A black-box self-consistent field convergence algorithm:: One step closer

A direct inversion iterative subspace version of the relaxed constrained algorithm is found to be a very powerful convergence acceleration technique for the solution of the self-consistent field equations found in the Hartree-Fock method and Kohn-Sham-based density functional theory (KS-DFT). The present algorithm, abbreviated EDIIS, is benchmarked against the direct inversion iterative subspace method based on the commutator of the density and Fock matrices developed by Pulay (DIIS). Our findings indicate that while EDIIS is able to rapidly bring the density matrix from any initial guess to a solution region, the DIIS method is faster when the density matrix is close to convergence. Consequently, we propose a combination of EDIIS and DIIS methods, which is both very robust and highly efficient. We also show how EDIIS can detect the presence and determine the value of fractional occupations in KS-DFT. (C) 2002 American Institute of Physics.