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Physical review. B, Condensed matter

Measurement of the spin-excitation continuum in one-dimensional KCuF3 using neutron scattering

D. M. Tennant, Roger Arthur Cowley, S. E. Nagler, Alexei M. Tsvelik

Published Nov 1, 1995• 157 citations
Publisher

Abstract

In this, and the following paper, we present the results of a detailed experimental investigation into the spin dynamics of the quasi-one-dimensional S=1/2 Heisenberg antiferromagnet ${\mathrm{KCuF}}_{3}$. In this paper we report results of inelastic neutron-scattering measurements made using the MARI time-of-flight spectrometer at the Rutherford Appleton Laboratory. Measurement of the magnetic excitation spectrum was made in both the low-temperature phase, where the chains are ordered together, and in the high-temperature phase, where the correlations between chains become unimportant. We compare our measurements with the M\"uller ansatz, which is identified with a two-spinon cross section, and find excellent agreement with this. The effect of temperature on the excitation continuum was also investigated. A series of measurements were made at temperatures ranging from 20 to 200 K. These results are compared to the predictions of field theory for the one-dimensional Heisenberg chain. Again good agreement is found with the theoretical predictions. In the following paper measurements of the low-energy scattering in the ordered phase, made on a triple-axis spectrometer, are presented.

DOI
10.1103/physrevb.52.13368

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In this, and the following paper, we present the results of a detailed experimental investigation into the spin dynamics of the quasi-one-dimensional S=1/2 Heisenberg antiferromagnet KCuF3{\mathrm{KCuF}}_{3}KCuF3​. In this paper we report results of inelastic neutron-scattering measurements made using the MARI time-of-flight spectrometer at the Rutherford Appleton Laboratory. Measurement of the magnetic excitation spectrum was made in both the low-temperature phase, where the chains are ordered together, and in the high-temperature phase, where the correlations between chains become unimportant. We compare our measurements with the M"uller ansatz, which is identified with a two-spinon cross section, and find excellent agreement with this. The effect of temperature on the excitation continuum was also investigated. A series of measurements were made at temperatures ranging from 20 to 200 K. These results are compared to the predictions of field theory for the one-dimensional Heisenberg chain. Again good agreement is found with the theoretical predictions. In the following paper measurements of the low-energy scattering in the ordered phase, made on a triple-axis spectrometer, are presented.
The magnetic excitations of a nearly ideal realization of a one-dimensional S=1/2 Heisenberg antiferromagnet, KCuF3{\mathrm{KCuF}}_{3}KCuF3​, have been studied by inelastic neutron scattering. The experimments were performed using the pulsed neutron source ISIS and show that the magnetic scattering occurs at energies well above the top of the linearized spin-wave band. This result shows that it is essential to take account of quantum effects in discussing the excitations. The results are in excellent accord with theoretical predictions for the dynamical correlation function.
The research presented here focuses on the theoretical investigation of spinons in quasi one-dimensional quantum spin chains from the perspective of neutron scattering, with emphasis placed on the calculation of dynamic spin structure factors for both unpolarised and polarised incident neutrons. Two anisotropic versions of the Heisenberg spin chain are considered for such an examination: the spin-1/21/21/2 antiferromagnetic XXZXXZXXZ model and the spin-1/21/21/2 ferromagnetic XYZXYZXYZ model.The XYZXYZXYZ model supports spinon scattering (modelled at finite temperature) and is related to the so-called Villain mode. The introduction of a perturbation in the form of an external transverse magnetic field or Dzyaloshinskii-Moriya interaction (DMI) leads to the emergence of incommensurability in the system; such a result is a signature of fractional excitations. The presence of these interactions also give rise to a chiral response associated with the spinons in the polarised term of the scattering cross section. The inelastic scattering cross section is computed for both unpolarised and polarised neutrons.In relation to the antiferromagnetic XXZXXZXXZ model, emphasis is on spinon pair creation (modelled at T=0rmKT = 0 {rm K}T=0rmK). Motivated by the presence of a chiral response in the case of the XYZXYZXYZ model mentioned above, a new technique is developed in order to incorporate DMI and the transverse magnetic field so that one can determine if there is a chiral property associated with the two-spinon system. This technique is numerical in nature and is based on Green function methods. Using the results produced by the Green function approach, the inelastic cross section in the presence of an external transverse magnetic field is computed for the first time. The result is compared with experimental neutron scattering data; good agreement is demonstrated between theory and experiments on rmCsCoBr3{rm CsCoBr}_3rmCsCoBr3​.Finally, the Green function approach is generalised to account for the interactions between spin chains in magnetic compounds described by a staggered field. Various dynamic structure factors are computed for this scenario with results compared to experiment; good agreement between the theory and experiments on rmRbCoCl3{rm RbCoCl}_3rmRbCoCl3​ is shown.
Many phenomena in magnetism can be described using classical models, yet magnetism is a quantum mechanical effect. In addition to thermal fluctuations, quantum fluctuations arise due to the quantum uncertainty of the ground state. These fluctuations are enhanced by low dimensionality and low spin. Spin chains show interesting excitations associated with quasiparticles. Model materials for spin chains can be realized in compounds where the interchain interactions are weak enough. This thesis presents neutron scattering studies of two model materials for spin chains with different spin symmetry. The spin2 Heisenberg antiferromagnetic chain CuSO4*5D2O has a main exchange of J ∼ 3 K, which permits to study its excitation spectrum up to temperatures of ten times the exchange. The spin2 Heisenberg magnet has been studied widely both theoretically and experimentally. The excitation spectrum of the spin2 Heisenberg antiferromagnet consists of quasiparticles called spinons, and calculations for it exist for T = 0 and as a function of temperature. A quantitative comparison between experimental data and theoretical models across a range of temperatures is presented. The excitation spectrum of CuSO4*5D2O is excellently described by the excitation spectrum of a spin2 Heisenberg antiferromagnetic chain at finite temperatures. Energy-temperature scaling is observed at temperatures up to 2J . For these temperatures the Luttinger liquid description of the spin2 Heisenberg antiferromagnetic chain is valid. A spinon continuum is confirmed at all measured temperatures. Therefore, even at ten times the main exchange (T ≈ 10 J), CuSO4*5D2O shows the behavior of a quantum magnet, and not of a classical system at infinite temperatures, for which one would expect single spin flips. The Ising chain is one of the most studied models in magnetism, one model compound for it is RbCoCl3. Optical spectroscopy measurements suggest a lower gap than for similar compounds, which makes it better suited for high resolution neutron spectroscopy. Magnetic correlations along the chains arise in RbCoCl3 below 80 K. A gapped continuum is observed, which arises from isolated antiferromagnetic Ising chains. Below the first magnetic ordering temperature TN1 ≈ 28 K bound states are observed, which arise due to correlations which form between the chains. Strong diffuse scattering leads to the conclusion that disorder is still present. At the second magnetic ordering transition, at TN2 ≈ 14 K, the bound states split as the correlations between the chains change. Fits indicate that the correlations change continuously as a function of temperature. Above TN2 the excitation spectrum of RbCoCl3 can be described by a spin1 2 Ising chain with an XY-component which is treated as a perturbation. Below TN2 the main features are reproduced correctly, but deviations from the details indicate that additional terms in the Hamiltonian may be necessary. This thesis was carried out at the Institut Laue-Langevin, the Laboratory for Neutron Scattering and Imaging at the Paul Scherrer Institute and ETH Zurich.
We report inelastic time-of-flight and triple-axis neutron scattering measurements of the excitation spectrum of the coupled antiferromagnetic spin-1 Heisenberg chain system CsNiCl3.{\mathrm{CsNiCl}}_{3}.CsNiCl3​. Measurements over a wide range of wave-vector transfers along the chain confirm that above TNCsNiCl3{T}_{N} {\mathrm{CsNiCl}}_{3}TN​CsNiCl3​ is in a quantum-disordered phase with an energy gap in the excitation spectrum. The spin correlations fall off exponentially with increasing distance with a correlation length $\ensuremath{\xi}=4.0(2)$ sites at T=6.2K.T=6.2\mathrm{K}.T=6.2K. This is shorter than the correlation length for an antiferromagnetic spin-1 Heisenberg chain at this temperature, suggesting that the correlations perpendicular to the chain direction and associated with the interchain coupling lower the single-chain correlation length. A multiparticle continuum is observed in the quantum-disordered phase in the region in reciprocal space where antiferromagnetic fluctuations are strongest, extending in energy up to twice the maximum of the dispersion of the well-defined triplet excitations. We show that the continuum satisfies the Hohenberg-Brinkman sum rule. The dependence of the multiparticle continuum on the chain wave vector resembles that of the two-spinon continuum in antiferromagnetic spin-1/2 Heisenberg chains. This suggests the presence of spin-1/2 degrees of freedom in CsNiCl3{\mathrm{CsNiCl}}_{3}CsNiCl3​ for T< 12K,T<~12 \mathrm{K},T< 12K, possibly caused by multiply frustrated interchain interactions.
Quasi-one-dimensional magnetic materials provide important test beds for rigorous models of interacting many-body systems. Nevertheless, there have been few studies of finite temperature effects on spin correlations in low-spin systems, though these are most likely to exhibit quantum effects. Copper benzoate, Cu(C6D5COO)2⋅3D2O, is a good realization of the S=1/2 Heisenberg antiferromagnetic chain (HAFC). We have performed ac susceptibility and inelastic neutron scattering experiments on this material which establish the Hamiltonian and an excitation spectrum which is consistent with the spinon continuum ansatz of Müller et al. We present inelastic neutron scattering measurements of the temperature evolution of the dynamic spin–spin correlation function Szz(π,ω). Comparison will be made to the classical prediction and to a finite temperature field theory of Schulz as applied to this S=1/2 HAFC.
Inelastic neutron scattering has been used to study the temperature dependence of the magnetic response in the one-dimensional S=1/2 Heisenberg antiferromagnet KCuF3{\mathrm{KCuF}}_{3}KCuF3​. The scattering is consistent with that expected for unbound spinon pair excitations.