Density-functional calculations of α, β, γ, δ, δ′, and ε plutonium -: art. no. 185702

Total energies for the six known polymorphs of plutonium metal have been calculated within spin and orbital polarized density-functional theory as a function of lattice constant. Theoretical equilibrium volumes and bulk moduli correspond well with experimental data and the calculated total energies are consistent with the known phase diagram of Pu. It is shown that a preference for the formation of magnetic moments, increasing through the alpha-->beta-->gamma phases, explains their position in the ambient pressure phase diagram and their anomalous variation of atomic density. A simple model is presented that establishes a relationship between atomic density, crystal symmetry, and magnetic moments which is universally valid for all Pu phases.