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CrBr_{3} is an excellent realization of the two-dimensional honeycomb ferromagnet, which offers a bosonic equivalent of graphene with Dirac magnons and topological character. We perform inelastic neutron scattering measurements using state-of-the-art instrumentation to update 50-year-old data, thereby enabling a definitive comparison both with recent experimental claims of a significant gap at the Dirac point and with theoretical predictions for thermal magnon renormalization. We demonstrate that CrBr_{3} has next-neighbor J_{2} and J_{3} interactions approximately 5% of J_{1}, an ideal Dirac magnon dispersion at the K point, and the associated signature of isospin winding. The magnon lifetime and the thermal band renormalization show the universal T^{2} evolution expected from an interacting spin-wave treatment, but the measured dispersion lacks the predicted van Hove features, pointing to the need for more sophisticated theoretical analysis.
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This corrects the article DOI: 10.1103/PhysRevLett.116.217201.
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Establishing the physical mechanism governing exchange interactions is fundamental for exploring exotic phases such as quantum spin liquids in real materials. In this Letter, we address exchange interactions in Sr_{2}CuTe_{x}W_{1-x}O_{6}, a series of double perovskites that realize a spin-1/2 square lattice and are suggested to harbor a quantum spin liquid ground state arising from the random distribution of nonmagnetic ions. Our ab initio multireference configuration interaction calculations show that replacing Te atoms with W atoms changes the dominant couplings from nearest to next-nearest neighbor due to the crucial role of unoccupied states of the nonmagnetic ions in the super-superexchange mechanism. Combined with spin-wave theory simulations, our calculated exchange couplings provide an excellent description of the inelastic neutron scattering spectra of the parent compounds, as well as explaining that the magnetic excitations in Sr_{2}CuTe_{0.5}W_{0.5}O_{6} emerge from bond-disordered exchange couplings. Our results demonstrate the crucial role of the nonmagnetic cations in exchange interactions paving the way to further explore quantum spin liquid phases in bond-disordered materials.
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The spin-1/2 kagome antiferromagnet is an archetypal frustrated system predicted to host a variety of exotic magnetic states. We show using neutron scattering measurements that deuterated vesignieite BaCu_{3}V_{2}O_{8}(OD)_{2}, a fully stoichiometric S=1/2 kagome magnet with <1% lattice distortion, orders magnetically at T_{N}=9 K into a multi-k coplanar variant of the predicted triple-k octahedral structure. We find that this structure is stabilized by a dominant antiferromagnetic third-neighbor exchange J_{3} with minor first- or second-neighbor exchanges. The spin-wave spectrum is well described by a J_{3}-only model including a tiny symmetric exchange anisotropy.
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Excitations in a spin ice behave as magnetic monopoles, and their population and mobility control the dynamics of a spin ice at low temperature. CdEr_{2}Se_{4} is reported to have the Pauling entropy characteristic of a spin ice, but its dynamics are three orders of magnitude faster than the canonical spin ice Dy_{2}Ti_{2}O_{7}. In this Letter we use diffuse neutron scattering to show that both CdEr_{2}Se_{4} and CdEr_{2}S_{4} support a dipolar spin ice state-the host phase for a Coulomb gas of emergent magnetic monopoles. These Coulomb gases have similar parameters to those in Dy_{2}Ti_{2}O_{7}, i.e., dilute and uncorrelated, and so cannot provide three orders faster dynamics through a larger monopole population alone. We investigate the monopole dynamics using ac susceptometry and neutron spin echo spectroscopy, and verify the crystal electric field Hamiltonian of the Er^{3+} ions using inelastic neutron scattering. A quantitative calculation of the monopole hopping rate using our Coulomb gas and crystal electric field parameters shows that the fast dynamics in CdEr_{2}X_{4} (X=Se, S) are primarily due to much faster monopole hopping. Our work suggests that CdEr_{2}X_{4} offer the possibility to study alternative spin ice ground states and dynamics, with equilibration possible at much lower temperatures than the rare earth pyrochlore examples.
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A hidden order that emerges in the frustrated pyrochlore Tb_{2+x}Ti_{2-x}O_{7+y} with T_{c}=0.53 K is studied using specific heat, magnetization, and neutron scattering experiments on a high-quality single crystal. Semiquantitative analyses based on a pseudospin-1/2 Hamiltonian for ionic non-Kramers magnetic doublets demonstrate that it is an ordered state of electric quadrupole moments. The elusive spin liquid state of the nominal Tb_{2}Ti_{2}O_{7} is most likely a U(1) quantum spin-liquid state.
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Sr_{2}CuTeO_{6} presents an opportunity for exploring low-dimensional magnetism on a square lattice of S=1/2 Cu^{2+} ions. We employ ab initio multireference configuration interaction calculations to unravel the Cu^{2+} electronic structure and to evaluate exchange interactions in Sr_{2}CuTeO_{6}. The latter results are validated by inelastic neutron scattering using linear spin-wave theory and series-expansion corrections for quantum effects to extract true coupling parameters. Using this methodology, which is quite general, we demonstrate that Sr_{2}CuTeO_{6} is an almost ideal realization of a nearest-neighbor Heisenberg antiferromagnet but with relatively weak coupling of 7.18(5) meV.
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High-resolution neutron resonance spin-echo measurements of superfluid 4He show that the roton energy does not have the same temperature dependence as the inverse lifetime. Diagrammatic analysis attributes this to the interaction of rotons with thermally excited phonons via both four- and three-particle processes, the latter being allowed by the broken gauge symmetry of the Bose-condensate. The distinct temperature dependence of the roton energy at low temperatures suggests that the net roton-phonon interaction is repulsive.
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Polarized and unpolarized neutron scattering experiments on the frustrated ferromagnetic spin-1/2 chain LiCuVO4 show that the phase transition at H(Q) of 8 T is driven by quadrupolar fluctuations and that dipolar correlations are short range with moments parallel to the applied magnetic field in the high-field phase. Heat-capacity measurements evidence a phase transition into this high-field phase, with an anomaly clearly different from that at low magnetic fields. Our experimental data are consistent with a picture where the ground state above H(Q) has a next-nearest neighbor bond-nematic order along the chains with a fluidlike coherence between weakly coupled chains.
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Magnetic susceptibility, NMR, muon spin relaxation, and inelastic neutron scattering measurements show that kapellasite, Cu3Zn(OH)6Cl2, a geometrically frustrated spin-1/2 kagome antiferromagnet polymorphic with herbertsmithite, is a gapless spin liquid showing unusual dynamic short-range correlations of noncoplanar cuboc2 type which persist down to 20 mK. The Hamiltonian is determined from a fit of a high-temperature series expansion to bulk susceptibility data and possesses competing exchange interactions. The magnetic specific heat calculated from these exchange couplings is in good agreement with experiment. The temperature dependence of the magnetic structure factor and the muon relaxation rate are calculated in a Schwinger-boson approach and compared to experimental results.
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Inelastic neutron scattering measurements show the existence of a strong two-spinon continuum in the frustrated ferromagnetic spin-1/2 chain compound LiCuVO4. The dynamic magnetic susceptibility is well described by a mean-field model of two coupled interpenetrating antiferromagnetic Heisenberg chains. The extracted values of the exchange integrals are in good agreement with the static magnetic susceptibility data and an earlier spin-wave description of the bound state near the lower boundary of the two-spinon continuum. In addition, there is clear evidence for a four-spinon continuum at high energies.
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The complexity embedded in condensed matter fertilizes the discovery of new states of matter, enriched by ingredients like frustration. Illustrating examples in magnetic systems are Kitaev spin liquids, skyrmions phases, or spin ices. These unconventional ground states support exotic excitations, for example the magnetic charges in spin ices, also called monopoles. Here, we propose a mechanism to inject monopoles in a spin ice at equilibrium through a staggered magnetic field. We show theoretically, and demonstrate experimentally in the Ho2Ir2O7 pyrochlore iridate, that it results in the stabilization of a monopole crystal, which exhibits magnetic fragmentation. In this new state of matter, the magnetic moment fragments into an ordered part and a persistently fluctuating one. Compared to conventional spin ices, the different nature of the excitations in this fragmented state opens the way to tunable field-induced and dynamical behaviors.Exploring unconventional magnetism facilities both fundamental understanding of materials and their real applications. Here the authors demonstrate that a magnetic monopole crystal is stabilized by a staggered magnetic field in the pyrochlore iridate Ho2Ir2O7, leading to a fragmented magnetization.
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We report the first observation of two-dimensional layer modes in both fully filled and partially filled aerogel. Using complementary high-energy resolution and high statistical precision neutron scattering instruments, and two different 87% porous aerogel samples, we show that the three-dimensional (3D) phonon-roton excitation energies and lifetimes of liquid 4He in aerogel are the same as in bulk 4He within current precision. The layer modes are the excitations that distinguish aerogel from the bulk rather than a difference in the 3D roton energy.
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Using inelastic neutron scattering, we have observed well-defined phonon-roton ( p-r) excitations in superfluid 4He in Vycor over a wide wave-vector range, 0.3
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The origin of the well-defined collective excitations found in liquid para-H2 by recent experiments is investigated. The persistence of their relatively long lifetimes down to microscopic scales is well accounted for by calculations carried out by means of path-integral-centroid molecular dynamics. In contrast only overdamped excitations are found in calculations carried within the classical limit. The results provide fully quantitative evidence of quantum effects on the dynamics of a simple liquid.
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We infer that soft-x-ray absorption spectroscopy is a versatile method for the determination of the crystal-field ground state symmetry of rare earth heavy fermion systems, complementing neutron scattering. Using realistic and universal parameters, we provide a theoretical mapping between the polarization dependence of Ce M(4,5) spectra and the charge distribution of the Ce 4f states. The experimental resolution can be orders of magnitude larger than the 4f crystal-field splitting itself. To demonstrate the experimental feasibility of the method, we investigated CePd2Si2, thereby settling an existing disagreement about its crystal-field ground state.