Precise modelling of infrared absorption by carbon dioxide is of primary importance for radiative transfer calculations in CO-rich atmospheres like those of Venus and Mars. Despite various measurements and theoretical models dedicated to this subject, accurate data at different temperatures and pressures are still lacking in numerous spectral regions. In this work, using two Fourier Transform Spectrometers, we have measured spectra of pure CO in a large spectral region range, from 750 to 8500cm at various densities (3-57amagat) and temperatures (230-473K). Comparisons between measured dipolar absorption bands and spectra calculated with the widely used Lorentz line shape show very large discrepancies. This result is expected since the Lorentz approach neglects line-coupling effects due to intermolecular collisions which transfer absorption from the wings to the band center. In order to account for this effect, a theoretical approach based on the impact and Energy Corrected Sudden approximations has been developed. Comparisons of this model with numerous laboratory spectra in a wide range of pressure, temperature and spectral domain show satisfactory agreements for band centers and near wing regions where the impact approximation is valid. However, as expected, due to the breakdown of the impact approximation, the model fails when considering far wing regions. In the absence of precise models accounting for line-mixing and finite collision duration (non impact) effects, empirical approximations are proposed in order to model the far wings. © 2010 Elsevier Ltd.
Measurements and modelling of high pressure pure CO2 spectra from 750 to 8500cm-1. I-central and wing regions of the allowed vibrational bands
Snels M;
2011
Abstract
Precise modelling of infrared absorption by carbon dioxide is of primary importance for radiative transfer calculations in CO-rich atmospheres like those of Venus and Mars. Despite various measurements and theoretical models dedicated to this subject, accurate data at different temperatures and pressures are still lacking in numerous spectral regions. In this work, using two Fourier Transform Spectrometers, we have measured spectra of pure CO in a large spectral region range, from 750 to 8500cm at various densities (3-57amagat) and temperatures (230-473K). Comparisons between measured dipolar absorption bands and spectra calculated with the widely used Lorentz line shape show very large discrepancies. This result is expected since the Lorentz approach neglects line-coupling effects due to intermolecular collisions which transfer absorption from the wings to the band center. In order to account for this effect, a theoretical approach based on the impact and Energy Corrected Sudden approximations has been developed. Comparisons of this model with numerous laboratory spectra in a wide range of pressure, temperature and spectral domain show satisfactory agreements for band centers and near wing regions where the impact approximation is valid. However, as expected, due to the breakdown of the impact approximation, the model fails when considering far wing regions. In the absence of precise models accounting for line-mixing and finite collision duration (non impact) effects, empirical approximations are proposed in order to model the far wings. © 2010 Elsevier Ltd.I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.