1996/08/08 by Stefan Goedecker, S. Goedecker, C. J. Umrigar · 6 citations
Engineering · Materials Science · Physics and Astronomy · #Advanced Chemical Physics Studies #Machine Learning in Materials Science #Molecular Junctions and Nanostructures #cond-mat
paper · pdf · doi:10.1103/physreva.55.1765
14 pages, 5 figures
arxiv created 1996/08/08 · openalex publication_date 1997/03/01 · arxiv updated 2009/11/30 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28
We calculate the electronic structure of several atoms and small molecules by direct minimization of the self-interaction-corrected--local-density-approximation (SIC-LDA) functional. To do this, we first derive an expression for the gradient of this functional under the constraint that the orbitals be orthogonal and then show that previously given expressions do not correctly incorporate this constraint. In our atomic calculations, the SIC-LDA yields total energies, ionization energies, and charge densities that are superior to results obtained with the local density approximation (LDA). However, for molecules, SIC-LDA gives bond lengths and reaction energies that are inferior to those obtained from LDA. The nonlocal Beck-Lee-Yang-Parr functional, which we include as a representative generalized gradient approximation functional, outperforms both LDA and SIC-LDA for all ground-state properties we considered.