Elsevier

Chemical Physics

Volume 52, Issue 3, November 1980, Pages 363-379
Chemical Physics

Theory of time-resolved level anticrossing experiment

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Abstract

The purpose of the present paper is to present a general treatment of steady state and time-resolved level-anticrossing (LAC) experiments using the generalized master equation approach in which both radiate and nonradiative decays and dephasing processes have been considered. Several models are treated to demonstrate the theoretical method. The theory is applicable to both atoms and molecules. It is shown that under appropriate conditions, as derived in this paper, quantum beats can be observed in the time-resolved LAC experiment. Numerical calculations have been performed to show the time-dependent behavior (build-up and decay) of the time-resolved LAC experiment. These quantum beats are then a direct measurement of the microscopic coupling parameters in intersystem crossing, etc. It will be shown that combining the steady state and the time-resolved LAC experiments one can determine not only the microscopic coupling parameters but also the relaxation and/or the dephasing rate constants. Hence the particular virtues of time dependent LAC experiments are seen in these model calculations.

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Permanent address: Department of Chemistry, Arizona State University, Tempe, Arizona 85281, USA.

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