Abstract
We explore the ultrafast spin-flip dynamics in a diatomic molecule imbedded in a rare gas matrix using the combination of a quantum mechanical and a semiclassical surface hopping method. Specifically, we investigate (1) the extent to which the phenomenon of electronically-localized eigenstates in strongly-coupled manifolds survives in the presence of rapid decay and a multitude of electronically coupled states; (2) the ability of the surface hopping method to predict the short time dynamics; and (3) the time range over which frozen lattice models are valid. Our results point to the active role played by a large number of coupled electronic states in the F2/Ar dynamics while substantiating our confidence in the validity of the popular surface hopping approach for the system considered.
| Original language | English (US) |
|---|---|
| Pages (from-to) | 1651-1659 |
| Number of pages | 9 |
| Journal | Laser Physics |
| Volume | 19 |
| Issue number | 8 |
| DOIs | |
| State | Published - Aug 2009 |
Funding
ACKNOWLEDGMENTS We thank Professor J. Manz for helpful discussions. T.S. is grateful to the National Science Foundation (grant number CHE 0616927) for support and to the Weston Foundation for a Visiting Professor Award under the auspices of which this research was carried out. R.B.G. thanks the Deutsche Forschungsgemein schaft in the framework of the SFB 450 project, “Anal ysis and control of ultrafast photoinduced reactions.” Our numerical work used in part the resources of the Argonne Leadership Computing Facility at Argonne National Laboratory, which is supported by the Office of Science of the U.S. Department of Energy under Contract no. DE AC02 06CH11357.
ASJC Scopus subject areas
- Atomic and Molecular Physics, and Optics
- Instrumentation
- Condensed Matter Physics
- Industrial and Manufacturing Engineering