An efficient orbital transformation method for electronic structure calculations

An efficient method for optimizing single-determinant wave functions of medium and large systems is presented. It is based on a minimization of the energy functional using a new set of variables to perform orbital transformations. With this method convergence of the wave function is guaranteed. Preconditioners with different computational cost and efficiency have been constructed. Depending on the preconditioner, the method needs a number of iterations that is very similar to the established diagonalization–DIIS approach, in cases where the latter converges well. Diagonalization of the Kohn–Sham matrix can be avoided and the sparsity of the overlap and Kohn–Sham matrix can be exploited. If sparsity is taken…

• NS
  National Science Foundation
• SN
  Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung

  Award: 63305