- Conference date: 29 Aug - 1 Sep 1999
- Location: Kobe-Sanda (Japan)
We calculated the 3rd-, 5th-, and 7th-order Raman signals for an Iodine dimer in the condensed phase, which was modeled by a Morse potential coupled to a heat bath. It is shown that the 5th- and 7th-order signals are very sensitive to the anharmonicity of the potential and useful to study intramolecular vibrational modes. In the case of harmonic vibrational modes, the 5th- and 7th-order signals are the function of both the linear and nonlinear linear coordinate dependence of the polarizability, whereas the present case they are the function of the linear coordinate dependence of the polarizability. Thus, the signals in the present case are expected to be much stronger than in the harmonic case. We also showed that the 7th-order 2D signal for a harmonic system with a nonlinear system-bath interaction, which is a possible model of an inhomogeneously distributed molecular-vibrational system, depends in the lowest order on the nonlinear coordinate dependence of the polarizability and is useful to see the effects of the inhomogeneity, in cases where the 5th-order 2D signals were very weak.
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