Intermediate case radiationless decay: the excited state dynamics of pyrazine (original) (raw)
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1B3u Pyrazine. Experimental Tests of the Theory of Radiationless Transitions
Laser Chemistry, 1983
Pyrazine (1,4-diazabenzene) has played a central role in the development of the theory of radiationless transitions. In this paper, we will describe studies of the decay behavior and fluorescence quantum yield of the isolated molecule and several of its isotopically labelled derivatives following pulsed dye laser excitation of “single” rotational levels of the 1B3u (nπ*) state in a seeded supersonic jet, both in the presence and absence of an external magnetic field. We shall demonstrate that pyrazine can be transformed from a “small” molecule to a “large” molecule by very small perturbations; e.g., by climbing up the rotational ladder of the first excited singlet state, by isotopic labeling, and/or by applying dc magnetic fields of the order of 100 G. Thus, the experiments provide important tests of the predictions of the theory for the first time. Specifically, we will show that, under “intermediate-case” conditions, (1) the fast component of the decay is indeed coherent in nature...
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