The isotropic spectrum of the CO2 Raman 2 nu(3) overtone: A line-mixing band shape analysis at pressures up to several tens of atmospheres

A line-mixing shape analysis of the isotropic remnant Raman spectrum of the 2 nu(3) overtone of CO2 is reported at room temperature and for densities, rho, rising up to tens of amagats. The analysis, experimental and theoretical, employs tools of non-resonant light scattering spectroscopy and uses t...

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Bibliographic Details
Published in:The Journal of chemical physics 2011-06, Vol.134 (22)
Main Authors: Verzhbitskiy, I.-A., Kouzov, A.-P., Rachet, Florent, Chrysos, Michel
Format: Article
Language:English
Subjects:
Chemical Sciences
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Summary:A line-mixing shape analysis of the isotropic remnant Raman spectrum of the 2 nu(3) overtone of CO2 is reported at room temperature and for densities, rho, rising up to tens of amagats. The analysis, experimental and theoretical, employs tools of non-resonant light scattering spectroscopy and uses the extended strong collision model (ESCM) to simulate the strong line mixing effects and to evidence motional narrowing. Excellent agreement at any pressure is observed between the calculated spectra and our experiment, which, along with the easy numerical implementation of the ESCM, makes this model stand out clearly above other semiempirical models for band shape calculations. The hitherto undefined, explicit rho-dependence of the vibrational relaxation rate is given. Our study intends to improve the understanding of pressure-induced phenomena in a gas that is still in the forefront of the news. (C) 2011 American Institute of Physics. [doi:10.1063/1.3596750]
ISSN:0021-9606
1089-7690
DOI:10.1063/1.3596750