Effect of density on the Raman scattering of molecular fluids. II. Study of intermolecular interaction in CO2

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Abstract
The low frequency intermolecular light scattering in CO2 was studied as a function of the gas and liquid density up to 560 amagats. At low gas density the shape of the observed spectrum can be described qualitatively by a contour describing the pure rotational S‐branch spectrum. Significant deviations from the pure rotational spectral shape were observed at increasing density, evolving into that resembling the collision‐induced type of the quasiexponential spectral shape found in monatomic fluids at high density. With the temperature properly scaled, the low frequency spectra of liquid and gaseous CO2 at the same density are superimposable. The integrated intensity of the low frequency depolarized Raman spectrum has also been measured as a function of density. An empirical method to correlate the low frequency spectral data is also introduced.