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Averaged Atomic Natural Pseudo-Orbital (ANPO) Basis Sets

A.Zaitsevskii

ANPO are the counterparts of well-known Averaged Atomic Natural Orbitals (ANO) for core pseudopotential calculations. Its use appears to be recommendable for high-level correlation and  possibly spin-orbit treatment  when the computational cost of integral evaluation stage is negligible while the reduction of basis set size is of crucial importance for other stages. The employed procedure of ANPO basis construction is essentially that used to produce  density-averaged ANO in [K.Pierloot, B.Dumez, P.-O.Wildmark, B.O.Roos, Theor.Chim.Acta 90,  87 (1995)]:
  • Normally I started with an even-tempered primitive Gaussian manifold crudely optimized at SCF (for low momentum values) or AQCC (higher angular momentum values) levels and extended by one diffuse function per angular momentum. Innermost d exponents (for atoms with d shell treated explicitely) were optimized separately . For second row atoms I took f exponents from [P.-O.Wildmark, B.J.Persson,  B.O.Roos,  Theor.Chim.Acta 79, 419 (1991)]
  • (MC)SCF procedure with averaging over the neutral atom (A), negative ion (A-) and positive ion (A+) ground states weighted as 2:1:1 (1:0:1 for rare gas atoms having no negative ions) is employed to generate initial common orthogonal orbital basis, 
  • using this common basis, AQCC calculations  for A, A- and A+ ground states are performed. The resulting densities are averaged with the same weights 2(A) :  1(A-) : 1(A+) (or 1(A) : 1(A+)  for rare-gas atoms) and  then diagonalized to yield the ANPO. 
  • the procedure applied to transition elements was somewhat more complicated, involving electronic states with different d-shell occupancies in the averaging procedure.
  • The present calculations were performed by means of (slightly modified) routines from the Columbus  program suite. The ANPO are adapted to the use of shape-consistent core pseudopotentials of Christiansen et al. (see e.g. [L.A.LaJohn et al., J.Chem.Phys. 87, 2812 (1987)]).  For heavier elements,  small-core (spd-valence) pseudopotentials were chosen; to obtain ANPO well suited for sp-only correlation calculations, the d shell was frozen at AQCC step. Au basis for use with energy-adjusted small-core pseudopotential [Andrae et al., Theor.Chim.Acta 77, 123 (1990)] is given.

    Available Basis Sets

     Cl  Ar
     Br
     Te  I  Xe
     Au
     At
    The basis sets are given in the Columbus  format:

    line: [comment line]
    line: [number_of_contractions]
    do i = 1 , [number_of_contractions]
      line: [number_of_primitives] [angular_momentum+1] [max_number_of_ANPO]
      do j = 1, [number_of_primitives]
        line: [exp_of_primitive] ([coef_of_primitive_in_kth_ANPO], k=1,max_number_of_ANPO])
      end do
    end do

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