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Bulk and interface vibrational Raman spectroscopy with coherence modulated optical susceptibilities




Wilson, Jesse W., author
Bartels, Randy, advisor
Krapf, Diego, committee member
Marconi, Mario, committee member
Roberts, Jacob, committee member

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The effect on an ultrashort probe pulse of an impulsively prepared vibrational coherence is described by effective linear and nonlinear optical susceptibility perturbations. Linear susceptibility perturbations modulate both the amplitude and phase of a probe pulse. Three spectral interferometry methods are described for measuring this phase modulation, geared toward spectral resolution, noise suppression, and rapid data acquisition. Third-order nonlinear interactions perturbations may be used to acquire surface-specific Raman spectra. While second-order spectroscopy is an established surface-specific technique, odd-order methods have been passed over because the signal is generated in the bulk media. We show that through a surface Fresnel modulation, coherence-modulated third harmonic generation can be used to obtain surface-specific vibrational information. Bulk and interface contributions to the vibrational signal are separated by scanning the interface through the focus of the laser beam.


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impulsive stimulated Raman scattering
third harmonic generation
second hyper-Raman scattering


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