Abstract
The ternary iron sulfides, monoclinic TlFeS 2 (linear tetrahedral chains) and orthorhombic Tl 3Fe 2S 4 (folded tetrahedral chains), have been investigated by means of magnetic susceptibility measurements, powder neutron diffraction, and Mössbauer spectroscopy. Both compounds exhibit three-dimensional antiferromagnetic order with Néel temperatures of 190(10) and 90(5) K, respectively. The low-temperature magnetic structures have been obtained and the moment values are 1.85(6) μ B for TlFeS 2 and 1.5(2) μ B for Tl 3Fe 2S 4. The magnitude and the coupling of moments in the Fe-S tetrahedral frameworks are seen to be strongly influenced by direct Fe-Fe interactions for edge-sharing tetrahedra, while the Fe-S bond may be described as ionic. The Fe-Fe interaction apparently goes along with a metallic state, permitting an intermediate valence (Fe 2.5+) in the folded chain compound.
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