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arXiv:cond-mat/0109065 · Journal of Applied Physics

Continuum spin excitations in S=1 one-dimensional antiferromagnet

Igor A. Zaliznyak

Published May 15, 2002• 6 citations
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Abstract

We present detailed measurement of the nonhydrodynamic part of the spin excitation spectrum in the model quasi-one-dimensional S=1 antiferromagnet CsNiCl3 by inelastic magnetic neutron scattering. In the better part of the Brillouin zone the effect of interchain coupling is negligible, and the spin dynamics reflects that of a single Haldane chain. We find that at q≲0.6π this quantum spin system ceases to support coherent propagating excitation, which gradually turns into a continuum band of states, whose width grows with decreasing q. This finding is consistently verified under different resolution conditions, obtained with two different high-luminosity experimental setups.

DOI
10.1063/1.1456440

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We present detailed measurement of the nonhydrodynamic part of the spin excitation spectrum in the model quasi-one-dimensional S=1 antiferromagnet CsNiCl3 by inelastic magnetic neutron scattering. In the better part of the Brillouin zone the effect of interchain coupling is negligible, and the spin dynamics reflects that of a single Haldane chain. We find that at q≲0.6π this quantum spin system ceases to support coherent propagating excitation, which gradually turns into a continuum band of states, whose width grows with decreasing q. This finding is consistently verified under different resolution conditions, obtained with two different high-luminosity experimental setups.
The spin-excitation continuum, expected to dominate the low-energy fluctuation spectrum in the Haldane spin chain around the Brillouin zone center, q=0q\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}0q=0, is directly observed by inelastic magnetic neutron scattering in the S=1S\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}1S=1 quasi-1D antiferromagnet CsNiCl3{\mathrm{CsNiCl}}_{3}CsNiCl3​. We find that the single mode approximation fails, and that a finite energy width appears in the dynamic correlation function $S(q,\ensuremath{\omega})$ for $q\ensuremath{\lesssim}0.5\ensuremath{\pi}$. The width increases with decreasing qqq, while $S(q,\ensuremath{\omega})$ acquires an asymmetric shape qualitatively similar to that predicted for the two-magnon continuum in the nonlinear $\ensuremath{\sigma}$-model.
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.
A continuum of magnetic states has been observed by neutron scattering from the spin-1 chain compound CsNiCl3 in its disordered gapped one-dimensional phase. Results using both triple-axis and time-of-flight spectrometers show that around the antiferromagnetic point Qc = pi, the continuum lies higher in energy than the Haldane gapped excitations. At 6 K the integrated intensity of the continuum is about 12(2)% of the total spectral weight. This result is considerably larger than the 1%-3% weight predicted by the nonlinear sigma model for the three-particle continuum.
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.
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.
Inelastic neutron scattering is used to study transverse-polarized magnetic excitations in the quasi-one-dimensional S=1/2S\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}1/2S=1/2 antiferromagnet BaCu2Si2O7{\mathrm{BaCu}}_{2}{\mathrm{Si}}_{2}{\mathrm{O}}_{7}BaCu2​Si2​O7​, where the saturation value for the N\'eel order parameter is ${m}_{0}\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}0.12{\ensuremath{\mu}}_{\mathrm{B}}$ per spin. At low energies the spectrum is totally dominated by resolution-limited spin-wave-like excitations. An excitation continuum sets in above a well-defined threshold frequency. Experimental results are discussed in the context of current theories for weakly interacting quantum half-integer-spin chains.