Fifth-order two-dimensional Raman spectroscopy of liquid water, crystalline ice Ih and amorphous ices: sensitivity to anharmonic dynamics and local hydrogen bond network structure |
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Authors: | Saito Shinji Ohmine Iwao |
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Institution: | Department of Computational Molecular Science, Institute for Molecular Science, Myodaiji, Okazaki, Aichi 444-8585, Japan. shinji@ims.ac.jp |
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Abstract: | The theoretical study of off-resonant fifth-order two-dimensional (2D)-Raman spectroscopy is made to analyze the intermolecular dynamics of liquid and solid water. The 2D-Raman spectroscopy is susceptible to the nonlinear anharmonic dynamics and local hydrogen bond structure in water. It is found that the distinct 2D-Raman response appears as the negative signal near the t(2) axis. The origin of this negative signal for t(2)<15 fs is from the nonlinear polarizability in the librational motions, whereas that for 30 fs
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