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Light emission under near-resonant excitation by a pulsed optical field is described using a semiclassical (Bloch) model for the near-resonant transition. Adiabatic excitation of this transition leads to Raman emission, whereas nonadiabaticity gives fluorescence. The model describes quantitatively observed relaxation effects. It further predicts that such experiments can determine the power spectrum of the correlation function characterizing collisions, offering an alternative to off-resonance spectroscopy.
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Szöke et al. (1975) studied this question.
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