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Physical review. B, Condensed matter

Finite-chain approach to the study of CsNiCl3

L. S. Campana, Alvaro Caramico D’Auria, Francesco Esposito, Ugo Esposito, G. Kamieniarz

Published Mar 1, 1992• 8 citations
Publisher

Abstract

The specific heat and magnetic susceptibility of the antiferromagnetic Heisenberg chain have been calculated using a numerical finite-size technique. An agreement with experiment for the quasi-one-dimensional compound ${\mathrm{CsNiCl}}_{3}$, which displays a Haldane gap, is revealed.

DOI
10.1103/physrevb.45.5035

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The specific heat and magnetic susceptibility of the antiferromagnetic Heisenberg chain have been calculated using a numerical finite-size technique. An agreement with experiment for the quasi-one-dimensional compound CsNiCl3{\mathrm{CsNiCl}}_{3}CsNiCl3​, which displays a Haldane gap, is revealed.
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 phenomenological expression $\ensuremath{\chi}T∕(N{g}^{2}{\ensuremath{\mu}}_{B}^{2}∕k)={C}_{1n}\phantom{\rule{0.2em}{0ex}}\mathrm{exp}(\ensuremath{-}{W}_{1n}∕T)+{C}_{2n}\phantom{\rule{0.2em}{0ex}}\mathrm{exp}(\ensuremath{-}{W}_{2n}∕T)$ describes very accurately the temperature dependence of the magnetic susceptibility computed for antiferromagnetic rings of Heisenberg spins S=1S=1S=1, whose size nnn is even and ranges from 6 to 20. This expression has been obtained through a strategy justified by scaling considerations together with finite size numerical calculations. For nnn large, the coefficients of the expression converge towards C1=0.125{C}_{1}=0.125C1​=0.125, W1=0.451J{W}_{1}=0.451JW1​=0.451J, C2=0.564{C}_{2}=0.564C2​=0.564, W2=1.793J{W}_{2}=1.793JW2​=1.793J (JJJ is the exchange constant), which are appropriate for describing the susceptibility of the spin-1 Haldane chain. The Curie constant, the paramagnetic Curie--Weiss temperature, the correlation length at T=0T=0T=0 and the Haldane gap are found to be closely related to these coefficients. With this expression, a very good description of the magnetic behavior of Y2BaNiO5{\mathrm{Y}}_{2}\mathrm{Ba}\mathrm{Ni}{\mathrm{O}}_{5}Y2​BaNiO5​ and of Ni(C2H8N2)2NO2ClO4\mathrm{Ni}{({\mathrm{C}}_{2}{\mathrm{H}}_{8}{\mathrm{N}}_{2})}_{2}\mathrm{N}{\mathrm{O}}_{2}\mathrm{Cl}{\mathrm{O}}_{4}Ni(C2​H8​N2​)2​NO2​ClO4​ (NENP), the archetype of the Haldane gap systems, is achieved over the whole temperature range.
Since Haldane conjectured that ground state of one-dimensional Heisenberg antiferromagnet has a finite spin gap for integer spins, while gapless excitations for half-odd integer spins, it has inspired lots of theoretical and experimental studies on low-dimensional quantum magnets. Several one-dimensional chain systems of integer spins, so called Haldane chain, have been discovered and studied, such as CsNiCl3, Y2BaNiO5, PbNi2V2O8, SrNi2V2O8, AgVP2S6. It has been known that most of the Haldane chain has antiferromagnetic coupling for the intrachain exchange interaction. Recently, we have found a Haldane chain compound in which antiferromagnetic order is accompanied by antiferromagnetic interchain coupling between one-dimensional ferromagnetic chains below 30.5 Kelvin. In this presentation, we present comprehensive study of its magnetic and thermal properties.
Finite-size effects in a spin-1/21/21/2 one-dimensional (1D) Heisenberg antiferromagnet (HAF) are studied experimentally and theoretically. The calculated susceptibility is compared with that observed in the quasi-1D HAF ${\mathrm{SrCu}}_{1\ensuremath{-}x}{\mathrm{Mg}}_{x}{\mathrm{O}}_{2}$. Excellent agreement between theory and experiment is obtained without any adjustable parameters above about 0.02J0.02J0.02J, where JJJ is the dominant exchange interaction constant.