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Self-interaction-corrected time-dependent density functional theory calculations of x-ray absorption spectra
Laboratory of Theoretical Chemistry, Royal Institute of Technology, Stockholm, Sweden.
Laboratory of Theoretical Chemistry, Royal Institute of Technology, Stockholm, Sweden.
Laboratory of Theoretical Chemistry, Royal Institute of Technology, Stockholm, Sweden.
Laboratory of Theoretical Chemistry, Royal Institute of Technology, Stockholm, Sweden.
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2007 (English)In: Physical Review A, ISSN 1050-2947, Vol. 76, no 2, 022506- p.Article in journal (Refereed) Published
Abstract [en]

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 et al., 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.
National Category
Natural Sciences
Identifiers
URN: urn:nbn:se:liu:diva-12693DOI: 10.1103/PhysRevA.76.022506OAI: oai:DiVA.org:liu-12693DiVA: diva2:16867
Available from: 2007-10-30 Created: 2007-10-30 Last updated: 2009-05-15
In thesis
1. Time-dependent molecular properties in the optical and x-ray regions
Open this publication in new window or tab >>Time-dependent molecular properties in the optical and x-ray regions
2007 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Time-dependent molecular properties are important for the experimental characterization of molecular materials. We show how these properties can be calculated, for optical and x-ray frequencies, using novel quantum chemical methods. For xray absorption there are important relativistic effects appearing, due to the high velocity electrons near the atomic nuclei. These effects are treated rigorously within the four-component static exchange approximation. We also show how electron correlation can be taken into account in the calculation of x-ray absorption spectra, in time-dependent density functional theory based on the complex polarization propagator approach. The methods developed have been applied to systems of experimental interest|molecules in the gas phase and adsorbed on metal surfaces. The effects of molecular vibrations have been take into account both within and beyond the harmonic approximation.

Place, publisher, year, edition, pages
Institutionen för fysik, kemi och biologi, 2007
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1131
Keyword
Quantum chemistry, molecular physics, x-ray spectroscopy, relativity
National Category
Other Physics Topics
Identifiers
urn:nbn:se:liu:diva-10125 (URN)978-91-85895-88-5 (ISBN)
Public defence
2007-10-23, Planck, Fysikhuset, Campus Valla, Linköpings universitet, Linköping, 10:15 (English)
Opponent
Supervisors
Available from: 2007-10-30 Created: 2007-10-30 Last updated: 2009-04-26

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Ekström, UlfNorman, Patrick

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