http://www.cnr.it/ontology/cnr/individuo/prodotto/ID39309
The relativistic four-component static-exchange approximation for core excitation processes in molecules (Articolo in rivista)
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- Label
- The relativistic four-component static-exchange approximation for core excitation processes in molecules (Articolo in rivista) (literal)
- Anno
- 2006-01-01T00:00:00+01:00 (literal)
- Alternative label
- Http://www.cnr.it/ontology/cnr/pubblicazioni.owl#autori
- Ekstrom U., Norman P., Carravetta V. (literal)
- Pagina inizio
- Http://www.cnr.it/ontology/cnr/pubblicazioni.owl#numeroVolume
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- ISI Web of Science (WOS) (literal)
- Http://www.cnr.it/ontology/cnr/pubblicazioni.owl#affiliazioni
- Department of Physics, Chemistry and Biology,
Linkoeping University, SE-581 83 Linkoeping, Sweden
Istituto per i Processi Chimico-Fisici,
Area della Ricerca del C.N.R., via G. Moruzzi 1,
56124 Pisa, Italy (literal)
- Titolo
- The relativistic four-component static-exchange approximation for core excitation processes in molecules (literal)
- Abstract
- A generalization of the static-exchange approximation for core-electron spectroscopies to the relativistic four-component realm is presented. The initial state is a Kramers restricted Hartree--Fock state and the final state is formed as the configuration interaction single excited state, based on the average-of-configurations for (n-1) electrons in n near-degenerate core-orbitals for the reference ionic state. It is demonstrated that the static-exchange Hamiltonian can be made real by considering a set of time-reversal symmetric electron excitation operators. The static-exchange Hamiltonian is constructed at a cost that parallels a single Fock matrix construction in a quaternion framework that fully exploits time-reversal and spatial symmetries for the D_{2h} point group and subgroups. The $K$- and $L$-edge absorption spectra of H2S are used to illustrate the novelties of the methodology. The calculations adopts the Dirac--Coulomb Hamiltonian, but the theory is open-ended towards improvements in the electron-electron interaction operator. It is demonstrated that relativistic effects are substantial for the $L$-edge spectrum of sulphur, and substantial deviations from the statistical 2:1 spin-orbit splitting of the intensity distribution are found. The average ratio in the mixed region is 1.54 at the present level of theory. (literal)
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