We present a single-crystal neutron diffraction study on the Shastry-Sutherland lattice system TbB$_4$ at zero magnetic field and under pulsed high magnetic fields up to 35 T applied along the crystallographic $c$ axis. While our results confirm the magnetic structures at zero-field as well as those at the half- and full-magnetization plateaus, they offer new insight into the $\frac{2}{9}$- and $\frac{1}{3}$-magnetization plateaus observed in this system. A stripe model of polarized 4-spin-plaquettes whose stripe density proportionally increases with the macroscopic magnetization is in full agreement with the neutron diffraction data. Equally well suited alternative models exist which explain the observed Bragg peaks which are inherently limited in a pulsed high magnetic field experiment. We discuss the different intensity distribution in $Q$ space which can be used to distinguish these models in future experiments.
H.F. Fong, P. Bourges, Y. Sidis, L.P. Regnault, J. Bossy, A. Ivanov, D.L. Milius, I.A. Aksay, B. Keimer 1 Department of Physics, Princeton University, Princeton, NJ 08544 USA 2 Laboratoire Léon Brillouin, CEA-CNRS, CE Saclay, 91191 Gif sur Yvette, France 3 CEA Grenoble, Département de Recherche Fondamentale sur la matière Condensée, 38054 Grenoble cedex 9, France 4 CNRS-CRTBT, BP 166, 38042 Grenoble cedex 9, France 5 Institut Laue-Langevin, 156X, 38042 Grenoble Cedex 9, France 6 Department of Chemical Engineering, Princeton University, Princeton, NJ 08544, USA 7 Max-Planck-Institut für Festkörperforschung, 70569 Stuttgart, Germany
Disorder is important in the study of quantum spin liquids, but its role on the spin dynamics remains elusive. Here, we explore the disorder effect by investigating the magnetic-field dependence of the low-energy magnetic excitations in a triangular-lattice frustrated magnet YbZnGaO4 with inelastic neutron scattering. With an intermediate field of 2.5 T applied along the c axis, the broad continuum at zero field becomes more smeared both in energy and momentum. With a field up to 10 T, which fully polarizes the magnetic moments, we observe clear spin-wave excitations with a gap of similar to 1.4 meV comparable to the bandwidth. However, the spectra are significantly broadened. The excitation spectra both at zero and high fields can be reproduced by performing classical Monte Carlo simulations which take into account the disorder effect arising from the random site mixing of nonmagnetic Zn2+ and Ga3+ ions. These results elucidate the critical role of disorder in broadening the magnetic excitation spectra and mimicking the spin-liquid features in frustrated quantum magnets.
The dynamical properties of free and bound domain-wall excitations in Ising-chain materials have recently become the focus of intense research interest. New materials and spectrometers have made it possible to control the environment of coupled Ising chains by both effective internal and applied external fields, which can be both longitudinal and transverse, and thus to demonstrate how the resulting magnetic phase transitions and the nature of the associated excited states obey fundamental symmetry properties. In RbCoCl$_3$, the weakly coupled Ising chains form a triangular lattice whose frustrated geometry and magnetic ordering transitions at low temperature open new possibilities for the Ising-chain environment. We have investigated the structure and magnetism in RbCoCl$_3$ by high-resolution x-ray diffraction and neutron scattering measurements on powder and single crystal samples between 1.5 K and 300 K. Upon cooling, the Co$^{2+}$ spins develop one-dimensional antiferromagnetic correlations along the chain axis ($c$-axis) below 90 K. Below the first N\'eel temperature, $T_{N1}$ = 28 K, a partial 3D magnetic order sets in, with propagation vector ${\vec k}_1$ = (1/3,1/3,1), the moments aligned along the $c$-axis and every third chain uncorrelated from its neighbours. Only below a second magnetic phase transition at $T_{N2}$ = 13 K does the system achieve a fully ordered state, with two additional propagation vectors: ${\vec k}_2$ = (0,0,1) establishes a "honeycomb" $c$-axis order, in which 1/3 of the chains are subject to a strong effective mean field due to their neighbours whereas 2/3 experience no net field, while ${\vec k}_3$ = (1/2,0,1) governs a small, staggered in-plane ordered moment. We conclude that RbCoCl$_3$ is an excellent material to study the physics of Ising chains in a wide variety of temperature-controlled environments.
Inelastic neutron scattering spectra in the antiferromagnetic ferroborates Nd1-xTbxFe3(BO3)(4) (x = 0, 0.1, 0.2, and 1) reveal various magnetic excitations of the interacting iron and rare-earth subsystems. We observe an evolution of the magnetic system from "easy-plane", in the Tb-free (x = 0) case, to "easy-axis" anisotropy for samples substituted with Tb. The spectra show hybridized Fe and Nd branches, which are determined by the Fe-Nd exchange splitting of the ground-state Nd3+ doublet. In the easy-plane configuration, near the Brillouin zone center, there are two different pairs of anticrossing quasiacoustic Fe and Nd modes in contrast to the easy-axis state, where the two corresponding pairs of the branches are degenerated. The high-energy (exchange) branches are similar in both spin configurations. The Ising-type anisotropy of the Tb ion prevents the magnetic moment from precession. The increasing of the Tb content changes the effective magnetic anisotropy and stabilizes the easy-axis state. The spin-wave dispersion in the substituted and pure TbFe3(BO3)(4) compounds, which have the same, easy-axis magnetic structure, but different crystal symmetry, strongly differ. The observed spectra were analysed in the frame of linear spin-wave theory and the exchange parameters were determined.
We use polarized inelastic neutron scattering to study the spin-excitation anisotropy in the bilayer iron-based superconductor CaKFe4As4 (T-c = 35 K). In the superconducting state, both odd and even L modulations of spin resonance have been observed in our previous unpolarized neutron-scattering experiments [Xie et al., Phys. Rev. Lett. 120, 267003 (2018)]. Here we find that the high-energy even mode (similar to 18 meV) is isotropic in spin space, but the low-energy odd modes consist of a c-axis polarized mode around 9 meV along with another partially overlapped in-plane mode around 12 meV. We argue that such spin anisotropy is induced by the spin-orbit coupling in the spin-vortex-type fluctuations of this unique compound. The spin anisotropy is strongly affected by the superconductivity, where it is weak below 6 meV in the normal state and then transferred to higher energy and further enhanced in the odd modes of spin resonance below T-c.
Combining inelastic neutron and x-ray scattering with atomic scale simulation, we report on a comprehensive study of the lattice dynamics and its relationship with the low thermal conductivity of the o-Al13Co4 phase, a periodic approximant (about 100 atoms per cell) to a decagonal quasicrystal. The obtained experimental data, phonon lifetimes, and temperature-independent lattice thermal conductivity can only be fully described by molecular dynamics simulations, using oscillating pair potential, when the disorder of 12 Al sites is properly taken into account. Our results pave the way for a detailed understanding of materials where structural complexity and local disorder are at play.
Tb2Ti2O7 presents an ongoing conundrum in the study of rare-earth pyrochlores. Despite the expectation that it should be the prototypical unfrustrated noncollinear Ising antiferromagnet on the pyrochlore lattice, it presents a puzzling correlated state that persists to the lowest temperatures. Effects which can reintroduce frustration or fluctuations are therefore sought, and quadrupolar operators have been implicated. One consequence of strong quadrupolar effects is the possible coupling of magnetic and lattice degrees of freedom, and it has previously been shown that a hybrid magnetoelastic mode with both magnetic and phononic character is formed in Tb2Ti2O7 by the interaction of a crystal field excitation with a transverse-acoustic phonon. Here, using polarized and unpolarized inelastic neutron scattering, we present a detailed characterization of the magnetic and phononic branches of this magnetoelastic mode, particularly with respect to their composition, the anisotropy of any magnetic fluctuations, and also the temperature dependence of the different types of fluctuation that are involved. We also examine the dispersion relations of the exciton branches that develop from the crystal field excitation in the same temperature regime that the coupled mode appears, and find three quasidispersionless branches where four are expected, each with a distinctive structure factor indicating that they are nonetheless cooperative excitations. We interpret the overall structure of the spectrum as containing four branches, one hybridized with the phonons and gaining a strong dispersion, and three remaining dispersionless.
Spin wave dispersion in the frustrated fcc type-III antiferromagnet MnS_2 has been determined by inelastic neutron scattering using a triple-axis spectrometer. Existence of multiple spin wave branches, with significant separation between high-energy and low-energy modes highlighting the intrinsic magnetic frustration effect on the fcc lattice, is explained in terms of a spin wave analysis carried out for the antiferromagnetic Heisenberg model for this S=5/2 system with nearest and next-nearest-neighbor exchange interactions. Comparison of the calculated dispersion with spin wave measurement also reveals small suppression of magnetic frustration resulting from reduced exchange interaction between frustrated spins, possibly arising from anisotropic deformation of the cubic structure.
We use inelastic neutron scattering to study the low-energy spin excitations of the 112-type iron pnictide Ca_{0.82}La_{0.18}Fe_{0.96}Ni_{0.04}As_{2} with bulk superconductivity below T_{c}=22 K. A two-dimensional spin resonance mode is found around E=11 meV, where the resonance energy is almost temperature independent and linearly scales with T_{c} along with other iron-based superconductors. Polarized neutron analysis reveals the resonance is nearly isotropic in spin space without any L modulations. Because of the unique monoclinic structure with additional zigzag arsenic chains, the As 4p orbitals contribute to a three-dimensional hole pocket around the Γ point and an extra electron pocket at the X point. Our results suggest that the energy and momentum distribution of the spin resonance does not directly respond to the k_{z} dependence of the fermiology, and the spin resonance intrinsically is a spin-1 mode from singlet-triplet excitations of the Cooper pairs in the case of weak spin-orbital coupling.
The magnetic properties of the cobaltite BaCo2(AsO4)2, a good realization of the quasi two-dimensional frustrated honeycomb-lattice system with strong planar anisotropy, have been reinvestigated by means of spherical neutron polarimetry with CRYOPAD. From accurate measurements of polarization matrices both on elastic and inelastic contributions as a function of the scattering vector Q, we have been able to determine the low-temperature magnetic structure of BaCo2(AsO4)2 and reveal its puzzling in-plane spin dynamics. Surprisingly, the ground-state structure (described by an incommensurate propagation vector k1=(kx,0,kz), with kx=0.270±0.005 and kz≈−1.31) appears to be a quasi-collinear structure, and not a simple helix, as previously determined. In addition, our results have revealed the existence of a non-negligible out-of-plane moment component ≈0.25μB/Co2+, representing about 10% of the in-plane component, as demonstrated by the presence of finite off-diagonal elements Pyz and Pzy of the polarization matrix, both on elastic and inelastic magnetic contributions. Despite a clear evidence of the existence of a slightly inelastic contribution of structural origin superimposed to the magnetic excitations at the scattering vectors Q=(0.27,0,3.1) and Q=(0.73,0,0.8) (energy transfer ΔE≈2.3 meV), no strong inelastic nuclear-magnetic interference terms could be detected so far, meaning that the nuclear and magnetic degrees of freedom have very weak cross-correlations. The strong inelastic Pyz and Pzy matrix elements can be understood by assuming that the magnetic excitations in BaCo2(AsO4)2 are spin waves associated with trivial anisotropic precessions of the magnetic moments involved in the canted incommensurate structure.
A review of recent state-of-the-art pulsed field experiments performed on URu2Si2 under a magnetic field applied along its easy magnetic axis c is given. Resistivity, magnetization, magnetic susceptibility, Shubnikov-de Haas, and neutron diffraction experiments are presented, permitting to emphasize the relationship between Fermi surface reconstructions, the destruction of the hidden-order and the appearance of a spin-density wave state in a high magnetic field.
Yu Song, Xingye Lu, L.-P. Regnault, Yixi Su, Hsin-Hua Lai, Wen-Jun Hu, Qimiao Si, and Pengcheng Dai Department of Physics and Astronomy and Rice Center for Quantum Materials, Rice University, Houston, Texas 77005, USA Center for Advanced Quantum Studies and Department of Physics, Beijing Normal University, Beijing 100875, China Institut Laue Langevin, 71 Avenue des Martyrs, 38042 Grenoble, France Jülich Centre for Neutron Science, Forschungszentrum Jülich GmbH, Outstation at MLZ, D-85747 Garching, Germany
Since the seminal ideas of Berezinskii, Kosterlitz and Thouless, topological excitations have been at the heart of our understanding of a whole novel class of phase transitions. In most cases, those transitions are controlled by a single type of topological objects. There are, however, some situations, still poorly understood, where two dual topological excitations fight to control the phase diagram and the transition. Finding experimental realizations of such cases is thus of considerable interest. We show here that this situation occurs in BaCo 2 V 2 O 8 , a spin-1/2 Ising-like quasi-one-dimensional antiferromagnet, when subjected to a uniform magnetic field transverse to the Ising axis. Using neutron scattering experiments, we measure a drastic modification of the quantum excitations beyond a critical value of the magnetic field. This quantum phase transition is identified, through a comparison with theoretical calculations, to be a transition between two different types of solitonic topological object, which are captured by different components of the dynamical structure factor.
We present the first long-duration and high duty cycle 40-T pulsed-field cryomagnet addressed to single crystal neutron diffraction experiments at temperatures down to 2 K. The magnet produces a horizontal field in a bi-conical geometry, ±15° and ±30° upstream and downstream of the sample, respectively. Using a 1.15 MJ mobile generator, magnetic field pulses of 100 ms length are generated in the magnet, with a rise time of 23 ms and a repetition rate of 6-7 pulses per hour at 40 T. The setup was validated for neutron diffraction on the CEA-CRG three-axis spectrometer IN22 at the Institut Laue Langevin.
Unconventional superconductivity typically emerges in the presence of quasidegenerate ground states, and the associated intense fluctuations are likely responsible for generating the superconducting state. Here we use polarized neutron scattering to study the spin space anisotropy of spin excitations in Fe1.07Te exhibiting bicollinear antiferromagnetic (AF) order, the parent compound of FeTe1-xSex superconductors. We confirm that the low- energy spin excitations are transverse spin waves, consistent with a local-moment origin of the bicollinear AF order. While the ordered moments lie in the ab plane in Fe1.07Te, it takes less energy for them to fluctuate out of plane, similar to BaFe2As2 and NaFeAs. At energies above E greater than or similar to 20 meV, we find magnetic scattering to be dominated by an isotropic continuum that persists up to at least 50 meV. Although the isotropic spin excitations cannot be ascribed to spin waves from a long-range-ordered local-moment antiferromagnet, the continuum can result from the bicollinear magnetic order ground state of Fe1.07Te being quasidegenerate with plaquette magnetic order.
In the version of this Letter originally published, the year for ref. 30 was incorrectly listed as 2009; it should have been 2004. This has now been corrected.
Engineering lattice thermal conductivity requires to control the heat carried by atomic vibration waves, the phonons. The key parameter for quantifying it is the phonon lifetime, limiting the travelling distance, whose determination is however at the limits of instrumental capabilities. Here, we show the achievement of a direct quantitative measurement of phonon lifetimes in a single crystal of the clathrate Ba 7.81 Ge 40.67 Au 5.33 , renowned for its puzzling ‘glass-like’ thermal conductivity. Surprisingly, thermal transport is dominated by acoustic phonons with long lifetimes, travelling over distances of 10 to 100 nm as their wave-vector goes from 0.3 to 0.1 Å −1 . Considering only low-energy acoustic phonons, and their observed lifetime, leads to a calculated thermal conductivity very close to the experimental one. Our results challenge the current picture of thermal transport in clathrates, underlining the inability of state-of-the-art simulations to reproduce the experimental data, thus representing a crucial experimental input for theoretical developments.
Magnetic excitations and exchange interactions in multiferroic NdFe3(BO3)(4) were studied by inelastic neutron scattering in the phase with commensurate antiferromagnetic structure. The observed spectra were analyzed in the frame of the linear spin-wave theory. It was shown that only the model, which includes the exchange interactions within eight coordination spheres, describes satisfactorily all observed dispersion curves. The calculation showed that the spin-wave dynamics is governed by the strongest antiferromagnetic intra-chain interaction and three almost the same inter-chain interactions. Other interactions, including ferromagnetic exchange, appeared to be insignificant. The overall energy balance of the antiferromagnetic inter-chain exchange interactions, which couple the moments from the adjacent ferromagnetic layers as well as within a layer, stabilizes ferromagnetic arrangement in the latter. It demonstrates that the pathway geometry plays a crucial role in forming of the magnetic structure. (C) 2017 Published by Elsevier B.V.
In the spinel compound GeCo2O4, the Co2+ pyrochlore sublattice presents remarkable magnetic-field-induced behaviors that we unveil through neutron and x-ray single-crystal diffraction. The Neel-ordered magnetic phase is entered through a structural lowering of the cubic symmetry. In this phase, when a magnetic field is applied along a 2-fold cubic direction, a spin-flop transition of one-fourth of the magnetic moments releases the magnetic frustration and triggers magnetostructural effects. At high field, these ultimately lead to an unusual spin reorientation associated with structural changes.