Strictly localized basis sets for Uranium and Plutonium

The properties of allotropes and selected compounds of plutonium (Pu) and uranium (U) are evaluated using a first-principles approach with strictly localized basis sets as implemented in the density functional theory code SIESTA. The lattice parameters, first-order elastic properties, and phonon density of states of the allotropes and compounds are in good agreement with available experimental data and prior calculations based on plane-wave methodologies. The advantage of the localized basis set approach is a good balance between speed and accuracy, which is demonstrated by modeling, for the first time, the properties of large systems of U using parameter-free ab initio molecular dynamics.