Graduate Thesis Or Dissertation
 

Applications of nonlinear raman spectroscopy

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  • Two nonlinear optical experiments are presented in which the third-order electronic susceptibility of molecules is used to generate Raman signals. The first one uses a single 532 nm beam from a Nd:YAG laser to produce Stimulated Raman Scattering in benzene and deuterated benzene. With a simple experimental set-up, stimulated emission involving CC and CH (CD) stretching modes from both C₆H₆ and C₆D₆ can be visually witnessed. Collinear and conical stimulated Raman beams are observed and explained. Measuring the wavelengths of the coherent beams with a meter stick and a grating permits the calculation of CC and CH force constants in benzene. This experiment has been developed as a lab in graduate and undergraduate courses and has been submitted to J. Chem. Ed. for publication. The second experiment uses a high resolution Coherent Anti-Stokes spectrometer to investigate the v₁ vibrational mode of the CD₃ radical produced by photolysis of CD₃I. Calibrated spectra are obtained at much higher resolution than in an earlier published study and efforts are described to improve the range of data and to reconcile differences between the spectra. Modeling of the spectra leads to a "best fit" set of vibration-rotation parameters for CD₃ but a completely satisfactory fit of both high and low resolution spectra was not achieved.
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