Phase diagram of NaxCoO2 studied by gutzwiller density-functional theory

The ground state of NaxCoO2 (0.0<x<1.0) is studied by the local density approximation plus the Gutzwiller approach, where charge transfer and orbital fluctuations are all self-consistently treated ab initio. In contrast to previous studies, which are parameter-dependent, we characterized the phase diagram as (1) Stoner magnetic metal for x>0.6 due to a1g van Hove singularity near the band top, (2) correlated nonmagnetic metal without eg′ pockets for 0.3<x<0.6, and (3) eg′ pockets appear for x<0.3, and additional magnetic instability is revealed. Experimental quasiparticle properties are well explained, and the a1g-eg′ anticrossing is attributed to spin-orbital coupling.