A new all-electron Kohn-Sham method for molecules and clusters is introduced and applied. The local Kohn-Sham exchange potential and the exchange energy are treated exactly. The method yields high quality one-particle spectra. An exchange-correlation charge density which generates the exchange-correlation potential is introduced. It may turn out to be of great interpretative value. Within the new Kohn-Sham method the exchange part of this density is constructed.

• Received 11 June 1999

DOI:https://doi.org/10.1103/PhysRevLett.83.5459