REMPI detection of photofragments is discussed as a probe technique to measure the angular distribution of the velocity as well as the angular correlation between velocity and angular momentum existing in fragments formed during a polarized photolysis. The symmetry properties of the REMPI probe process induced by polarized light are expressed in terms of sensitivity to the moments of the rotational angular momentum distribution and the angular state of the photofragment is described in the formalism of bipolar moments. Original explicit expressions of the ion velocity profiles are given with probe geometry characteristics as parameters for two kinds of fragment detection (time-of-flight mass spectrometry and angular measurements of the ion yield) and the consequences of the v–J correlation on the observed profiles are discussed. Some experimental geometries are proposed in order to either determine the angular correlation or to avoid its effects.
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Mons et al. (1989) studied this question.