Correlated ab initio electronic structure calculations for large molecules

Density functional theory (DFT) and localized orbital methods for performing correlated ab initio electronic structure calculations for large molecules are analyzed. It is shown that DFT methods are the most accurate and easy to use for a variety of applications. However, localized orbital methods are the most practical alternatives in cases where DFT methods are unapplicable. Comparisons between DFT and localized orbital methods are discussed.