https://doi.org/10.1140/epjd/e2012-30056-x
Regular Article
Multiscale modeling of vibrational predissociation spectra under a chirped laser pulse
1
LASIM, CNRS and Université Claude Bernard Lyon 1,
Bât. A. Kastler, 43 bd du 11 novembre
1918, 69622
Villeurbanne,
France
2
ISMO, CNRS and Université Paris-Sud 11,
Bât. 210, 91405
Orsay Cedex,
France
a e-mail: fcalvo@lasim.univ-lyon1.fr
Received:
23
January
2012
Received in final form:
5
April
2012
Published online:
29
June
2012
The vibrational predissociation spectrum of the argon-tagged ionic cluster (NaCl)32 due to exposure to a chirped infrared laser was theoretically calculated in a time multiscale framework. The response to the laser field is modeled explicitly by molecular dynamics simulations, and statistical rate theories are used to evaluate the long-time dissociation probability. Due to anharmonicities and multiphoton processes, the predissociation spectrum shows some small but systematic red shift in the main absorption line. Negative chirping toward lower frequencies further enhances this effect, and also alters the band intensity and the band width. Positive chirping attenuates the dissociation efficiency.
Key words: Topical issue: Atomic Cluster Collisions. Guest editors: Andrey V. Solov’yov and Andrey V. Korol
© EDP Sciences, Società Italiana di Fisica and Springer-Verlag 2012