Some properties of multiresonance CARS spectra of polyatomic molecules in condensed phases are briefly discussed with reference to the possible effects of having a transfer of population under one-photon resonance conditions. Some experimental results are presented for the case of quinizarin in chloroform solution at room temperature. The observation of vibrational resonances of the first excited state as well as evidences of the participation of higher excited states to the multiresonant processes clearly indicate the need to go beyond the usual four level system description of the CARS spectra.
Volume 135, 2023
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