Analyzing atomic liquids and solids by means of two-dimensional Raman spectra in frequency domain.
A practical method to evaluate the contributions of the nonlinear polarizability and anharmonicity of potentials from the experimental and simulation data by using double Fourier transformation is presented. In a Lennard-Jones potential system, an approximated expression of the fifth-order response function using the ratio between nonlinear polarizability and anharmonicity exhibits a good agreement with the results of the molecular dynamics simulation. In a soft-core case, the fifth-order Raman signal indicates that the system consists of the delocalized and localized modes, and only the delocalized mode affects the dramatic change of the fifth-order Raman response functions between solid and liquid phases through nonlinear polarizability.
Nagata
Yuki
Y
Department of Chemistry, Graduate School of Science, Kyoto University, Sakyoku, Kyoto 606-8502, Japan. nagata@kuchem.kyoto-u.ac.jp
Hasegawa
Taisuke
T
Tanimura
Yoshitaka
Y