NMR study of magnetic order, metamagnetic transitions, and low-temperature spin freezing in Ca3Co2O6

We report on a (59)Co NMR investigation of the trigonal cobaltate Ca(3)Co(2)O(6) carried out on a single crystal, providing precise determinations of the electric field gradient and chemical shift tensors, and of the internal magnetic fields at the nonmagnetic Co I sites, unavailable from former studies on powders. The magnetic-field-induced ferri-and ferromagnetic phases at intermediate temperature (e.g., 10 K) are identified by distinct internal fields, well accounted for by purely dipolar interactions. The vanishing transferred hyperfine field at the Co I site indicates that the Co(3+) (I) orbitals do not participate in the intrachain superexchange, in disagreement with a previous theore…