Charge Disproportionation and Spin Ordering Tendencies in Na(x)CoO2
Abstract
The strength and effect of Coulomb correlations in the (superconducting when hydrated) x~1/3 and ``enhanced'' x~2/3 regimes of Na(x)CoO2 are evaluated using the correlated band theory LDA+U method. Our results, neglecting quantum fluctuations, are: (1) allowing only ferromagnetic order, there is a critical U_c = 3 eV, above which charge disproportionation occurs for both x=1/3 and x=2/3, (2) allowing antiferromagnetic order at x=1/3, U_c drops to 1 eV for disproportionation, (3) disproportionation and gap opening occur simultaneously, (4) in a Co(3+)-Co(4+) ordered state, antiferromagnetic coupling is favored over ferromagnetic, while below U_c ferromagnetism is favored. Comparison of the calculated Fermi level density of states compared to reported linear specific heat coefficients indicates enhancement of the order of five for x~0.7, but negligible enhancement for x~0.3. This trend is consistent with strong magnetic behavior and local moments (Curie-Weiss susceptibility) for x>0.5 while there no magnetic behavior or local moments reported for x<0.5. We suggest that the phase diagram is characterized by a crossover from effective single-band character with U >> W for x>0.5 into a three-band regime for x<0.5, where U --> U_eff <= U/\sqrt(3) ~ W and correlation effects are substantially reduced.
Cite
@article{arxiv.cond-mat/0403018,
title = {Charge Disproportionation and Spin Ordering Tendencies in Na(x)CoO2},
author = {K. -W. Lee and J. Kunes and W. E. Pickett},
journal= {arXiv preprint arXiv:cond-mat/0403018},
year = {2009}
}
Comments
10 pages, 8 figures, corrected a few typos and changed references