Pressure broadening in the 2 nu sub(3) band of methane and its implication on atmospheric retrievals

N sub(2)-broadened half widths and pressure shifts were obtained for transitions in the 2 nu sub(3) methane band. Laboratory measurements recorded at 0.011 cm super(− 1) resolution with a Bruker 120 HR Fouriertransform spectrometer were analysed from 5860 to 6185 cm super(− 1). A 140 cm gas cell was...

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Veröffentlicht in:Atmospheric chemistry and physics 2008-09, Vol.8 (17), p.5061-5075
Hauptverfasser: Frankenberg, C, Warneke, T, Butz, A, Aben, I, Hase, F, Spietz, P, Brown, L R
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Sprache:eng
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Zusammenfassung:N sub(2)-broadened half widths and pressure shifts were obtained for transitions in the 2 nu sub(3) methane band. Laboratory measurements recorded at 0.011 cm super(− 1) resolution with a Bruker 120 HR Fouriertransform spectrometer were analysed from 5860 to 6185 cm super(− 1). A 140 cm gas cell was filled with methane at room temperature and N sub(2) as foreign gas at pressures ranging from 125 to 900 hPa. A multispectrum nonlinear constrained least squares approach based on Optimal Estimation was applied to derive the spectroscopic parameters by simultaneously fitting laboratory spectra at different ambient pressures assuming a Voigt line-shape. At room temperature, the half widths ranged between 0.030 and 0.071 cm super(− 1) atm super(− 1), and the pressure shifts varied from -0.002 to -0.025 cm super(− 1) atm super(− 1) for transitions up to JQUOTATION_MARK=10. Especially for higher rotational levels, we find systematically narrower lines than HITRAN predicts. The Q and R branch of the new set of spectroscopic parameters is further tested with ground based direct sun Fourier transform infrared (FTIR) measurements where systematic fit residuals reduce by about a factor of 3-4. We report the implication of those differences on atmospheric methane measurements using high-resolution ground based FTIR measurements as well as low-resolution spectra from the SCanning Imaging Absorption SpectroMeter for Atmospheric ChartographY (SCIAMACHY) instrument onboard ENVISAT. We find that for SCIAMACHY, a latitudinal and seasonally varying bias of about 1% can be introduced by erroneous broadening parameters.
ISSN:1680-7316
1680-7324