Can we outperform the DIIS approach for electronic structure calculations?

This article regroups various results on self-consistent field algorithms f or computing electronic structures of molecular systems. The first part dea ls with the convergence properties of the "conventional" Roothaan algorithm and of the level-shifting algorithm. In the second part, a new class of al gorithms is introduced, for which convergence is guaranteed by mathematical arguments. Computational performance on various test problems is reported; advantages of this new approach are demonstrated. (C) 2000 John Wiley & So ns, Inc.