DOI: 10.1063/1.465990 ISSN:

Coupled cluster theory for high spin, open shell reference wave functions

Peter J. Knowles, Claudia Hampel, Hans-Joachim Werner
  • Physical and Theoretical Chemistry
  • General Physics and Astronomy

The coupled cluster method restricted to single and double excitations (CCSD) is considered for the case of a spin restricted Hartree–Fock open shell reference determinant. A spin–orbital based formulation, in which the cluster operator spans exactly the minimal first order interacting space, is presented, and computationally optimal working equations are given. In the limit of a large number of closed shell orbitals, the cost is identical to that of an optimum treatment of an equivalent closed shell problem, which is obtained as a special case of the formulation presented. The theory is applied to the calculation of a number of diatomic potential energy functions and compared with spin-unrestricted theory.

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