Abstract
Detailed time-resolved photodissociation and caging dynamics in clusters are studied using I-2(OCS)11 as a model system. We report new observations of product channel-dependent properties of nuclear coherence in the dissociated chromophore, reflecting complex dynamics of the solvent cage. The coherence feature is most pronounced in the caged two-photon channels and its relative amplitude increases with the product size. Shorter delays, on the time scale of coherent I⋯I- motion, favor larger products, allowing for incoherent control of two-photon dissociation pathways by appropriately timing the two laser pulses. As an example of such control, I-2(OCS)2 is produced most effectively by a limited set of pump-probe excitations at short delays. We emphasize generality of these results that relate to caging dynamics in any cluster ions.
| Original language | English (US) |
|---|---|
| Pages (from-to) | 5155-5158 |
| Number of pages | 4 |
| Journal | Journal of Chemical Physics |
| Volume | 108 |
| Issue number | 13 |
| DOIs | |
| State | Published - Apr 1 1998 |
| Externally published | Yes |
ASJC Scopus subject areas
- General Physics and Astronomy
- Physical and Theoretical Chemistry