Isostructural bridging diferrous chalcogenide cores [Fe^II(μ-E)Fe^II] (E = O, S, Se, Te) with decreasing antiferromagnetic coupling down the chalcogenide series.

A clear trend of decreasing magnetic moment with lighter chalcogenides is observed and is attributed to increased antiferromagnetic coupling caused by the linearity of the ∠Fe–E–Fe angle and greater Fe–E orbital overlap.

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With the aid of solid-state SQUID magnetometry, we observed a marked trend of lesser antiferromagnetic coupling when expanding substitution to the heavier chalcogenide congeners which we attribute to the ∠Fe–E–Fe angle becoming more acute due to decreased hybridization in the heavier chalcogenides and poorer orbital overlap with Fe II d-orbitals.

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