Abstract

The usefulness of multiresonant nonlinear spectroscopy for analyzing complicated mixtures requires understanding of the factors controlling the relative signal positions and intensities of individual components. In this study the effects of different types of detuning from resonance, of the interactions of such detunings, and of the incident laser powers are illustrated. CARS spectra specific to the different pentacene sites in <i>p</i>-terphenyl are observed for different types of detunings from resonance, and the complications introduced by multiple components are interpreted. Population changes at moderate laser powers due to resonance with the allowed <i>S</i>₀ to <i>S</i>₁ transition lead to striking changes in the observed spectra, and markedly affect the interpretation of the observed resonances.

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