Spin Density Wave versus Fractional Magnetization Plateau in a Triangular Antiferromagnet.

We report an excellent realization of the highly nonclassical incommensurate spin-density wave (SDW) state in the quantum frustrated antiferromagnetic insulator Cs_{2}CoBr_{4}. In contrast to the well-known Ising spin chain case, here the SDW is stabilized by virtue of competing planar in-chain anisotropies and frustrated interchain exchange. Adjacent to the SDW phase is a broad m=1/3 magnetization plateau that can be seen as a commensurate locking of the SDW state into the up-up-down (UUD) spin structure. This represents the first example of the long-sought SDW-UUD transition in triangular-type quantum magnets.

Broadband critical dynamics in disordered lead-based perovskites.

Materials based on the cubic perovskite unit cell continue to provide the basis for technologically important materials with two notable recent examples being lead-based relaxor piezoelectrics and lead-based organic-inorganic halide photovoltaics. These materials carry considerable disorder, arising from site substitution in relaxors and molecular vibrations in the organic-inorganics, yet much of our understanding of these systems derives from the initial classic work of Prof. Roger A Cowley, who applied both theory and neutron scattering methods while at Chalk River Laboratories to the study of lattice vibrations in SrTiO3. Neutron scattering continues to play a vital role in characterizing lattice vibrations in perovskites owing to the simple cross section and the wide range of energy resolutions achievable with current neutron instrumentation. We discuss the dynamics that drive the phase transitions in the relaxors and organic-inorganic lead-halides in terms of neutron scattering and compare them to those in phase transitions associated with a 'central peak' and also a soft mode. We review some of the past experimental work on these materials and present new data from high-resolution time-of-flight backscattering spectroscopy taken on organic-inorganic perovskites. We will show that the structural transitions in disordered lead-based perovskites are driven by a broad frequency band of excitations.

Lifetime-shortened acoustic phonons and static order at the Brillouin zone boundary in the organic-inorganic perovskite CH3NH3PbCl3.

Lead halide hybrid perovskites consist of an inorganic framework hosting a molecular cation located in the interstitial space. These compounds have been extensively studied as they have been identified as promising materials for photovoltaic applications with the interaction between the molecular cation and the inorganic framework implicated as influential for the electronic properties. CH3NH3PbCl3 undergoes two structural transitions from a high temperature cubic unit cell to a tetragonal phase at 177 K and then a subsequent orthorhombic transition at 170 K. We have measured the low-frequency lattice dynamics using neutron spectroscopy and observe an energy broadening in the acoustic phonon linewidth towards the high-symmetry point Q X = ( 2 , 1 2 , 0 ) when approaching the transitions. Concomitant with these zone boundary anomalies is a hardening of the entire acoustic phonon branch measured in the q → 0 limit near the (2, 0, 0) Bragg position with decreasing temperature. Measurements of the elastic scattering at the Brillouin zone edges Q X = ( 2 , 1 2 , 0 ) , Q M = ( 3 2 , 1 2 , 0 ) , and Q R = ( 3 2 , 3 2 , 5 2 ) show Bragg peaks appearing below these structural transitions. Based on selection rules of neutron scattering, we suggest that the higher 177 K transition is displacive with a distortion of the local octahedral environment and the lower transition is a rigid tilt transition of the octahedra. We do not observe any critical broadening in energy or momentum, beyond resolution, of these peaks near the transitions. We compare these results to the critical properties reported near the structural transitions in other perovskites and particularly CsPbCl3 [Y. Fujii, S. Hoshino, Y. Yamada, and G. Shirane, Phys. Rev. B 9, 4549 (1974)]. We suggest that the simultaneous onset of static resolution-limited Bragg peaks at the zone boundaries and the changes in acoustic phonon energies near the zone center is evidence of a coupling between the inorganic framework and the molecular cation. The results also highlight the importance of displacive transitions in organic-inorganic hybrid perovskites.

Complementary Response of Static Spin-Stripe Order and Superconductivity to Nonmagnetic Impurities in Cuprates.

We report muon-spin rotation and neutron-scattering experiments on nonmagnetic Zn impurity effects on the static spin-stripe order and superconductivity of the La214 cuprates. Remarkably, it was found that, for samples with hole doping x≈1/8, the spin-stripe ordering temperature T_{so} decreases linearly with Zn doping y and disappears at y≈4%, demonstrating a high sensitivity of static spin-stripe order to impurities within a CuO_{2} plane. Moreover, T_{so} is suppressed by Zn in the same manner as the superconducting transition temperature T_{c} for samples near optimal hole doping. This surprisingly similar sensitivity suggests that the spin-stripe order is dependent on intertwining with superconducting correlations.

Coupled multiferroic domain switching in the canted conical spin spiral system Mn2GeO4.

Despite remarkable progress in developing multifunctional materials, spin-driven ferroelectrics featuring both spontaneous magnetization and electric polarization are still rare. Among such ferromagnetic ferroelectrics are conical spin spiral magnets with a simultaneous reversal of magnetization and electric polarization that is still little understood. Such materials can feature various multiferroic domains that complicates their study. Here we study the multiferroic domains in ferromagnetic ferroelectric Mn2GeO4 using neutron diffraction, and show that it features a double-Q conical magnetic structure that, apart from trivial 180o commensurate magnetic domains, can be described by ferromagnetic and ferroelectric domains only. We show unconventional magnetoelectric couplings such as the magnetic-field-driven reversal of ferroelectric polarization with no change of spin-helicity, and present a phenomenological theory that successfully explains the magnetoelectric coupling. Our measurements establish Mn2GeO4 as a conceptually simple multiferroic in which the magnetic-field-driven flop of conical spin spirals leads to the simultaneous reversal of magnetization and electric polarization.

A novel type of splayed ferromagnetic order observed in Yb2Ti2O7.

The pyrochlore insulator Yb2Ti2O7 has attracted the attention of experimentalists and theoreticians alike for about 15 years. Conflicting neutron diffraction data on the possible existence of magnetic Bragg reflections at low temperature have been published. Here we report the observation of magnetic Bragg reflections by neutron powder diffraction at 60 mK. The magnetic diffraction pattern is analyzed using representation theory. We find Yb2Ti2O7 to be a splayed ferromagnet as reported for Yb2Sn2O7, a sibling compound with also dominating ferromagnetic interactions as inferred from the positive Curie-Weiss temperature. However, the configuration of the magnetic moment components perpendicular to the easy axis is of the all-in-all-out type in Yb2Ti2O7 while it is two-in-two-out in the Yb2Sn2O7. An overall experimental picture of the magnetic properties emerges.

Correlated decay of triplet excitations in the Shastry-Sutherland compound SrCu2(BO3)2.

The temperature dependence of the gapped triplet excitations (triplons) in the 2D Shastry-Sutherland quantum magnet SrCu(2)(BO(3))(2) is studied by means of inelastic neutron scattering. The excitation amplitude rapidly decreases as a function of temperature, while the integrated spectral weight can be explained by an isolated dimer model up to 10 K. Analyzing this anomalous spectral line shape in terms of damped harmonic oscillators shows that the observed damping is due to a two-component process: one component remains sharp and resolution limited while the second broadens. We explain the underlying mechanism through a simple yet quantitatively accurate model of correlated decay of triplons: an excited triplon is long lived if no thermally populated triplons are nearby but decays quickly if there are. The phenomenon is a direct consequence of frustration induced triplon localization in the Shastry-Sutherland lattice.

Phase transition of the uniaxial disordered ferroelectric Sr(0.61)Ba(0.39)Nb(2)O(6).

We report a neutron scattering study of a ferroelectric phase transition in Sr0.61Ba0.39Nb2O6 (SBN-61). The ferroelectric polarization is along the crystallographic c-axis but the transverse acoustic branch propagating along the 〈1, 1, 0〉 direction does not show any anomaly associated with this transition. We find no evidence for a soft transverse optic phonon. We do, however, observe elastic diffuse scattering. The intensity of this scattering increases as the sample is cooled from a temperature well above the phase transition. The susceptibility associated with this diffuse scattering follows the anomaly of the dielectric permittivity of SBN-61 well. Below Tc the shape of this scattering is consistent with the scattering expected from ferroelectric domain walls. Our results suggest that despite apparent chemical disorder SBN-61 behaves as a classic order-disorder uniaxial ferroelectric with critical fluctuations in the range <10(-11) s.

Magnetoelastic excitations in the pyrochlore spin liquid Tb2Ti2O7.

At low temperatures, Tb2Ti2O7 enters a spin liquid state, despite expectations of magnetic order and/or a structural distortion. Using neutron scattering, we have discovered that in this spin liquid state an excited crystal field level is coupled to a transverse acoustic phonon, forming a hybrid excitation. Magnetic and phononlike branches with identical dispersion relations can be identified, and the hybridization vanishes in the paramagnetic state. We suggest that Tb2Ti2O7 is aptly named a "magnetoelastic spin liquid" and that the hybridization of the excitations suppresses both magnetic ordering and the structural distortion. The spin liquid phase of Tb2Ti2O7 can now be regarded as a Coulomb phase with propagating bosonic spin excitations.

The structure and low-energy phonons of the nonferroelectric mixed perovskite: BaMg1/3Ta2/3O3.

The structure of BaMg(1/3)Ta(2/3)O(3) (BMT) has been studied using x-ray scattering. The phonons have been measured and the results are similar to those of other materials with a perovskite structure such as PbMg(1/3)Nb(2/3)O(3) (PMN). The acoustic and lowest energy optic branches were measured but it was not possible to measure the branches of higher energy, possibly this is because they largely consist of oxygen motions. High-resolution inelastic measurements also showed that the diffuse scattering was strictly elastic and not directly related to the phonon spectra. Diffuse scattering was observed in BMT near the (H ± 1/2, K ± 1/2, L ± 1/2) points in the Brillouin zone and these had a characteristic cube shape. This arises from ordering of the B-site ions in BMT. Additional experiments revealed the diffuse scattering in BMT similar in shape to Bragg reflections at wavevectors of the form (H ± 1/3, K ± 1/3, L ± 1/3). Such reflections were also observed by Lufaso (2004 Chem. Mater. 16 2148) from powders and suggest that this structure of BMT consists of four differently oriented domains of a trigonal structure and results from a different ordering of the B-site ions from that responsible for the scattering at the (H ± 1/2, K ± 1/2, L ± 1/2) points. The results lead us to suggest that for BMT single crystals the bulk has the properties of a cubic perovskite, whereas the surface may have quite different structure from that of the bulk. This difference resembles the behaviour of cubic relaxors like PMN and PMN doped by PbTiO(3), where significant surface effects have been reported.

Power-law spin correlations in the pyrochlore antiferromagnet Tb(2)Ti(2)O(7).

We investigate the low-temperature state of the rare-earth pyrochlore Tb(2)Ti(2)O(7) using polarized neutron scattering. Tb(2)Ti(2)O(7) is often described as an antiferromagnetic spin liquid with spin correlations extending over lengths comparable to individual tetrahedra of the pyrochlore lattice. We confirm this picture at 20 K but find that at 0.05 K the data contain evidence of pinch-point scattering, suggesting that the low temperature state of Tb(2)Ti(2)O(7) has power-law spin correlations.

Coupling of magnetic and ferroelectric hysteresis by a multicomponent magnetic structure in Mn2GeO4.

The olivine compound Mn(2)GeO(4) is shown to feature both a ferroelectric polarization and a ferromagnetic magnetization that are directly coupled and point along the same direction. We show that a spin spiral generates ferroelectricity, and a canted commensurate order leads to weak ferromagnetism. Symmetry suggests that the direct coupling between the ferromagnetism and ferroelectricity is mediated by Dzyaloshinskii-Moriya interactions that exist only in the ferroelectric phase, controlling both the sense of the spiral rotation and the canting of the commensurate structure. Our study demonstrates how multicomponent magnetic structures found in magnetically frustrated materials like Mn(2)GeO(4) provide a new route towards functional materials that exhibit coupled ferromagnetism and ferroelectricity.

The magnetic structure of multiferroic BaMnF4.

The multiferroic material BaMnF(4) has been investigated with unpolarized and polarized neutron diffraction. The structure has been shown to be antiferromagnetic. The magnetic moments are aligned at 12° to the b direction in the bc plane, 3° different from the previously determined value. The ferromagnetic component that is indicative of the linear magnetoelectric effect was not observed.

Magnetic excitations of Fe(1+y)Se(x)Te(1-x) in magnetic and superconductive phases.

We have used inelastic neutron scattering and muon-spin rotation to compare the low energy magnetic excitations in single crystals of superconducting Fe(1.01)Se(0.50)Te(0.50) and non-superconducting Fe(1.10)Se(0.25)Te(0.75). We confirm the existence of a spin resonance in the superconducting phase of Fe(1.01)Se(0.50)Te(0.50), at an energy of 7 meV and a wavevector of (1/2, 1/2, 0). The non-superconducting sample exhibits two incommensurate magnetic excitations at (1/2, 1/2, 0) ± (0.18, - 0.18, 0) which rise steeply in energy, but no resonance is observed at low energies. A strongly dispersive low energy magnetic excitation is also observed in Fe(1.10)Se(0.25)Te(0.75) close to the commensurate antiferromagnetic ordering wavevector (1/2 - δ, 0, 1/2), where δ≈0.03. The magnetic correlations in both samples are found to be quasi-two-dimensional in character and persist well above the magnetic (Fe(1.10)Se(0.25)Te(0.75)) and superconducting (Fe(1.01)Se(0.50)Te(0.50)) transition temperatures.

Magnetic and orbital ordering in the spinel MnV2O4.

Neutron inelastic scattering and diffraction techniques have been used to study the MnV2O4 spinel system. Our measurements show the existence of two transitions to long-range ordered ferrimagnetic states, the first collinear and the second noncollinear. The lower temperature transition, characterized by development of antiferromagnetic components in the basal plane, is accompanied by a tetragonal distortion and the appearance of a gap in the magnetic excitation spectrum. The low-temperature noncollinear magnetic structure has been definitively resolved. Taken together, the crystal and magnetic structures indicate a staggered ordering of the V d orbitals. The anisotropy gap is a consequence of unquenched V orbital angular momentum.

Magnetism in geometrically frustrated YMnO3 under hydrostatic pressure studied with muon spin relaxation.

The ferroelectromagnet YMnO3 consists of weakly coupled triangular layers of S=2 spins. Below T(N) approximately equal to 70 K muon-spin relaxation data show two oscillatory relaxing signals due to magnetic order, with no purely relaxing signals resolvable (which would require different coexisting spin distributions). The transition temperature T(N) increases with applied hydrostatic pressure, even though the ordered moment decreases. These results suggest that pressure increases both the exchange coupling between the layers and the frustration within the layers.

Spin dynamics and magnetic order in magnetically frustrated Tb2Sn2O7.

We report a study of the geometrically frustrated magnetic material Tb2Sn2O7 by the positive muon-spin relaxation technique. No signature of a static magnetically ordered state is detected while neutron magnetic reflections are observed in agreement with a published report. This is explained by the dynamical nature of the ground state of Tb2Sn2O7: the Tb3+ magnetic moment characteristic fluctuation time is approximately 10(-10) s. The strong effect of the magnetic field on the muon-spin-lattice relaxation rate at low fields indicates a large field-induced increase of the magnetic density of states of the collective excitations at low energy.

Magnetization dynamics in the normal and superconducting phases of UPd(2)Al(3): II. Inferences on the nodal gap symmetry.

This paper provides an analysis of neutron inelastic scattering experiments on single crystals of UPd(2)Al(3). The emphasis is on establishing robust general inferences on the joint antiferromagnetic-superconducting state that characterizes UPd(2)Al(3) at low temperatures. A distinction is drawn between these conclusions and various theoretical perspectives of a more model-sensitive nature that have been raised in the literature.

Upward renormalization of fluctuations in CsMnBr3 with increasing temperature.

The temperature dependence of the spin-wave gap in the triangular antiferromagnet CsMnBr3 was studied above the three-dimensional ordering temperature T(N)=8.3 K along the main symmetry directions using inelastic neutron scattering. We find at T(N) two gapped dispersive modes, whose energy increases with temperature. Moreover, the width of the spin-wave band along the [110] direction increases also. In a second session, polarization analysis was applied in order to extract explicitly the components with in-plane and out-of-plane character. The results show that both gapped modes (with axial and radial symmetry) renormalize upwards with rising temperature. We show that this behavior is not compatible with spin-wave theory. In addition, we find a new magnetic anomaly in the paramagnetic phase.

Chiral fluctuations in MnSi above the Curie temperature.

Polarized neutrons are used to determine the antisymmetric part of the magnetic susceptibility in noncentrosymmetric MnSi. The paramagnetic fluctuations are found to be incommensurate with the chemical lattice and to have a chiral character. We argue that antisymmetric interactions must be taken into account to properly describe the critical dynamics in MnSi above T(C). The possibility of directly measuring the polarization dependent part of the dynamical susceptibility in a large class of compounds by polarized inelastic neutron scattering is outlined as it can yield evidence for antisymmetric interactions such as spin-orbit coupling in metals as well as in insulators.