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FePS3 is a layered antiferromagnet (T N=123 K) with a marked Ising anisotropy in magnetic properties. The anisotropy arises from the combined effect of the trigonal distortion from octahedral symmetry and spin-orbit coupling on the orbitally degenerate5 T 2g  ground state of the Fe2+ ion. The anisotropic paramagnetic susceptibilities are interpreted in terms of the zero field Hamiltonian, ℋ=Σi [δ(L  iz 2 −2)+|λ|L i .S i ]−Σ ij J ij S i .S j . The crystal field trigonal distortion parameter Δ, the spin-orbit coupling λ and the isotropic Heisenberg exchange,J ij, were evaluated from an analysis of the high temperature paramagnetic susceptibility data using the Correlated Effective Field (CEF) theory for many-body magnetism developed by Lines. Good agreement with experiment were obtained for Δ/k=215.5 K; λ/k=166.5 K;J nn k=27.7 K; andJ nnn k=−2.3 K. Using these values of the crystal field and exchange parameters the CEF predicts aT N=122 K for FePS3, which is remarkably close to the observed value of theT N. The accuracy of the CEF approximation was also ascertained by comparing the calculated susceptibilities in the CEF with the experimental susceptibility for the isotropic Heisenberg layered antiferromagnet MnPS3, for which the high temperature series expansion susceptibility is available.

Magnetism, exchange and crystal field parameters in the orbitally unquenched Ising antiferromagnet FePS3