Diffusive excitonic bands from frustrated triangular sublattice in a singlet-ground-state system.

Magnetic order in most materials occurs when magnetic ions with finite moments arrange in a particular pattern below the ordering temperature. Intriguingly, if the crystal electric field (CEF) effect results in a spin-singlet ground state, a magnetic order can still occur due to the exchange interactions between neighboring ions admixing the excited CEF levels. The magnetic excitations in such a state are spin excitons generally dispersionless in reciprocal space. Here we use neutron scattering to study stoichiometric Ni2Mo3O8, where Ni2+ ions form a bipartite honeycomb lattice comprised of two triangular lattices, with ions subject to the tetrahedral and octahedral crystalline environment, respectively. We find that in both types of ions, the CEF excitations have nonmagnetic singlet ground states, yet the material has magnetic order. Furthermore, CEF spin excitons from the tetrahedral sites form a dispersive diffusive pattern around the Brillouin zone boundary, likely due to spin entanglement and geometric frustrations.

A Ferrotoroidic Candidate with Well-Separated Spin Chains.

The search of novel quasi-1D materials is one of the important aspects in the field of material science. Toroidal moment, the order parameter of ferrotoroidic order, can be generated by a head-to-tail configuration of magnetic moment. It has been theoretically proposed that 1D dimerized and antiferromagnetic (AFM)-like spin chain hosts ferrotoroidicity and has the toroidal moment composed of only two antiparallel spins. Here, the authors report a ferrotoroidic candidate of Ba6 Cr2 S10 with such a theoretical model of spin chain. The structure consists of unique dimerized face-sharing CrS6 octahedral chains along the c axis. An AFM-like ordering at ≈10 K breaks both space- and time-reversal symmetries and the magnetic point group of mm'2'allows three ferroic orders in Ba6 Cr2 S10 : (anti)ferromagnetic, ferroelectric, and ferrotoroidic orders. Their investigation reveals that Ba6 Cr2 S10 is a rare ferrotoroid ic candidate with quasi 1D spin chain, which can be considered as a starting point for the further exploration of the physics and applications of ferrotoroidicity.

Neutron Scattering Studies of the Breathing Pyrochlore Antiferromagnet LiGaCr_{4}O_{8}.

We report neutron scattering measurements of the spinel oxide LiGaCr_{4}O_{8}, in which magnetic ions Cr^{3+} form a breathing pyrochlore lattice. Our experiments reveal the coexistence of a nearly dispersionless resonance mode and dispersive spin-wave excitations in the magnetically ordered state, which can be quantitatively described by a quantum spin model of hexagonal loops and linear spin-wave theory with the same set of exchange parameters, respectively. Comparison to other Cr spinel oxides reveals a linear relationship between the resonance energy and lattice constant across all these materials, which is in agreement with our hexagonal loop calculations. Our results suggest a unified picture for spin resonances in Cr spinel oxides.

Sinusoidally modulated magnetic structure of Kramers local moments in CePd5Al2.

The crystalline electric field (CEF) level scheme and magnetic structure of a tetragonal antiferromagnet CePd5Al2 with [Formula: see text] K and [Formula: see text] K were studied by neutron scattering, magnetization and magnetoresistance measurements. Inelastic neutron scattering measurements on the powder sample revealed CEF excitations at 21.3 and 22.4 meV. The derived wave functions of the CEF ground state for the Ce3+ ion consist primarily of [Formula: see text] under the tetragonal symmetry. By means of single-crystal neutron diffraction, magnetic Bragg peaks characterized by a propagation vector [Formula: see text] were observed at [Formula: see text]. Our analysis indicates a sinusoidally modulated magnetic structure with amplitude of 2.0(1) [Formula: see text]/Ce, where the magnetic moments point to the [Formula: see text]-axis. The intensity of the third-order harmonic at 0.8 K is 1/30 as small as that expected for an antiphase structure, suggesting that the modulated structure remains at least down to 0.8 K. Both the magnetization and magnetoresistance show several anomalies in the magnetically ordered phase, indicating field-induced successive changes of the magnetic structure.

Magnetic Structure and Excitations in CeCuxAl4-x System.

CeCuAl3 crystallizing in the tetragonal BaNiSn3-type structure and CeCuxAl4-x solid solutions were investigated by means of elastic and inelastic neutron scattering. Powder neutron diffraction brought information on both temperature evolution of crystallographic parameters and magnetic order at low temperatures. No structural change was observed in the investigated temperature range from 1.5 to 300 K. Weak magnetic peaks outside nuclear Bragg positions observed in solid solutions with 0.90 ≤ x ≤ 1.10 were described by the propagation vector k = (0.40 + δx, 0.60 + δy, 0), where δx ≈ 0.02 and δy ≈ 0.01. The magnetic structure of CeCu0.75Al3.25 consists of two components: an anti-ferromagnetic one described by the same k and a ferromagnetic one with k0 = (0, 0, 0) and magnetic moments lying within the tetragonal basal plane. The evolution of magnetic excitations as a function of Cu-Al concentration in CeCuxAl4-x was studied by inelastic neutron scattering. The measured spectra of CeCuAl3 and the solution with x = 0.95 point to a three-magnetic-peak energy scheme, while only two excitations are expected from the local symmetry conditions on Ce atoms. The standard two-peak spectrum of crystal electric field excitations was observed for Cu-Al substitutions further from the 1:1:3 stoichiometry (x = 0.75 and 1.10). The intermediate concentrations (x = 0.90 and 1.05) exhibit spectra on the border between the former cases with a less clear pronounced first inelastic magnetic peak. The observed behavior is discussed considering the evolution of structural parameters in the CeCuxAl4-x system and the coupling between the lattice vibrations and the crystal electric field excitations.

Coulomb spin liquid in anion-disordered pyrochlore Tb2Hf2O7.

The charge ordered structure of ions and vacancies characterizing rare-earth pyrochlore oxides serves as a model for the study of geometrically frustrated magnetism. The organization of magnetic ions into networks of corner-sharing tetrahedra gives rise to highly correlated magnetic phases with strong fluctuations, including spin liquids and spin ices. It is an open question how these ground states governed by local rules are affected by disorder. Here we demonstrate in the pyrochlore Tb2Hf2O7, that the vicinity of the disordering transition towards a defective fluorite structure translates into a tunable density of anion Frenkel disorder while cations remain ordered. Quenched random crystal fields and disordered exchange interactions can therefore be introduced into otherwise perfect pyrochlore lattices of magnetic ions. We show that disorder can play a crucial role in preventing long-range magnetic order at low temperatures, and instead induces a strongly fluctuating Coulomb spin liquid with defect-induced frozen magnetic degrees of freedom.Experimental studies of frustrated spin systems such as pyrochlore magnetic oxides test our understanding of quantum many-body physics. Here the authors show experimentally that Tb2Hf2O7 may be a model material for investigating how structural disorder can stabilize a quantum spin liquid phase.