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The peculiar field-dependent magnetism of Na0.82CoO2 has been investigatedthrough an analysis of its DC and AC spin susceptibilities. To account for theeasily activated narrow b2g-a1g gap of the crystal field for Co in the cobaltoxide layer, the spin-state transition of Co3+ (3d6) between the low spin (LS)state b2g^2-a1g^0 of S=0 and the intermediate spin (IS) state b2g^1-a1g^1 ofS=1 is thus seen as thermally activated and exhibits a Boltzmann distribution.The IS state of Co3+ within each sqrt(13a) hexagonal superlattice formed by theS=1/2 state of the Co4+ ions appears randomly within each supercell and showssignificant temperature and field dependence. The magnetic field is found toassist in pinning down the thermally activated state of Co3+ and swings theBoltzmann distribution weight toward a higher fraction of the IS state. Thefield dependence of the in-plane magnetic moment from the added number of S=1spins is used to explain the origin of A-type antiferromagnetic (AF) ordering,particularly that the ferromagnetic (FM)-like behavior below TN at low field isactually a ferrimagnetic IS spin ordering of Co3+.

Ferrimagnetic ordering and spin entropy of field-dependent intermediate spins in Na0.82CoO2