Optimizing the Full Potential Linear Muffin Tin Orbital Basis Set

Density functional theory (DFT) calculations for 5f and 5d block materials and materials in high compression require the use of all-electron methods that explicitly treat core electrons. The full potential linear muffin-tin orbital (FP-LMTO) method is one of the most efficient all-electron approaches. However, the accuracy of this method relies on a judicious choice of so-called “tail energies” in constructing the basis for FP-LMTO calculations. Since the tail energies satisfy a variational principle, they can, in principle, be chosen to optimize the accuracy of calculations. We investigate ways to choose tail energies, including through the use of physics-informed choices.