Accelerating self-consistent field convergence with the augmented Roothaan-Hall energy function.
Based on Pulay's direct inversion iterative subspace (DIIS) approach, we present a method to accelerate self-consistent field (SCF) convergence. In this method, the quadratic augmented Roothaan-Hall (ARH) energy function, proposed recently by Høst and co-workers [J. Chem. Phys. 129, 124106 (2008)], is used as the object of minimization for obtaining the linear coefficients of Fock matrices within DIIS. This differs from the traditional DIIS of Pulay, which uses an object function derived from the commutator of the density and Fock matrices. Our results show that the present algorithm, abbreviated ADIIS, is more robust and efficient than the energy-DIIS (EDIIS) approach. In particular, several examples demonstrate that the combination of ADIIS and DIIS ("ADIIS+DIIS") is highly reliable and efficient in accelerating SCF convergence.
Department of Chemistry, Duke University, Durham, North Carolina 27708-0354, USA. xqhu@duke.edu
Xiangqian
X
Hu
Weitao
W
Yang
D000054:Acceleration; D001703:Biophysics / Q000379:methods*; D003198:Computer Simulation; D004867:Equipment Design; D007090:Image Interpretation, Computer-Assisted; D011487:Protein Conformation; D011789:Quantum Theory