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Using x-ray absorption spectroscopy at the Rh-L_2,3, Co-L_2,3, and Fe-L_2,3edges, we find a valence state of Co^2+/Rh^4+ in Ca3CoRhO6 and of Fe^3+/Rh^3+in Ca3FeRhO6. X-ray magnetic circular dichroism spectroscopy at the Co-L_2,3edge of Ca3CoRhO6 reveals a giant orbital moment of about 1.7mu_B, which can beattributed to the occupation of the minority-spin d_0d_2 orbital state of thehigh-spin Co^2+ (3d^7) ions in trigonal prismatic coordination. This activerole of the spin-orbit coupling explains the strong magnetocrystallineanisotropy and Ising-like magnetism of Ca3CoRhO6.

X-ray absorption and x-ray magnetic dichroism study on Ca3CoRhO6 and Ca3FeRhO6