Electron correlation dynamics in atoms and molecules
- In this paper, we present quantum dynamical calculations on electron correlation dynamics in atoms and molecules using explicitly time-dependent ab initio configuration interaction theory. The goals are (i) to show that in which cases it is possible to switch off the electronic correlation by ultrashort laser pulses, and (ii) to understand the temporal evolution and the time scale on which it reappears. We characterize the appearance of correlation through electron-electron scattering when starting from an uncorrelated state, and we identify pathways for the preparation of a Hartree-Fock state from the correlated, true ground state. Exemplary results for noble gases, alkaline earth elements, and selected molecules are provided. For Mg we show that the uncorrelated state can be prepared using a shaped ultrashort laser pulse.
Author details: | Mathias NestGND, M. Ludwig, I. Ulusoy, Tillmann KlamrothORCiDGND, Peter SaalfrankORCiDGND |
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DOI: | https://doi.org/10.1063/1.4801867 |
ISSN: | 0021-9606 |
ISSN: | 1089-7690 |
Title of parent work (English): | The journal of chemical physics : bridges a gap between journals of physics and journals of chemistr |
Publisher: | American Institute of Physics |
Place of publishing: | Melville |
Publication type: | Article |
Language: | English |
Year of first publication: | 2013 |
Publication year: | 2013 |
Release date: | 2017/03/26 |
Volume: | 138 |
Issue: | 16 |
Number of pages: | 6 |
Funding institution: | Munich Centre for Advanced Photonics |
Organizational units: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie |
Peer review: | Referiert |