Magnetic excitations in frustrated fcc type-III antiferromagnet MnS2.

Spin wave dispersion in the frustrated fcc type-III antiferromagnet MnS2 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.

40-Tesla pulsed-field cryomagnet for single crystal neutron diffraction.

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.

Polarized-neutron investigation of magnetic ordering and spin dynamics in BaCo2(AsO4)2 frustrated honeycomb-lattice magnet.

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 [Formula: see text], with [Formula: see text] and [Formula: see text]) 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 [Formula: see text]/Co2+, representing about 10% of the in-plane component, as demonstrated by the presence of finite off-diagonal elements [Formula: see text] and [Formula: see text] 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 [Formula: see text] and [Formula: see text] (energy transfer [Formula: see text] 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 [Formula: see text] and [Formula: see text] 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.

Field-induced spin-density wave beyond hidden order in URu2Si2.

URu2Si2 is one of the most enigmatic strongly correlated electron systems and offers a fertile testing ground for new concepts in condensed matter science. In spite of >30 years of intense research, no consensus on the order parameter of its low-temperature hidden-order phase exists. A strong magnetic field transforms the hidden order into magnetically ordered phases, whose order parameter has also been defying experimental observation. Here, thanks to neutron diffraction under pulsed magnetic fields up to 40 T, we identify the field-induced phases of URu2Si2 as a spin-density-wave state. The transition to the spin-density wave represents a unique touchstone for understanding the hidden-order phase. An intimate relationship between this magnetic structure, the magnetic fluctuations and the Fermi surface is emphasized, calling for dedicated band-structure calculations.

Longitudinal and transverse Zeeman ladders in the Ising-like chain antiferromagnet BaCo(2)V(2)O(8).

We explore the spin dynamics emerging from the Néel phase of the chain compound antiferromagnet BaCo(2)V(2)O(8). Our inelastic neutron scattering study reveals unconventional discrete spin excitations, so-called Zeeman ladders, understood in terms of spinon confinement, due to the interchain attractive linear potential. These excitations consist of two interlaced series of modes, respectively, with transverse and longitudinal polarization. The latter, which correspond to a longitudinal fluctuation of the ordered moment, have no classical counterpart and are related to the zero-point fluctuations that weaken the ordered moment in weakly coupled quantum chains. Our analysis reveals that BaCo(2)V(2)O(8), with moderate Ising anisotropy and sizable interchain interactions, remarkably fulfills the conditions necessary for the observation of discrete long-lived longitudinal excitations.

Magneto- to electroactive transmutation of spin waves in ErMnO3.

The low-energy dynamical properties of the multiferroic hexagonal perovskite ErMnO3 have been studied by inelastic neutron scattering as well as terahertz and far infrared spectroscopies on a synchrotron source. From these complementary techniques, we have determined the magnon and crystal field spectra and identified a zone center magnon excitable only by the electric field of an electromagnetic wave. Using a comparison with the isostructural YMnO3 compound and crystal field calculations, we propose that this dynamical magnetoelectric process is due to the hybridization of a magnon with an electroactive crystal field transition.

Magnetic structure of phase II in U(Ru(0.96)Rh(0.04))2Si2 determined by neutron diffraction under pulsed high magnetic fields.

We report neutron diffraction measurements on U(Ru(0.96)Rh(0.04))(2)Si(2) single crystal under pulsed high magnetic fields up to 30 T applied along the tetragonal c axis. The high-field experiments revealed that the field-induced phase II above 26 T corresponds to a commensurate up-up-down ferrimagnetic structure characterized by the wave vector q=(2/3,0,0) with the magnetic moments parallel to the c axis, which naturally explains the one-third magnetization plateau and the substantially changed Fermi surface in phase II. This a-axis modulated magnetic structure indicates that the phase II near the hidden order phase is closely related to the characteristic incommensurate magnetic fluctuations at Q(1)=(0.6,0,0) in the pure system URu(2)Si(2), in contrast to the pressure-induced antiferromagnetic order at Q(0)=(1,0,0).

Lifetime of gapped excitations in a collinear quantum antiferromagnet.

We demonstrate that local modulations of magnetic couplings have a profound effect on the temperature dependence of the relaxation rate of optical magnons in a wide class of antiferromagnets in which gapped excitations coexist with acoustic spin waves. In a two-dimensional collinear antiferromagnet with an easy-plane anisotropy, the disorder-induced relaxation rate of the gapped mode, Γ(imp)≈Γ(0)+A(TlnT)2, greatly exceeds the magnon-magnon damping, Γ(m-m)≈BT5, negligible at low temperatures. We measure the lifetime of gapped magnons in a prototype XY antiferromagnet BaNi2(PO4)2 using a high-resolution neutron-resonance spin-echo technique and find experimental data in close accord with the theoretical prediction. Similarly strong effects of disorder in the three-dimensional case and in noncollinear antiferromagnets are discussed.

Macroscopic quantum coherence of the spin triplet in the spin-ladder compound Sr14Cu24O41.

We report the direct observation by inelastic neutron scattering experiments of a spin triplet of magnetic excitations in the response associated with the ladders in the composite cuprate Sr14Cu24O41. This appears as a peak at q(Q1D)=π and energy Δ1=32.5 meV, and we conjecture that all the triplets making up this conspicuous peak have the same phase and therefore interpret it as the signature of the occurrence of quantum coherence along the ladder direction between entangled spin pairs. From the comparison with previous neutron and x-ray data, we conclude that the temperature evolution of this mode is driven by the crystallization of holes into a charge density wave in the ladder sublattice.

Universal magnetic structure of the half-magnetization phase in Cr-based spinels.

Using an elastic neutron scattering technique under a pulsed magnetic field up to 30 T, we determined the magnetic structure in the half-magnetization plateau phase in the spinel CdCr2O4. The magnetic structure has a cubic P4{3}32 symmetry, which is the same as that observed in HgCr2O4. This suggests that despite their different zero-field ground states a universal field-induced spin-lattice coupling mechanism is at work in the Cr-based spinels.

Polarized-neutron-scattering study of the spin-wave excitations in the 3-k ordered phase of uranium antimonide.

The anisotropy of magnetic fluctuations propagating along the [1 1 0] direction in the ordered phase of uranium antimonide has been studied using polarized inelastic neutron scattering. The observed polarization behavior of the spin waves is a natural consequence of the longitudinal 3-k magnetic structure; together with recent results on the 3-k-transverse uranium dioxide, these findings establish this technique as an important tool to study complex magnetic arrangements. Selected details of the magnon excitation spectra of USb have also been reinvestigated, indicating the need to revise the currently accepted theoretical picture for this material.

Neutron diffraction study on the multiple magnetization plateaus in TbB4 under pulsed high magnetic field.

We present the first application of pulsed high magnetic fields up to 30 T for neutron diffraction experiments. As the first study, field variations of a couple of magnetic Bragg reflections have successfully been measured in the frustrated antiferromagnet TbB4. The results show that the conventional models fail, and a model, which is a mixture of the XY- and the Ising-type moments, matches for the half-magnetization state. We deduce an interaction that stabilizes an orthogonal moment arrangement as an origin of the unusual magnetization plateaus. Our results demonstrate the powerfulness of the present pulsed magnetic fields neutron diffraction system.

Extended universal finite-T renormalization of excitations in a class of one-dimensional quantum magnets.

Temperature dependencies of gap energies and magnon lifetimes are measured in the quasi-one-dimensional S=1/2 gapped quantum magnets (CH3)(2)CHNH(3)CuCL(3) (IPA-CuCl(3), where IPA denotes isopropyl ammonium) and Cu(2)Cl(4).D(8)C(4)SO(2) (Sul-Cu(2)Cl(4)) using inelastic neutron scattering. The results are compared to those found in literature for S=1 Haldane spin chain materials and to theoretical calculations for the O(3)- and O(N)- quantum nonlinear sigma-models. It is found that when the T=0 energy gap Delta is used as the temperature scale, all experimental and theoretical curves are identical to within system-dependent but temperature-independent scaling factors of the order of unity. This quasi-universality extends over a surprising broad T range, at least up to kappaT approximately 1.5 Delta.

Excitations in a four-leg antiferromagnetic Heisenberg spin tube.

Inelastic neutron scattering is used to investigate magnetic excitations in the quasi-one-dimensional quantum spin-liquid system Cu(2)Cl(4).D(8)C(4)SO(2). Contrary to previously conjectured models that relied on bond-alternating nearest-neighbor interactions in the spin chains, the dominant interactions are actually next-nearest-neighbor in-chain antiferromagnetic couplings. The appropriate Heisenberg Hamiltonian is equivalent to that of a S=1/2 4-leg spin-tube with almost perfect one dimensionality and no bond alternation. A partial geometric frustration of rung interactions induces a small incommensurability of short-range spin correlations.

Polarized-neutron study of spin dynamics in the Kondo insulator YbB12.

Inelastic neutron scattering experiments have been performed on the archetype compound YbB(12), using neutron polarization analysis to separate the magnetic signal from the phonon background. With decreasing temperature, components characteristic for a single-site spin-fluctuation dynamics are suppressed, giving place to specific, strongly Q-dependent, low-energy excitations near the spin-gap edge. This crossover is discussed in terms of a simple crystal-field description of the incoherent high-temperature state and a predominantly local mechanism for the formation of the low-temperature singlet ground state.

Quantum dynamics and entanglement of spins on a square lattice.

Bulk magnetism in solids is fundamentally quantum mechanical in nature. Yet in many situations, including our everyday encounters with magnetic materials, quantum effects are masked, and it often suffices to think of magnetism in terms of the interaction between classical dipole moments. Whereas this intuition generally holds for ferromagnets, even as the size of the magnetic moment is reduced to that of a single electron spin (the quantum limit), it breaks down spectacularly for antiferromagnets, particularly in low dimensions. Considerable theoretical and experimental progress has been made in understanding quantum effects in one-dimensional quantum antiferromagnets, but a complete experimental description of even simple two-dimensional antiferromagnets is lacking. Here we describe a comprehensive set of neutron scattering measurements that reveal a non-spin-wave continuum and strong quantum effects, suggesting entanglement of spins at short distances in the simplest of all two-dimensional quantum antiferromagnets, the square lattice Heisenberg system.

Magnetic excitations in multiferroic TbMnO3: evidence for a hybridized soft mode.

The magnetic excitations in multiferroic TbMnO3 have been studied by inelastic neutron scattering in the spiral and sinusoidally ordered phases. At the incommensurate magnetic zone center of the spiral phase, we find three low-lying magnons whose character has been fully determined using neutron-polarization analysis. The excitation at the lowest energy is the sliding mode of the spiral, and two modes at 1.1 and 2.5 meV correspond to rotations of the spiral rotation plane. These latter modes are expected to couple to the electric polarization. The 2.5 meV mode is in perfect agreement with recent infrared-spectroscopy data giving strong support to its interpretation as a hybridized phonon-magnon excitation.

Excitations from a Bose-Einstein condensate of magnons in coupled spin ladders.

The weakly coupled quasi-one-dimensional spin ladder compound (CH3)2CHNH3CuCl3 is studied by neutron scattering in magnetic fields exceeding the critical field of Bose-Einstein condensation of magnons. Commensurate long-range order and the associated Goldstone mode are detected and found to be similar to those in reference to spin-dimer materials. However, for the upper two massive magnon branches, the observed behavior is totally different, culminating in a drastic collapse of excitation bandwidth beyond the transition point.

Dynamics of composite haldane spin chains in IPA-CuCl3.

Magnetic excitations in the quasi-one-dimensional antiferromagnet IPA-CuCl3 are studied by cold neutron inelastic scattering. Strongly dispersive gap excitations are observed. Contrary to previously proposed models, the system is best described as an asymmetric quantum spin ladder. The observed spectrum is interpreted in terms of composite Haldane spin chains. The key difference from actual S=1 chains is a sharp cutoff of the single-magnon spectrum at a certain critical wave vector.

Spin excitations in an anisotropic bond-alternating quantum s = 1 chain in a magnetic field: contrast to haldane spin chains.

Inelastic neutron scattering experiments on the S = 1 quasi-one-dimensional bond-alternating antiferromagnet Ni(C9D24N4)(NO2)ClO4 have been performed under magnetic fields below and above a critical field Hc at which the energy gap closes. Normal field dependence of Zeeman splitting of the excited triplet modes below Hc has been observed, but the highest mode is unusually small and smears out with increasing field. This can be explained by an interaction with a low-lying two magnon continuum at q(parallel) = pi that is present in dimerized chains but absent in uniform ones. Above Hc, we find only one excited mode, in stark contrast with three massive excitations previously observed in the structurally similar Haldane-gap material NDMAP [A. Zheludev, Phys. Rev. B 68, 134438 (2003)].