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Journal of Physics Condensed Matter

Spin dynamics along the chain direction in an S =3/2, quasi-one-dimensional Heisenberg antiferromagnet CsVCl3

S. Itoh, Kazuhisa Kakurai, M. Arai, Y. Endoh

Published Sep 6, 1993• 8 citations
Publisher

Abstract

Inelastic neutron scattering experiments investigating the spin dynamics along the chain direction of an S = 3 / 2 quasi-one-dimensional Heisenberg antiferromagnet CsVCl 3 were performed up to the zone boundary energy. The authors observed the quantum renormalization in the exchange constant and found that the scattering function cannot be described by either the classical delta -function or the quantum Heisenberg model for S = 1 / 2 . The spin excitations have apparent linewidths and they are compared with the theory of the classical isotropic Heisenberg system at finite temperatures.

DOI
10.1088/0953-8984/5/36/032

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Inelastic neutron scattering experiments investigating the spin dynamics along the chain direction of an S = 3 / 2 quasi-one-dimensional Heisenberg antiferromagnet CsVCl 3 were performed up to the zone boundary energy. The authors observed the quantum renormalization in the exchange constant and found that the scattering function cannot be described by either the classical delta -function or the quantum Heisenberg model for S = 1 / 2 . The spin excitations have apparent linewidths and they are compared with the theory of the classical isotropic Heisenberg system at finite temperatures.
Well-defined spin-wave excitations were observed by using pulsed neutrons from CsVCl3{\mathrm{l}}_{3}l3​, an S=3/2S\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}3/2S=3/2 Heisenberg antiferromagnetic chain. The observed spin-wave dispersion relation shows an enhancement of the excitation energy by a factor of 1.26, which must be compared with the quantum renormalization factor of $\ensuremath{\pi}/2$ for an S=1/2S\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}1/2S=1/2 system. The linewidth of the spectrum at 40 K was broad and independent of qqq. The qqq-independent linewidth is the first experimental observation, which was predicted by rigorous theories for a classical chain at sufficiently low temperature.
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.
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.
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.
A full description of a series of spin-wave measurements in CsNiCl3{\mathrm{CsNiCl}}_{3}CsNiCl3​ in the three-dimensional (3D) and one-dimensional (1D) phases and their analysis to provide the first experimental evidence for the Haldane gap is presented. Neutron scattering experiments were performed on a single crystal of CsNiCl3{\mathrm{CsNiCl}}_{3}CsNiCl3​ with both (h,0,l) and (h,h,l) as the scattering plane. The order parameter in both 3D phases was measured and the spin-wave dispersion determined in the lower phase. The spin-wave spectrum calculated from a dynamic susceptibility method was compared with the experimental response in the lower 3D phase to obtain the following values for the exchange and anisotropy constants: J=0.345\ifmmode\pm\else\textpm\fi{}0.008 THz, J'=0.0060\ifmmode\pm\else\textpm\fi{}0.005 THz, and D=-0.0130\ifmmode\pm\else\textpm\fi{}0.0015 THz. These parameters confirm that CsNiCl3{\mathrm{CsNiCl}}_{3}CsNiCl3​ in its disordered phase is a good approximation to a one-dimensional Heisenberg antiferromagnet. In the 1D phase the gap frequency for an isolated chain of Ni2+{\mathrm{Ni}}^{2+}Ni2+ ions is found to be 0.32 THz close to the gap estimated in finite-chain calculations. The results constitute experimental support for the Haldane conjecture that the excitations of integer-spin chains, unlike half-integer--spin chains, exhibit an apparent anisotropy that arises not from the underlying isotropic Hamiltonian, but from many-body effects.
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.