Off-resonant fifth-order response function for two-dimensional Raman spectroscopy of liquids CS2 and H2O |
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Authors: | Saito Shinji Ohmine Iwao |
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Institution: | Department of Chemistry, Faculty of Science, Nagoya University, Furo-cho, Chikusa-ku, Nagoya, 464-8602, Japan. shinji@mbox.chem.nagoya-u.ac.jp |
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Abstract: | The off-resonant fifth-order response functions for two-dimensional (2D) Raman spectroscopy of molecular liquids CS2 and H2O are investigated by using molecular dynamics calculation. This spectroscopy, able to deal with a phase space dynamics, shows the existence of nodal lines in several polarization tensor elements see L. Kaufman et al., Phys. Rev. Lett. 88, 207402 (2002) for experimental results]. The nodal property is found to arise from the dynamical couplings among rotational modes, not accounted for in a normal mode picture. The effects of anharmonicities and "mode coupling through polarizability" are also investigated by comparing the 2D Raman signal with a constant temperature velocity reassignment echo method. |
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