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Picosecond spectroscopy of van der Waals clusters


Willberg, Dean Michael (1994) Picosecond spectroscopy of van der Waals clusters. Dissertation (Ph.D.), California Institute of Technology. doi:10.7907/605h-j578.


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This thesis presents pump/probe picosecond spectroscopic investigations of the dynamics of van der Waals clusters. The first phase of these investigations was the construction of a laboratory specifically designed for van der Waals cluster research consisting of a molecular beam apparatus and a two-color picosecond laser system. It is possible to perform both time resolved laser induced fluorescence (LE), and multi-photon ionization (MPI) experiments in this laboratory. A description of the construction and operation of the laboratory, focusing on the laser system, is presented. A full account of the real-time studies of the vibrational predissociation of [...] clusters where [...] is given. The first set of experiments described is the measurement of the rates of vibrational predissociation for [...] clusters. The results for [...] are compared with a number of theoretical models of vibrational predissociation, specifically focusing on the dependence of the rates on the initially prepared vibrational state of the cluster. The results for the [...] cluster are described in terms of the competition between two relaxation channels: vibrational predissociation of the van der Waals cluster, and electronic predissociation of the [...] moiety. The second set of experiments are the analogous measurements of the rates of vibrational predissociation of [...] clusters. These results are compared with the [...] results, as well as with lifetime estimates available from high resolution spectroscopy. The final chapter in this series describes our investigation of vibrational predissociation and intramolecular vibrational energy relaxation in [...] clusters. The dynamics of these larger clusters are inherently more complicated than when n = 1, however, a quantitative model for the fragmentation of n = 2 clusters is presented. This thesis also presents a preliminary description of an ongoing MPI experiment on the dynamics of t-stilbene clusters.

Item Type:Thesis (Dissertation (Ph.D.))
Degree Grantor:California Institute of Technology
Division:Chemistry and Chemical Engineering
Major Option:Chemistry
Thesis Availability:Public (worldwide access)
Research Advisor(s):
  • Zewail, Ahmed H.
Thesis Committee:
  • Unknown, Unknown
Defense Date:9 July 1993
Record Number:CaltechETD:etd-04042008-110156
Persistent URL:
Default Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:1270
Deposited By: Imported from ETD-db
Deposited On:04 Apr 2008
Last Modified:16 Apr 2021 23:11

Thesis Files

PDF (Willberg_dm_1994.pdf) - Final Version
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