EPR powder measurements above 77 K on two forms each of Li3MnO4 and Li2MnO3 are reported. Here the systems Mn5+/Td and Mn4+/Oh are presented. The new spin‐resonance data are compared with those of analogous systems, the g‐shift is discussed. The analysis of lineshapes indicates that exchange effects for Li3MnO4 as well as for Li2MnO3 must be taken into account. Magnetic susceptibility measurements down to 4 K show antiferromagnetism for the hexagonal β‐Li2MnO3 below 50 K. Examining the temperature dependence of intensity and linewidth of the EPR signal one can identify this magnetic behaviour already above TN. The antiferromagnetic coupling between the Mn4+‐ions (3d3) is realized by superexchange through O2‐‐ligand orbitals.
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Scharmann et al. (1975) studied this question.
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