Ultrafast electronic excitations of small sodium clusters and the onset of electron thermalization
- In this paper we report simulations of the ultrafast laser excitation and relaxation of the correlated valence electrons of a Na-8 cluster. The aim is twofold: first, while the total energy stays constant when the exciting laser pulse is over, we observe that the entropy computed from the reduced one electron density matrix rises on a much longer time scale. We discuss whether this can be understood as the onset of the thermalization of a finite system. Second, we describe this process with eight different methods of wavefunction-based electronic structure theory, which have been adapted for an explicitly time-dependent description. Their respective advantages and limitations for the simulation of the excitation and subsequent relaxation are explained.
| Author details: | Tillmann KlamrothORCiDGND, Mathias NestGND |
|---|---|
| URL: | http://pubs.rsc.org/en/Journals/JournalIssues/CP |
| DOI: | https://doi.org/10.1039/B813619j |
| ISSN: | 1463-9076 |
| Publication type: | Article |
| Language: | English |
| Year of first publication: | 2009 |
| Publication year: | 2009 |
| Release date: | 2017/03/25 |
| Source: | Physical chemistry chemical physics. - ISSN 1463-9076. - 11 (2009), 2, S. 349 - 357 |
| Organizational units: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie |
| Peer review: | Referiert |
