Abstract
The C 3-symmetric crystal-field potential in the Fe(II)Fe(III) bimetallic oxalates splits the L = 2 Fe(II) multiplet into two doublets and one singlet. In compounds that exhibit magnetic compensation, one of the doublets lies lowest in energy and carries an average orbital angular momentum L z cf that exceeds a threshold value of roughly 0.25. In a range of L z cf , a Jahn–Teller (JT) distortion enhances the splitting of the low-lying doublet and breaks the C 3 symmetry of the bimetallic planes around the ferrimagnetic transition temperature. Due to the competition with the spin-orbit coupling, the JT distortion disappears at low temperatures in compounds that display magnetic compensation. A comparison with recent measurements provides compelling evidence for this inverse, low-temperature JT transition. The size of the JT distortion is estimated using first-principles calculations, which suggest that the long-range ordering of smaller, non- C 3-symmetric organic cations can eliminate magnetic compensation.
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