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CARS studies were performed on these zones in crystals with low polymer content, where the polymer chains were embedded in the monomer matrix As mentioned, resonance Raman excitation within the strong absorption of the polymer chains, i e within the absorption of the colour zone, produced high luminescence levels which obscured the bands in linear Raman spectroscopy In contrast, luminescence free resonance CARS spectra could be obtained as shown in Fig 61-23 for the case of an FBS DA crystal at 10 K temperature (FBS = 2,4-hexadiynylene-di-p-fluorobenzenesulfonate, DA = diacetylene) On the left and right panels of Fig 61-23 CARS spectra are displayed for the region of the C=C and C-C stretching region around IS00 cm and 2100 cm I, respectively Spectra (a) and (b) are those of the P-colour zone (P = principal) and (c) (I) those of the Y-colour zone (Y=yellow).

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Note the very different CARS intensities as well as bandshapes for the various excitation wavelengths of the pump laser (A,, which corresponds to U L of the CARS process as outlined in Sec 3622) which are due to different resonant enhancements Comparing spectrum (k) with (c), for example, shows in addition the very high dynamic range (at least four orders of magnitude) inherent in this type of spectroscopy Analyzing the CARS spectra together with the absorption spectra of several substituted DA crystals, the authors were able to derive important structural as well as electronic properties of this type of crystal For details on resonance CARS studies on various types of diacetylene single crystals we refer to the original literature (Materny and Kiefer, 1992 a-e, 1993; Materny et al, 1992 a-c; Ganz et al, 1993).

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