Self-interaction-corrected time-dependent density-functional-theory calculations of x-ray-absorption spectra
2007 (English)In: Physical Review A. Atomic, Molecular, and Optical Physics, ISSN 1050-2947, E-ISSN 1094-1622, Vol. 76, no 2, 022506- p.Article in journal (Refereed) Published
We outline an approach within time-dependent density functional theory that predicts x-ray spectra on an absolute scale. The approach rests on a recent formulation of the resonant-convergent first-order polarization propagator [P. Norman , J. Chem. Phys. 123, 194103 (2005)] and corrects for the self-interaction energy of the core orbital. This polarization propagator approach makes it possible to directly calculate the x-ray absorption cross section at a particular frequency without explicitly addressing the excited-state spectrum. The self-interaction correction for the employed density functional accounts for an energy shift of the spectrum, and fully correlated absolute-scale x-ray spectra are thereby obtained based solely on optimization of the electronic ground state. The procedure is benchmarked against experimental spectra of a set of small organic molecules at the carbon, nitrogen, and oxygen K edges.
Place, publisher, year, edition, pages
2007. Vol. 76, no 2, 022506- p.
Benchmarking, Carbon, Density functional theory, Excited states, Ground state, Nitrogen, Optimization, Oxygen, Polarization, Energy shift, Organic molecules, Polarization propagator, Self-interaction energy
IdentifiersURN: urn:nbn:se:kth:diva-8410DOI: 10.1103/PhysRevA.76.022506ISI: 000249154900062ScopusID: 2-s2.0-34548203136OAI: oai:DiVA.org:kth-8410DiVA: diva2:13722
QC 201009142008-05-092008-05-092011-09-02Bibliographically approved