Abstract
The theory for the application of spectrally tailored (‘two color’) noisy light in an interferometric coherent Raman scattering (CRS) experiment called I(2)CRS(3c) is presented. The theory is concerned with the purely resonant contribution to the intensity level I(2)CRS(3c) signal. The tailored beam is modeled as a sum of two Lorentzians where the center frequency of each Lorentzian is assumed to be under experimental control. It is found that not only are the coherent Stokes–Raman scattering (CSRS) and coherent anti-Stokes–Raman scattering (CARS) signals emitted, but a third ‘hybrid’ frequency is also contained in the signal. It offers the promise of a new way to up-convert low frequency Raman active modes, while the same dynamic information contained in the radiation difference oscillations (RDOs) of previous incoherent CRS experiments remains. More generally, it offers an additional degree of freedom that allows for arbitrary experimental control over the position in frequency space in which the hybrid signal will emerge. In addition it is shown that the hybrid signal frequency contains dynamically important information in its arbitrarily placed (in frequency space) signal. Plots of monochromatically detected I(2)CRS(3c) interferograms calculated for different parameter sets are shown together with the signal spectra. © 1997 John Wiley & Sons, Ltd.
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