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Ca_3Co_{2-x}Mn_xO_6 (x ~ 0.96) is a multiferroic with spin-chains ofalternating Co(2+) and Mn(4+) ions. The spin state of Co(2+) remainsunresolved, due to a discrepancy between high temperature X-ray absorption(S=3/2) and low temperature neutron (S=1/2) measurements. Using a combinationof magnetic modeling and crystal-field analysis, we show that the existing lowtemperature data cannot be reconciled within a high spin scenario by invokingspin-orbit or Jahn-Teller distortions. To unify the experimental results, wepropose a spin-state crossover with specific experimental predictions.

Analysis of magnetization and a spin state crossover in the multiferroic Ca$_3$Co$_{2-x}$Mn$_x$O$_6$