title: Open-ended recursive calculation of single residues of response functions for perturbation-dependent basis sets.
abstract: We present theory, implementation, and applications of a recursive scheme for the calculation of single residues of response functions that can treat perturbations that affect the basis set. This scheme enables the calculation of nonlinear light absorption properties to arbitrary order for other perturbations than an electric field. We apply this scheme for the first treatment of two-photon circular dichroism (TPCD) using London orbitals at the Hartree-Fock level of theory. In general, TPCD calculations suffer from the problem of origin dependence, which has so far been solved by using the velocity gauge for the electric dipole operator. This work now enables comparison of results from London orbital and velocity gauge based TPCD calculations. We find that the results from the two approaches both exhibit strong basis set dependence but that they are very similar with respect to their basis set convergence.
authors.affiliation: Centre for Theoretical and Computational Chemisty (CTCC), Department of Chemistry, University of Tromsø , N-9037 Tromsø, Norway.
authors.forename: Daniel H
authors.initials: DH
authors.lastname: Friese
authors.affiliation: Centre for Theoretical and Computational Chemisty (CTCC), Department of Chemistry, University of Tromsø , N-9037 Tromsø, Norway.
authors.forename: Magnus
authors.initials: M
authors.lastname: Ringholm
authors.affiliation: Centre for Theoretical and Computational Chemisty (CTCC), Department of Chemistry, University of Tromsø , N-9037 Tromsø, Norway.
authors.forename: Bin
authors.initials: B
authors.lastname: Gao
authors.affiliation: Centre for Theoretical and Computational Chemisty (CTCC), Department of Chemistry, University of Tromsø , N-9037 Tromsø, Norway.
authors.forename: Kenneth
authors.initials: K
authors.lastname: Ruud