Density functional theory (DFT) is the foundation of nearly all atomistic modeling done in chemistry and materials science today. Computer calculations based on DFT are remarkably successful in describing the properties of molecules, surfaces, and solids when atoms are near their equilibrium positions.[4] Quantities such as bond lengths, bond angles, and vibrational frequencies computed using modern DFT methods agree closely with experimentally-determined values. And because the calculations use only the positions and identities of the atoms as inputs – and not additional parameters that must be tuned in order to achieve accurate results – they have predictive power. Many materials properties can be reliably predicted before they are measured – or even before a new material has been synthesized.

Despite this success, self-interaction error (SIE) remains a flaw in DFT, its effects surfacing most dramatically when electrons are shared over stretched bonds, as in the transition states of chemical reactions, and in many transition metal complexes even near equilibrium geometries. The Fermi-Löwdin orbital self-interaction correction (FLO-SIC) method is a promising new approach for removing SIE from DFT calculations. Work in this Center involves further development and implementation of FLO-SIC. The research spans a wide range, from basic theory questions related to how best to marry FLO-SIC to the most sophisticated DFTs, to applied efforts to create improved materials for energy applications.

The vision of our Center is to create a powerful and efficient FLO-SIC software package that will enable efficient and predictive descriptions of materials and chemical systems without the unphysical effects of electron self-interaction.