Cobalt spin states and hyperfine interactions in LaCoO3 investigated by LDA+U calculations

With a series of local-density approximation plus Hubbard U calculations, we have demonstrated that for lanthanum cobaltite (LaCoO3), the electric field gradient at the cobalt nucleus can be used as a fingerprint to identify the spin state of the cobalt ion. Therefore, in principle, the spin state of the cobalt ion can be unambiguously determined from nuclear magnetic resonance spectra. Our calculations also suggest that a crossover from the low-spin to intermediate-spin state in the temperature range of 0-90 K is unlikely, based on the half-metallic band structure associated with isolated IS Co ions, which is incompatible with the measured conductivity.