Pressure broadening in the 2ν3 band of methane and its implication on atmospheric retrievals
1Netherlands Institute for Space Research, Sorbonnelaan 2, 3584 CA Utrecht, The Netherlands
2Institute of Environmental Physics, Otto-Hahn-Allee 1, 28359 Bremen, Germany
3Institut für Meteorologie und Klimaforschung, Forschungszentrum Karlsruhe, 76021 Karlsruhe, Germany
4Jet Propulsion Laboratory, California Institute of Technology, 4800 Oak Grove Drive, Pasadena, CA 91109, USA
Abstract. N2-broadened half widths and pressure shifts were obtained for transitions in the 2ν3 methane band. Laboratory measurements recorded at 0.011 cm−1 resolution with a Bruker 120 HR Fouriertransform spectrometer were analysed from 5860 to 6185 cm−1. A 140 cm gas cell was filled with methane at room temperature and N2 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−1 atm−1, and the pressure shifts varied from –0.002 to –0.025 cm−1 atm−1 for transitions up to J"=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.
Citation: Frankenberg, C., Warneke, T., Butz, A., Aben, I., Hase, F., Spietz, P., and Brown, L. R.: Pressure broadening in the 2ν3 band of methane and its implication on atmospheric retrievals, Atmos. Chem. Phys., 8, 5061-5075, doi:10.5194/acp-8-5061-2008, 2008.