The form of the emission spectrum induced by scattering of a generalised light pulse from a single resonance is calculated from the known time dependence of such scattering. It is shown that the intensity of the scattered light is given by |F(ν)|2 = |Gai(ν)|2 |S(ν)|2, where F(ν), S(ν), and Gai(ν) are the probability amplitudes of the scattered light, the excitation source and the resonance at frequency ν. The implications of this equation in the interpretation of scattering experiments is discussed. In particular, defining resonance Raman scattering as that scattering in which the scattered light has the same bandwidth as the exciting light, it is concluded that although resonance Raman and resonance fluorescence spectra correspond to limiting cases of resonance scattering spectra, spectra in intermediate cases cannot be resolved into a sum of a Raman spectrum and a resonance fluorescence spectrum.
Chemical Physics Letters37, no. 2: 339–342.
The authors were affiliated with the National Research Council of Canada, Division of Chemistry when they authored this article.