Femtosecond real time probing of reactions XXII Kinetic description of probe absorption fluorescence depletion and mass spectrometry
作者:
SOREN PEDERSEN AHMED H ZEWAIL,
期刊:
Molecular Physics
(Taylor Available online 1996)
卷期:
Volume 89,
issue 5
页码: 1455-1502
ISSN:0026-8976
年代: 1996
DOI:10.1080/002689796173291
出版商: Taylor & Francis Group
数据来源: Taylor
摘要:
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.
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