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Abstract
Polarization CARS spectroscopy is known to considerably enhance the CARS sensitivity of weak Raman resonances by background suppression in transparent media. Experimental control of the spectral line shape through polarization enables the determination of molecular parameters by line shape analysis. We demonstrate that polarization CARS can also be applied to absorbing substances, i.e., under electronic resonance conditions, for the case of pseudoisocyanine chloride. The spectra, recorded in the multiplex mode, are interpreted theoretically and the parameters involved in the third order susceptibility are determined from experiment. Multiplex performance of polarization CARS spectroscopy is also demonstrated for solutions of pyridine in water and benzene in carbon tetrachloride as transparent systems.
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