Retrieval of tropospheric column-averaged CH4 mole fraction by solar absorption FTIR-spectrometry using N2O as a proxy

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Abstract

Tropospheric column-averaged CH4 mole fractions were derived from ground-based column absorption measurements. The method uses stratospheric N2O columns to correct for the stratospheric contribution to the CH4 total column. The method was applied to four Total Carbon Column Observing Network (TCCON) sites covering locations from the Northern Arctic to the tropics. It performs well for all sites. The derived tropospheric CH4 concentrations were compared with profiles measured by aircraft at three sites. The results indicate an inter-site consistency within 6 ppb (∼0.3%). With aircraft profiles up to 3 km, the seasonal behavior of the derived tropospheric CH4 concentration was also checked, revealing a difference of around 20 ppb. The mean relative uncertainty of the four sites, as estimated from the daily standard deviations, is 0.23%.

Figures

  • Figure 1. Correlations between the stratospheric mole fractions of N2O (right) and HF (left) with CH4 on a global scale. Correlation coefficient, slope and intercept are indicated in the legend. The data are from the ACE-FTS satellite.
  • Figure 2. The averaging kernels of HF, N2O and CH4 at Bialystok for all spectra from 2010. The colors indicate the solar zenith angle of the corresponding measurements.
  • Figure 3. Results at Spitsbergen, the red points correspond to the tropospheric column-averaged CH4 mole fraction derived from N2O, the blue to those derived using HF and the open circles are in situ CH4 data measured at Zeppelin mountain. The upper panel shows the difference between the in situ and tropospheric column-averaged CH4 mole fractions, the middle panel is the difference between the results using N2O and HF.
  • Figure 4. Same as Fig. 3 except for the Orléans site and with the black points in the lower panel representing tropospheric column-averaged CH4 mole fractions derived from low altitude aircraft flights at this site.
  • Figure 5. Same with Fig. 4 except for Bialystok.
  • Figure 6. Results at Darwin.
  • Figure 7. The multi-annual mean annual cycles of tropospheric column-averaged CH4 mole fraction for four sites. The red points correspond to the results derived from N2O and the blue to HF.
  • Figure 8. Comparison results with aircraft data. The aircraft profiles are smoothed using GFIT averaging kernels in troposphere using Eq. (14). The FTS data are averaged through aircraft measurements periods, and the error bars of FTS data are standard deviations of these averaged data.

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CITATION STYLE

APA

Wang, Z., Deutscher, N. M., Warneke, T., Notholt, J., Dils, B., Griffith, D. W. T., … Gerbig, C. (2014). Retrieval of tropospheric column-averaged CH4 mole fraction by solar absorption FTIR-spectrometry using N2O as a proxy. Atmospheric Measurement Techniques, 7(10), 3295–3305. https://doi.org/10.5194/amt-7-3295-2014

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