Molecular electronic structure problem solved by numerical one‐electron Green's functions

Abstract

AbstractA method for the calculation of the electronic structure of molecules is presented that is based on the Kohn–Sham formulation of density functional theory. The method avoids calculating global molecular orbitals; therefore, the electron density is defined by means of numerically calculated one‐electron Green's functions. The method adopts a strategy of dividing a molecule into atomic subsystems whereby the favorable linear scaling of computational costs is obtained. Formulating the electronic structure problem by means of Green's functions allows the introduction of an additional coupling between subsystems that is not present in familiar methods. Although the method is general and can be applied to molecules with an arbitrary structure, it is at present tested only on some linear molecules. © 2003 Wiley Periodicals, Inc. Int J Quantum Chem, 2004