Fast noniterative orbital localization for large molecules

Forskningsoutput: TidskriftsbidragArtikel i vetenskaplig tidskrift

Abstract

We use Cholesky decomposition of the density matrix in atomic orbital basis to define a new set of occupied molecular orbital coefficients. Analysis of the resulting orbitals ("Cholesky molecular orbitals") demonstrates their localized character inherited from the sparsity of the density matrix. Comparison with the results of traditional iterative localization schemes shows minor differences with respect to a number of suitable measures of locality, particularly the scaling with system size of orbital pair domains used in local correlation methods. The Cholesky procedure for generating orthonormal localized orbitals is noniterative and may be made linear scaling. Although our present implementation scales cubically, the algorithm is significantly faster than any of the conventional localization schemes. In addition, since this approach does not require starting orbitals, it will be useful in local correlation treatments on top of diagonalization-free Hartree-Fock optimization algorithms.

Detaljer

Författare
  • Francesco Aquilante
  • Thomas Pedersen
  • Alfredo Sanchez de Meras
  • Henrik Koch
Enheter & grupper
Forskningsområden

Ämnesklassifikation (UKÄ) – OBLIGATORISK

  • Teoretisk kemi
Originalspråkengelska
TidskriftJournal of Chemical Physics
Volym125
Utgivningsnummer17
StatusPublished - 2006
PublikationskategoriForskning
Peer review utfördJa