Resonance CARS and CSRS line shapes of Ni(II)-octaethylporphyrin

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Abstract
CARS and CSRS of Ni(II)‐octaethylporphyrin in benzene solution have been measured in the resonance condition with the first visible absorption (Q) band. The line shape behavior of some nontotally symmetric vibrations has been investigated by changing the pump frequency ω1 in the absorbing region, with the particular elaboration on 1308 cm−1 (A2g) line, which shows the inverse polarization and is most strikingly enhanced in ordinary resonance Raman. The observed line shapes were remarkably different between the CARS and CSRS by the common pumping frequency ω1. The whole result has been consistently interpreted in terms of the vibronic theory of Raman intensity, on the basis of semiclassical perturbation theory by Lotem et al. The effect of concurrent resonances of ω1 and ω3 (or ω2) has been demonstrated in a definite manner.