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LINESHAPE ANALYSIS OF CLOSELY SPACED RAMAN LINES IN A RESONANCE ENHANCED COHERENT ANTI-STOKES RAMAN EXPERIMENT

Please use this identifier to cite or link to this item: http://hdl.handle.net/1811/11062

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Title: LINESHAPE ANALYSIS OF CLOSELY SPACED RAMAN LINES IN A RESONANCE ENHANCED COHERENT ANTI-STOKES RAMAN EXPERIMENT
Creators: Carreira, L. A.; Goss, L. P.; Antcliff, R. R.; Berkowitz, D.; Irwin, R. M.
Issue Date: 1979
Abstract: When multiple vibrations of interest are close to each other, in a CARS experiment, many cross terms must be taken into account. These include not only neighboring peaks, but peaks up to $50 cm^{-1}$ away. The intensity of such a system is given by: \begin{eqnarray*} && |X(1)|^{2} = \theta^{2} \sum^{N}_{r = 1} \frac{R_{r} \delta_{r} - l_{r} r_{r}}{\delta^{2}_{r} + r^{2}_{r}}\\ && +\sum^{N}_{r = 1} \sum^{N}_{r =1} \left[(R_{r} R_{r^{\prime}} + l_{r} l_{r^{\prime}})(\delta_{r} \delta_{r^{\prime}} + r_{r} r_{r^{\prime}}), (l_{r} R_{r^{\prime}} - R_{r} l_{r^{\prime}})\delta_{r} \delta_{r} + (l_{r^{\prime}} R_{r} - R_{r^{\prime}} l_{r}) \delta_{r^{\prime}} r_{r}\right]/(\delta^{2}_{r} + r^{2}_{r})(\delta^{2}_{r^{\prime}} + r^{2}_{r^{\prime}}) \end{eqnarray*} where N = Number of peak Expanding the summations leads to four distinct types of terms. They are a) background terms, b) pure Lorentzian terms, c) solvent-solute cross terms and d) solute-solute (Raman-Raman) terms. With multiple cross terms possible, it is necessary to develop a technique to be able to extract the real and imaginary parts of the third order susceptibility associated with each peak in order to extract meaningful excitation profiles near resonance. The method developed in our laboratory will be presented along with an application to the analysis of the resonance enhanced bands of N,N–diethyl paranitros oaniline in the $1300-1500 cm^{-1}$ region.
URI: http://hdl.handle.net/1811/11062
Other Identifiers: 1979-TH-04
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