Nonmagnetic Ground State in RuO_{2} Revealed by Muon Spin Rotation.

The magnetic ground state of single crystalline RuO_{2} was investigated by the muon spin rotation and relaxation (µSR) experiment. The spin precession signal due to the spontaneous internal magnetic field B_{loc}, which is expected in the magnetically ordered phase, was not observed in the temperature range 5-400 K. Muon sites were evaluated by first-principles calculations using dilute hydrogen simulating muon as pseudohydrogen, and B_{loc} was simulated for the antiferromagnetic structures with a Ru magnetic moment |m_{Ru}|≈0.05µ_{B} suggested from diffraction experiments. As a result, the possibility was ruled out that muons are localized at sites where B_{loc} accidentally cancels. Conversely, assuming that the slow relaxation observed in µSR spectra was part of the precession signal, the upper limit for the magnitude of |m_{Ru}| was estimated to be 4.8(2)×10^{-4}µ_{B}, which is significantly less than 0.05µ_{B}. These results indicate that the antiferromagnetic order, as reported, is unlikely to exist in the bulk crystal.

Dimensional reduction and incommensurate dynamic correlations in the [Formula: see text] triangular-lattice antiferromagnet Ca3ReO5Cl2.

The observation of spinon excitations in the [Formula: see text] triangular antiferromagnet Ca3ReO5Cl2 reveals a quasi-one-dimensional (1D) nature of magnetic correlations, in spite of the nominally 2D magnetic structure. This phenomenon is known as frustration-induced dimensional reduction. Here, we present high-field electron spin resonance spectroscopy and magnetization studies of Ca3ReO5Cl2, allowing us not only to refine spin-Hamiltonian parameters, but also to investigate peculiarities of its low-energy spin dynamics. We argue that the presence of the uniform Dzyaloshinskii-Moriya interaction (DMI) shifts the spinon continuum in momentum space and, as a result, opens a zero-field gap at the Γ point. We observed this gap directly. The shift is found to be consistent with the structural modulation in the ordered state, suggesting this material as a perfect model triangular-lattice system, where a pure DMI-spiral ground state can be realized.

A series of magnon crystals appearing under ultrahigh magnetic fields in a kagomé antiferromagnet.

Geometrical frustration and a high magnetic field are two key factors for realizing unconventional quantum states in magnetic materials. Specifically, conventional magnetic order can potentially be destroyed by competing interactions and may be replaced by an exotic state that is characterized in terms of quasiparticles called magnons, the density and chemical potential of which are controlled by the magnetic field. Here we show that a synthetic copper mineral, Cd-kapellasite, which comprises a kagomé lattice consisting of corner-sharing triangles of spin-1/2 Cu2+ ions, exhibits an unprecedented series of fractional magnetization plateaus in ultrahigh magnetic fields of up to 160 T. We propose that these quantum states can be interpreted as crystallizations of emergent magnons localized on the hexagon of the kagomé lattice.

Author Correction: Two-magnon scattering in the 5d all-in-all-out pyrochlore magnet Cd2Os2O7.

A correction to this article has been published and is linked from the HTML version of this article.

Maximizing T c by tuning nematicity and magnetism in FeSe1-x S x superconductors.

A fundamental issue concerning iron-based superconductivity is the roles of electronic nematicity and magnetism in realising high transition temperature (T c). To address this issue, FeSe is a key material, as it exhibits a unique pressure phase diagram involving non-magnetic nematic and pressure-induced antiferromagnetic ordered phases. However, as these two phases in FeSe have considerable overlap, how each order affects superconductivity remains perplexing. Here we construct the three-dimensional electronic phase diagram, temperature (T) against pressure (P) and isovalent S-substitution (x), for FeSe1-x S x . By simultaneously tuning chemical and physical pressures, against which the chalcogen height shows a contrasting variation, we achieve a complete separation of nematic and antiferromagnetic phases. In between, an extended non-magnetic tetragonal phase emerges, where T c shows a striking enhancement. The completed phase diagram uncovers that high-T c superconductivity lies near both ends of the dome-shaped antiferromagnetic phase, whereas T c remains low near the nematic critical point.

Classical Spin Nematic Transition in LiGa_{0.95}In_{0.05}Cr_{4}O_{8}.

We present the results of a combined ^{7}Li-NMR and diffraction study on LiGa_{0.95}In_{0.05}Cr_{4}O_{8}, a member of the LiGa_{1-x}In_{x}Cr_{4}O_{8} "breathing" pyrochlore family. Via specific heat and NMR measurements, we find that the complex sequence of first-order transitions observed for LiGaCr_{4}O_{8} is replaced by a single second-order transition at T_{f}=11 K. Neutron and x-ray diffraction rule out both structural symmetry lowering and magnetic long-range order as the origin of this transition. Instead, reverse Monte Carlo fitting of the magnetic diffuse scattering indicates that the low-temperature phase may be described as a collinear spin nematic state, characterized by a quadrupolar order parameter. This state also shows signs of short-range order between collinear spin arrangements on tetrahedra, revealed by mapping the reverse Monte Carlo spin configurations onto a three-state color model.

Two-magnon scattering in the 5d all-in-all-out pyrochlore magnet Cd2Os2O7.

5d pyrochlore oxides with all-in-all-out magnetic order are prime candidates for realizing strongly correlated, topological phases of matter. Despite significant effort, a full understanding of all-in-all-out magnetism remains elusive as the associated magnetic excitations have proven difficult to access with conventional techniques. Here we report a Raman spectroscopy study of spin dynamics in the all-in-all-out magnetic state of the 5d pyrochlore Cd2Os2O7. Through a comparison between the two-magnon scattering and spin-wave theory, we confirm the large single ion anisotropy in this material and show that the Dzyaloshinskii-Moriya and exchange interactions play a significant role in the spin-wave dispersions. The Raman data also reveal complex spin-charge-lattice coupling and indicate that the metal-insulator transition in Cd2Os2O7 is Lifshitz-type. Our work establishes Raman scattering as a simple and powerful method for exploring the spin dynamics in 5d pyrochlore magnets.Pyrochlore 5d transition metal oxides are expected to have interesting forms of magnetic order but are hard to study with conventional probes. Here the authors show that Raman scattering can be used to measure magnetic excitations in Cd2Os2O7 and that it exhibits complex spin-charge-lattice coupling.

Strong Spin-Phonon Coupling Mediated by Single Ion Anisotropy in the All-In-All-Out Pyrochlore Magnet Cd_{2}Os_{2}O_{7}.

Spin-phonon coupling mediated by single ion anisotropy was investigated using optical spectroscopy and first-principles calculations in the all-in-all-out pyrochlore magnet Cd_{2}Os_{2}O_{7}. Clear anomalies were observed in both the phonon frequencies and linewidths at the magnetic ordering temperature. The renormalization of the phonon modes was exceptionally large, signifying the presence of an unconventional magnetoelastic term from large spin-orbit coupling. In addition, the relative phonon frequency shifts show a strong correlation with the modulation of noncubic crystal field by the corresponding lattice distortion. Our observation establishes a new type of spin-phonon coupling through single ion anisotropy, a second-order spin-orbit coupling term, in Cd_{2}Os_{2}O_{7}.

One-Third Magnetization Plateau with a Preceding Novel Phase in Volborthite.

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 ^{51}V 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 studies 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 bears a striking similarity to those of frustrated spin chains with a ferromagnetic nearest-neighbor coupling J_{1} competing with an antiferromagnetic next-nearest-neighbor coupling J_{2}.

Optical Spectroscopic Studies of the Metal-Insulator Transition Driven by All-In-All-Out Magnetic Ordering in 5d Pyrochlore Cd(2)Os(2)O(7).

We investigated the metal-insulator transition (MIT) driven by all-in-all-out (AIAO) antiferromagnetic ordering in the 5d pyrochlore Cd(2)Os(2)O(7) using optical spectroscopy and first-principles calculations. We showed that the temperature evolution in the band-gap edge and free carrier density were consistent with rigid upward (downward) shifts of electron (hole) bands, similar to the case of Lifshitz transitions. The delicate relationship between the band gap and free carrier density provides experimental evidence for the presence of an AIAO metallic phase, a natural consequence of such MITs. The associated spectral weight change at high energy and first-principles calculations further support the origin of the MIT from the band shift near the Fermi level. Our data consistently support that the MIT induced by AIAO ordering in Cd(2)Os(2)O(7) is not close to a Slater type but instead to a Lifshitz type.

Giant phonon softening and enhancement of superconductivity by phosphorus doping of BaNi2As2.

The effects of phosphorus doping on the structural and superconducting phase transitions of BaNi2(As(1-x)P(x))2 were studied. The specific heat, resistivity, and magnetic susceptibility were measured. The results revealed an abrupt increase in the superconducting transition temperature (T(c)) from 0.6 K in the triclinic phase (space group P1¯) with less phosphorus (x≤0.067) to 3.3 K in the tetragonal phase (space group I4/mmm) with more phosphorus (x≥0.067). Our data analysis suggests that a doping-induced softening related to an in-plane Ni and As(P) phonon mode is responsible for the enhanced superconductivity in the tetragonal phase.

Tetrahedral magnetic order and the metal-insulator transition in the pyrochlore lattice of Cd2Os2O7.

Cd2Os2O7 shows a peculiar metal-insulator transition at 227 K with magnetic ordering in a frustrated pyrochlore lattice, but its magnetic structure in the ordered state and the transition origin are yet uncovered. We observed a commensurate magnetic peak by resonant x-ray scattering in a high-quality single crystal. X-ray diffraction and Raman scattering experiments confirmed that the transition is not accompanied with any spatial symmetry breaking. We propose a noncollinear all-in-all-out spin arrangement on the tetrahedral network made of Os atoms. Based on this we suggest that the transition is not caused by the Slater mechanism as believed earlier but by an alternative mechanism related to the formation of the specific tetrahedral magnetic order on the pyrochlore lattice in the presence of strong spin-orbit interactions.

The spin dynamics in distorted kagome lattices: a comparative Raman study.

Despite the conceptional importance of realizing spin liquids in solid states only few compounds are known. On the other hand the effect of lattice distortions and anisotropies on the magnetic exchange topology and the fluctuation spectrum is an interesting problem. We compare the excitation spectra of the two s = 1/2 kagome lattice compounds, volborthite and vesignieite, using Raman scattering. We demonstrate that even small modifications of the crystal structure may have a huge effect on the phonon spectrum and low-temperature properties.

Phase diagram and spin dynamics in volborthite with a distorted kagome lattice.

We report a (51)V-NMR study on a high-quality powder sample of volborthite Cu3V2O7(OH)2 . 2H2O, a spin-1/2 Heisenberg antiferromagnet on a distorted kagome lattice formed by isosceles triangles. In the magnetic fields below 4.5 T, a sharp peak in the nuclear spin-lattice relaxation rate 1/T(1) accompanied with line broadening revealed a magnetic transition near 1 K. The low temperature phase shows anomalies such as a Lorentzian line shape, a 1/T(1) proportional, variantT behavior indicating dense low-energy excitations, and a large spin-echo decay rate 1/T(2) pointing to unusually slow fluctuations. Another magnetic phase appears above 4.5 T with less anomalous spectral shape and dynamics.

Interplay of superconductivity and rattling phenomena in beta-pyrochlore KOs2O6 studied by photoemission spectroscopy.

The electronic structure near the Fermi level (EF) of the beta-pyrochlore superconductor KOs2O6 is studied using laser-excited ultrahigh-resolution photoemission spectroscopy. The superconducting gap clearly opens across the superconducting transition (Tc=9.6 K), with the strong electron-phonon coupling value of 2Delta(0)/k B Tc>or=4.56. A fitting analysis identifies clear anomalies at Tp=7.5 K in the temperature dependencies of the superconducting gap size and the quasiparticle relaxation lifetime. These anomalies and the fine spectral structures arising from phonons suggest that the existence of the rattling behavior of K ions significantly affects the superconductivity in KOs2O6.

NMR observation of rattling phonons in the pyrochlore superconductor KOs2O6.

We report nuclear magnetic resonance studies on the beta-pyrochlore oxide superconductor KOs2O6. The nuclear relaxation at the K sites is entirely caused by fluctuations of the electric field gradient, which we ascribe to highly anharmonic low frequency oscillation (rattling) of K ions. A phenomenological analysis shows a crossover from overdamped to underdamped behavior of the rattling phonons with decreasing temperature and its sudden sharpening below the superconducting transition temperature T(c). Suppression of the Hebel-Slichter peak in the relaxation rate at the O sites below T(c) also indicates strong electron-phonon coupling.

Isotropically gapped strong-coupling superconductivity in the beta-pyrochlore KOs2O6: evidence from penetration depth measurements.

We report on measurements of the temperature dependence of the magnetic penetration depth down to 0.04 K in a high-quality sample of the beta-pyrochlore KOs2O6 (Tc=9.65 K) with a spin-frustrated lattice. We observe temperature-independent behavior below T approximately 0.3Tc, which is firm evidence for the presence of an isotropic superconducting gap in this material. In the whole temperature range the superfluid density is very well described, without the need of adjustable parameters, by a strong-coupling extension of the BCS model for an isotropic gap. Thus, the penetration depth results indicate that KOs2O6 is a strong-coupling superconductor with a fully developed energy gap. No effect of the second phase transition taking place at Tp=7.5 K was observed on the penetration depth, which suggests that the Cooper pairs remain unperturbed across this transition.

effects of rattling phonons on the dynamics of quasiparticle excitation in the beta-pyrochlore KOs(2)O(6) Superconductor.

Microwave penetration depth lambda and surface resistance at 27 GHz are measured in high quality crystals of KOs(2)O(6). Firm evidence for fully gapped superconductivity is provided from lambda(T). Below the second transition at T(p) approximately 8 K, the superfluid density shows a steplike change with a suppression of effective critical temperature T(c). Concurrently, the extracted quasiparticle scattering time shows a steep enhancement, indicating a strong coupling between the anomalous rattling motion of K ions and quasiparticles. The results imply that the rattling phonons help to enhance superconductivity, and that K sites freeze to an ordered state with long quasiparticle mean free path below T(p).

Vortex redistribution below the first-order transition temperature in the beta-pyrochlore superconductor KOs2O6.

A miniature Hall-sensor array was used to detect magnetic induction locally in the vortex states of the beta-pyrochlore superconductor KOs2O6. Below the first-order transition at T{p} approximately 8 K, which is associated with a change in the rattling motion of K ions, the lower critical field and the remanent magnetization both show a distinct decrease, suggesting that the electron-phonon coupling is weakened below the transition. At high magnetic fields, the local induction shows an unexpectedly large jump at T{p} whose sign changes with position inside the sample. Our results demonstrate a novel redistribution of vortices whose energy is reduced abruptly below the first-order transition at T{p}.

Thermal conductivity of the pyrochlore superconductor KOs2O6: strong electron correlations and fully gapped superconductivity.

To elucidate the nature of the superconducting ground state of the geometrically frustrated pyrochlore KOs2O6 (Tc=9.6 K), the thermal conductivity was measured down to low temperatures (approximately Tc/100). We found that the quasiparticle mean free path is strikingly enhanced below a transition at Tp=7.8 K, indicating enormous electron inelastic scattering in the normal state. In magnetic fields, the conduction at T-->0 K is nearly constant up to approximately 0.4Hc2, in contrast with the rapid growth expected for superconductors with an anisotropic gap. This unambiguously indicates a fully gapped superconductivity, in contrast with previous studies. These results highlight that KOs2O6 is unique among superconductors with strong electron correlations.