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Femtosecond real-time probing of reactions XXII. Kinetic description of probe absorption, fluorescence, depletion and mass spectrometry

Pedersen, Soren and Zewail, Ahmed (1996) Femtosecond real-time probing of reactions XXII. Kinetic description of probe absorption, fluorescence, depletion and mass spectrometry. Molecular Physics, 89 (5). pp. 1455-1502. ISSN 0026-8976. doi:10.1080/002689796173291. https://resolver.caltech.edu/CaltechAUTHORS:20160831-095952077

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Abstract

A theoretical description of femtosecond transition-state dynamics is developed and compared with experimental results, with numerous examples. We focus on the population flow, employing a kinetic model, with the objective of studying the general trends and signal control parameters; we do not include coherence for the sake of acquiring a simplified picture with operational parameters. Different methods of detection are addressed, such as laser-induced fluorescence, depletion, absorption, and mass spectrometry. The response of the molecular system is derived for various types of dynamics with one or more rate determining processes. The significance of the relative time scales associated with the rates is explored and the effect on transients of the ratio of probing cross-sections is examined. Furthermore, the influence on the observed signal of the finite temporal width and shape of the laser pulses is quantified. Effects are discussed both in the unsaturated and saturated regimes of transition probabilities, demonstrating characteristic features of both regimes.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1080/002689796173291DOIArticle
http://www.tandfonline.com/doi/abs/10.1080/002689796173291PublisherArticle
Additional Information:© 1996 Taylor & Francis.
Issue or Number:5
DOI:10.1080/002689796173291
Record Number:CaltechAUTHORS:20160831-095952077
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20160831-095952077
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:70067
Collection:CaltechAUTHORS
Deposited By: Ruth Sustaita
Deposited On:31 Aug 2016 17:28
Last Modified:11 Nov 2021 04:23

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