − w ) : 3 : 8.6 with w = − 0.1 , indicating that the stoichiometry is greatly improved compared to those in the earlier reports. For larger w detailed structural analysis indicates that the mixed sites of Li and Zn are preferentially occupied by Li atoms, as well as the fraction of the non-magnetic secondary phase Zn 2 Mo 3 O 8 decreases. Magnetic susceptibility of the improved stoichiometry powder samples shows a broad hump in the temperature range of 100 T 200 K . This suggests that the development of antiferromagnetic correlations at the high temperatures is inherent to the ideal stoichiometric Li Zn 2 Mo 3 O 8 .

We report the synthesis, crystal structure, and magnetic properties of two new quantum antiferromagnets A3ReO5Cl2 (A = Sr and Ba). The crystal structure is isostructural with the mineral pinalite Pb3WO5Cl2, in which the Re6+ ion is square-pyramidally coordinated by five oxide atoms, and forms an anisotropic triangular lattice (ATL) made of S = 1/2 spins. The magnetic interactions J and J' in the ATL are estimated from magnetic susceptibilities to be 19.5 (44.9) and 9.2 (19.3) K, respectively, with J'/J = 0.47 (0.43) for A = Ba (Sr). For each compound, heat capacity at low temperatures shows a large T-linear component with no signature of long-range magnetic order above 2 K, which suggests a gapless spin liquid state of one-dimensional character of the J chains in spite of the significantly large J' couplings. This is a consequence of one-dimensionalization by geometrical frustration in the ATL magnet; a similar phenomenon has been observed in two compounds with slightly smaller J'/J values: Cs2CuCl4 (J'/J = 0.3) and the related compound Ca3ReO5Cl2 (0.32). Our findings demonstrate that 5d mixed-anion compounds provide a unique opportunity to explore novel quantum magnetism., Comment: 24 pages, 7 figures, 2 Tables

This work presents the inelastic neutron scattering spectrum on the spin-1/2 anisotropic triangular lattice antiferromagnetCa_3 ReO_5 Cl_2 , and show that the spinon-like continuum coexists with dispersive modes due to the formation of bound spinon pairs.

We report the synthesis, crystal structure, and magnetic properties of the two new quantum antiferromagnets A

We performed neutron diffraction experiments on a single crystal of an $S=\frac{1}{2}$ frustrated ferromagnetic chain compound ${\mathrm{NaCuMoO}}_{4}$(OH) at zero and finite magnetic fields. Three magnetic Bragg peaks with the propagation vector of $\mathbit{q}=(0,\ensuremath{\delta},0)$ $[\ensuremath{\delta}=0.481(1)]$ were observed at the zero field, which means that an incommensurate helical magnetic order was realized. Using the ratio of the intensities between these magnetic peaks, a proper-screw structure was suggested, where the spiral plane is the crystallographic $ac$ plane. While the $\ensuremath{\delta}$ is unchanged at lower fields, it decreases linearly with the field where ${\ensuremath{\mu}}_{0}H\ensuremath{\ge}2.5\phantom{\rule{0.16em}{0ex}}\mathrm{T}$. The field dependence is consistent with that of the field-induced spin density wave state that originated from the formation of the bound state of two magnons in the $S=\frac{1}{2}$ frustrated ferromagnetic chain.

We investigated the magnetic properties of the ilmenite-type manganates $\mathrm{MgMn}{\mathrm{O}}_{3}$ and $\mathrm{ZnMn}{\mathrm{O}}_{3}$, both of which are composed of a honeycomb lattice of magnetic $\mathrm{M}{\mathrm{n}}^{4+}$ ions. Both compounds show antiferromagnetic order with weak ferromagnetic moments. In particular, $\mathrm{MgMn}{\mathrm{O}}_{3}$ exhibits a magnetization ``reversal'' behavior which can be described by the $N$-type ferrimagnetism in the N\'eel's classification. The relationship between the magnetic properties and the crystal and magnetic structures probed by the neutron diffraction experiments indicates that the two honeycomb lattice magnets have different ${J}_{1}\ensuremath{-}{J}_{2}$ parameter sets, placing them in the distinct regions in the phase diagram; both nearest neighbor (NN) and next nearest neighbor (NNN) exchange interactions are antiferromagnetic in $\mathrm{MgMn}{\mathrm{O}}_{3}$, while NN and NNN interactions become ferromagnetic and antiferromagnet, respectively, in $\mathrm{ZnMn}{\mathrm{O}}_{3}$.

We report on the emergence of antiferromagnetic spin chains from two-dimensionally aligned spins on the anisotropic triangular lattice (ATL) in the insulating calcium rhenium oxychloride Ca3ReO5Cl2. The compound contains Re6+ ions each with one unpaired electron in the dxy orbital, which are arranged to form a spin-1/2 ATL with J'/J ~ 0.32 and J = 41 K, where J and J' are magnetic interactions in and between the chains, respectively. In spite of the apparent two dimensionality, we observe clear evidence of a gapless spin liquid that is characteristic of the spin-1/2 Heisenberg chain. This one-dimensionalization must be caused by geometrical frustration: growing antiferromagnetic correlations in every chain effectively cancel out inter-chain zigzag couplings at low temperature. Ca3ReO5Cl2 provides us with a detailed insight into the interesting physics of the ATL antiferromagnet, especially via comparison with the typical ATL compound Cs2CuCl4., 9 pages, 4 figures, 1 Table

We revisited the crystal structure of α-Cu2V2O7. An absolute structure determination have been performed. Ten pieces of crystals were randomly selected from a single large crystal. Inclusion of inv...

We have investigated magnetic properties of the rare-earth based intermetallic compound Yb3Ni11Ge4.63 (YNG), where Yb3+ ions form a breathing-kagome lattice. Single-site 4f electron wavefunctions o...

In an ideal classical pyrochlore antiferromagnet without perturbations, an infinite degeneracy in a ground state leads to the absence of magnetic order and a spin-glass transition. Here we present ${\mathrm{Na}}_{3}\mathrm{Mn}{({\mathrm{CO}}_{3})}_{2}\mathrm{Cl}$ 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 magnetic order is detected in magnetization and heat capacity measurements or powder neutron diffraction experiments. On the other hand, antiferromagnetic short-range order of the nearest neighbors is evidenced by the $Q$ dependence of the diffuse scattering which develops around $0.85\phantom{\rule{0.16em}{0ex}}{\AA{}}^{\ensuremath{-}1}$. A high degeneracy near the ground state in ${\mathrm{Na}}_{3}\mathrm{Mn}{({\mathrm{CO}}_{3})}_{2}\mathrm{Cl}$ is supported by the magnetic entropy, estimated as almost $4\phantom{\rule{0.16em}{0ex}}\mathrm{J}\phantom{\rule{0.16em}{0ex}}{\mathrm{K}}^{\ensuremath{-}2}\phantom{\rule{0.16em}{0ex}}{\mathrm{mol}}^{\ensuremath{-}1}$ at 0.5 K.

The phase diagram of the quasi-one-dimensional magnet ${\mathrm{NaCuMoO}}_{4}(\mathrm{OH})$ is established through single-crystal NMR and heat-capacity measurements. The $^{23}\mathrm{Na}$ and $^{1}\mathrm{H}$ NMR experiments indicate a spiral and a collinear spin density wave (SDW) order below and above ${B}_{c}$ = 1.5--1.8 T, respectively. Moreover, in the paramagnetic state above the SDW transition temperature, the nuclear spin-lattice relaxation rate $1/{T}_{1}$ indicates anisotropic spin fluctuations that have gapped excitations in the transverse spectrum but gapless ones in the longitudinal spectrum. These static and dynamic properties are well described by a theoretical model assuming quasi-one-dimensional chains with competing ferromagnetic nearest-neighbor interactions ${J}_{1}$ and antiferromagnetic next-nearest-neighbor interactions ${J}_{2}$ (${J}_{1}\ensuremath{-}{J}_{2}$ chains). Because of the excellent crystal quality and good one-dimensionality, ${\mathrm{NaCuMoO}}_{4}(\mathrm{OH})$ is a promising compound to elucidate the unique physics of the frustrated ${J}_{1}\ensuremath{-}{J}_{2}$ chain.

We report single-crystal 51V NMR studies on volborthite Cu3V2O7(OH)2 2H2O, which is regarded as a quasi-two-dimensional frustrated magnet with competing ferromagnetic and antiferromagnetic interactions. In the 1/3 magnetization plateau above 28 T, the nuclear spin-lattice relaxation rate 1/T1 indicates an excitation gap with a large effective g factor in the range of 4.6-5.9, pointing to magnon bound states. Below 26 T where the gap has closed, the NMR spectra indicate small internal fields with a Gaussian-like distribution, whereas 1/T1 shows a power-law-like temperature dependence in the paramagnetic state, which resembles a slowing down of spin fluctuations associated with magnetic order. We discuss the possibility of an exotic spin state caused by the condensation of magnon bound states below the magnetization plateau., 10 pages, 13 figures

We investigated magnetic and thermodynamic properties of $S=\frac{1}{2}$ quasi-one-dimensional antiferromagnet ${\mathrm{KCuMoO}}_{4}(\mathrm{OH})$ through single-crystalline magnetization and heat capacity measurements. At zero field, it behaves as a uniform $S=\frac{1}{2}$ Heisenberg antiferromagnet with $J=238\phantom{\rule{0.28em}{0ex}}\mathrm{K}$, and exhibits a canted antiferromagnetism below ${T}_{\mathrm{N}}=1.52\phantom{\rule{0.28em}{0ex}}\mathrm{K}$. In addition, a magnetic field $H$ induces the anisotropy in magnetization and opens a gap in the spin-excitation spectrum. These properties are understood in terms of an effective staggered field induced by staggered $g$ tensors and Dzyaloshinsky-Moriya (DM) interactions. Temperature dependencies of the heat capacity and their field variations are consistent with those expected for quantum sine-Gordon model, indicating that spin excitations consist of soliton, antisoliton, and breather modes. From field dependencies of the soliton mass, the staggered field normalized by the uniform field ${c}_{\mathrm{s}}$ is estimated as 0.041, 0.174, and 0.030, for $H\ensuremath{\parallel}a$, $b$, and $c$, respectively. Such a large variation of ${c}_{\mathrm{s}}$ is understood as the combination of staggered $g$ tensors and DM interactions which induce the staggered field in the opposite direction for $H\ensuremath{\parallel}a$ and $c$ but almost the same direction for $H\ensuremath{\parallel}b$ at each Cu site.

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., 9 pages, 10 figures

We report on the dynamics of the spin-1/2 quasi-one-dimensional frustrated magnet LiCuVO$\mathrm{_4}$ measured by nuclear spin relaxation in high magnetic fields 10--34 T, in which the ground state has spin-density-wave order. The spin fluctuations in the paramagnetic phase exhibit striking anisotropy with respect to the magnetic field. The transverse excitation spectrum probed by $^{51}$V nuclei has an excitation gap, which increases with field. On the other hand, the gapless longitudinal fluctuations sensed by $^7$Li nuclei grow with lowering temperature, but tend to be suppressed with increasing field. Such anisotropic spin dynamics and its field dependence agree with the theoretical predictions and are ascribed to the formation of bound magnon pairs, a remarkable consequence of the frustration between ferromagnetic nearest neighbor and antiferromagnetic next-nearest-neighbor interactions., Comment: 7 pages, 6 figures

We report on the electronic ground state of a layered perovskite vanadium oxide ${\mathrm{Sr}}_{2}{\mathrm{VO}}_{4}$ studied by the combined use of synchrotron radiation x-ray diffraction (SR-XRD) and muon spin rotation/relaxation $(\ensuremath{\mu}\mathrm{SR})$ techniques, where $\ensuremath{\mu}\mathrm{SR}$ measurements were extended down to 30 mK. We found an intermediate orthorhombic phase between ${T}_{\mathrm{c}2}\ensuremath{\sim}130$ K and ${T}_{\mathrm{c}1}\ensuremath{\sim}100$ K, whereas a tetragonal phase appears for $Tg{T}_{\mathrm{c}2}$ and $Tl{T}_{\mathrm{c}1}$. The absence of long-range magnetic order was confirmed by $\ensuremath{\mu}\mathrm{SR}$ at the reentrant tetragonal phase below ${T}_{\mathrm{c}1}$, where the relative enhancement in the $c$-axis length versus that of the $a$-axis length was observed. However, no clear indication of the lowering of the tetragonal lattice symmetry with superlattice modulation, which is expected in the orbital order state with superstructure of ${d}_{yz}$ and ${d}_{zx}$ orbitals, was observed by SR-XRD below ${T}_{\mathrm{c}1}$. Instead, it was inferred from $\ensuremath{\mu}\mathrm{SR}$ that a magnetic state developed below ${T}_{\mathrm{c}0}\ensuremath{\sim}10$ K, which was characterized by the highly inhomogeneous and fluctuating local magnetic fields down to 30 mK. We argue that the anomalous magnetic ground state below ${T}_{\mathrm{c}0}$ originates from the coexistence of ferromagnetic and antiferromagnetic correlations.

Single crystals of the new compound KCuMoO4(OH) are hydrothermally synthesized from aqueous solutions of Cu(NO3)2 and K2MoO4 (autoclave, 433 K followed by slow heating to 493 K in 240 h).

We have synthesized high-quality single crystals of volborthite, a seemingly distorted kagome antiferromagnet, and carried out high-field magnetization measurements up to 74 T and 51V NMR measurements up to 30 T. An extremely wide 1/3 magnetization plateau appears above 28 T and continues over 74 T at 1.4 K, which has not been observed in previous study using polycrystalline samples. NMR spectra reveal an incommensurate order (most likely a spin-density wave order) below 22 T and a simple spin structure in the plateau phase. Moreover, a novel intermediate phase is found between 23 and 26 T, where the magnetization varies linearly with magnetic field and the NMR spectra indicate an inhomogeneous distribution of the internal magnetic field. This sequence of phases in volborthite bear a striking similarity to those of frustrated spin chains with a ferromagnetic nearest-neighbor coupling J1 competing with an antiferromagnetic next-nearest-neighbor coupling J2., 12 pages, 5 figures

A new spin-1/2 quasi-one-dimensional antiferromagnet KCuMoO_4(OH) is prepared by the hydrothermal method. The crystal structures of KCuMoO_4(OH) and the already-known Na-analogue, NaCuMoO_4(OH), are isotypic, comprising chains of Cu^{2+} ions in edge-sharing CuO_4(OH)_2 octahedra. Despite the structural similarity, their magnetic properties are quite different because of the different arrangements of d_{x2-y2} orbitals carrying spins. For NaCuMoO_4(OH), d_{x2-y2} orbitals are linked by superexchange couplings via two bridging oxide ions, which gives a ferromagnetic nearest-neighbor interaction J_1 of -51 K and an antiferromagnetic next-nearest-neighbor interaction J_2 of 36 K in the chain. In contrast, a staggered d_{x2-y2} orbital arrangement in KCuMoO_4(OH) results in superexchange couplings via only one bridging oxide ion, which makes J_1 antiferromagnetic as large as 238 K and J_2 negligible. This comparison between the two isotypic compounds demonstrates an important role of orbital arrangements in determining the magnetic properties of cuprates., Comment: 7 pages, 5 figures published to Inorg. Chem. (2015)

In a frustrated J_1-J_2 chain with the nearest-neighbor ferromagnetic interaction J_1 and the next-nearest-neighbor antiferromagnetic interaction J_2, novel magnetic states such as a spin-nematic state are theoretically expected. However, they have been rarely examined in experiments because of the difficulty in obtaining suitable model compounds. We show here that the quasi-one-dimensional antiferromagnet NaCuMoO_4(OH), which comprises edge-sharing CuO_2 chains, is a good candidate J_1-J_2 chain antiferromagnet. The exchange interactions are estimated as J_1 = - 51 K and J_2 = 36 K by comparing the magnetic susceptibility, heat capacity, and magnetization data with the data obtained using calculations by the exact diagonalization method. High-field magnetization measurements at 1.3 K show a saturation above 26 T with little evidence of a spin nematic state expected just below the saturation field, which is probably due to smearing effects caused by thermal fluctuations and the polycrystalline nature of the sample., 6 pages, 4 figures

We have performed NMR experiments on the quasi one-dimensional frustrated spin-1/2 system LiCuVO$_4$ in magnetic fields $H$ applied along the c-axis up to field values near the saturation field $H_{\rm sat}$. For the field range $H_{\rm c2} 41.4$T, indicating that the majority of magnetic moments in LiCuVO$_4$ are already saturated in this field range. This result is inconsistent with the previously observed linear field dependence of the magnetization $M(H)$ for $H_{\rm c3}, Comment: 8 pages, 9 figures

We report results of NMR experiments on a single crystal of the quasi one-dimensional frustrated magnet LiCuVO_4. The NMR spectra of ^7Li and ^{51}V nuclei indicate a helical spin order in a magnetic field of 4 T with the helical spin plane perpendicular to the field and a spin-density-wave (SDW) order at 10 T with modulation in the magnitude of the moments aligned along the field, in agreement with earlier reports. The nuclear spin-lattice relaxation rate 1/T_1 at ^{51}V nuclei, which is selectively coupled to the transverse spin fluctuations perpendicular to the field, shows a pronounced peak near the helical ordering temperature in the field of 4 T applied along the a-axis. In the field of 10 T, however, such a peak is absent. Instead 1/T_1 at ^7Li nuclei probing longitudinal spin fluctuations shows divergent behavior towards the SDW ordering temperature. These results are qualitatively consistent with the theoretical description that the SDW correlation is due to bound magnon pairs, which produce an energy gap in the transverse spin excitation spectrum., Comment: 14 pages, 7 figures, 3 tables, accepted for publication in J. Phys. Soc. Jpn

Pb2V3O9 was found to have antiferromagnetic alternating chains of S=1/2 and show the antiferromagnetic long range ordered (AFLRO) state under the magnetic field between 4 and 38 T. We succeeded in growing single crystals of Pb2V3O9 by floating zone method and determined the asymmetric H-T phase diagram of Pb2V3O9 from measurements of the magnetization and the heat capacity. Previous reports focused on the AFLRO state in the low magnetic field region and that in high magnetic field region was not discussed so much. In this paper, we examined the AFLRO state in terms of the mean field theory and the picture of Bose-Einstein condensation of magnons to discuss the whole phase diagram. Consequently, the asymmetry of the phase boundary in Pb2V3O9 is explained by the mixing contribution of excited states and by interchain interactions., Comment: 14 pages, 14 figures

We synthesized single crystals of NH4CuPO4 H2O by a chemical reaction in aqueous solutions. Magnetization and specific heat are well reproduced by a dimer model, and NH4CuPO4 H2O does not show any field-induced magnetic phase transitions. The interdimer interactions would be too weak to observe field-induced phase transitions.