@article{KlamrothNest2009, author = {Klamroth, Tillmann and Nest, Mathias}, title = {Ultrafast electronic excitations of small sodium clusters and the onset of electron thermalization}, issn = {1463-9076}, doi = {10.1039/B813619j}, year = {2009}, abstract = {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.}, language = {en} }