Photoinduced excitation and relaxation of organic molecules (C2H4 and CH2NH+2) are investigated by means of nonadiabatic quantum molecular dynamics with hopping (NA-QMD-H), developed recently [Fischer, Handt, and Schmidt, paper I of this series, Phys. Rev. A 90, 012525 (2014)]. This method is first applied to molecules assumed to be initially ad hoc excited to an electronic surface. Special attention is drawn to elaborate the role of electron-nuclear correlations, i.e., of quantum effects in the nuclear dynamics. It is found that they are essential for a realistic description of the long-time behavior of the electronic relaxation process, but only of minor importance to portray the short-time scenario of the nuclear dynamics. Migration of a hydrogen atom, however, is identified as a quantum effect in the nuclear motion. Results obtained with explicit inclusion of an fs-laser field are presented as well. It is shown that the laser-induced excitation process generally leads to qualitatively different gross features of the relaxation dynamics, as compared to the field-free case. Nevertheless, the nuclear wave packet contains all subtleties of the cis-trans isomerization mechanism as observed without a laser field.
| Identifer | oai:union.ndltd.org:DRESDEN/oai:qucosa:de:qucosa:28261 |
| Date | January 2014 |
| Creators | Fischer, Michael, Handt, Jan, Schmidt, Rüdiger |
| Contributors | Technische Universität Dresden |
| Publisher | The American Physical Society |
| Source Sets | Hochschulschriftenserver (HSSS) der SLUB Dresden |
| Language | English |
| Detected Language | English |
| Type | doc-type:article, info:eu-repo/semantics/article, doc-type:Text |
| Source | PHYSICAL REVIEW A, Bd. 90 (2014), Nr. 1, S. 012527, ISSN: 1094-1622 |
| Rights | info:eu-repo/semantics/openAccess |
| Relation | 10.1103/PhysRevA.90.012527 |
Page generated in 0.0019 seconds