Abstract
Ca3Co2-xMnxO6 (x similar to 0.96) is a multiferroic with spin-chains of alternating Co2+ and Mn4+ ions. The spin state of Co2+ remains unresolved due to a discrepancy between high-temperature x-ray absorption (S=3/2) and low-temperature neutron (S=1/2) measurements. Using a combination of magnetic modeling and crystal-field analysis, we show that the existing low temperature data cannot be reconciled within a high spin scenario by invoking spin-orbit or Jahn-Teller distortions. To unify the experimental results, we propose a spin-state crossover with specific experimental predictions.