1Department of Physics, University of Toronto, Toronto, ON, Canada
2JIFRESSE, University of California, Los Angeles, Los Angeles, CA, USA
3National Center for Atmospheric Research, Boulder, CO, USA
4Department of Mechanical Engineering, University of Colorado Boulder, Boulder, CO, USA
*now at: Jet Propulsion Laboratory, California Institute of Technology, Pasadena CA, USA
Received: 08 Aug 2014 – Discussion started: 08 Sep 2014
Abstract. We assessed the sensitivity of regional CO source estimates to the modeled vertical CO distribution by assimilating multi-spectral MOPITT (Measurements of Pollution In The Troposphere) V5J CO retrievals with the GEOS-Chem model. We compared the source estimates obtained by assimilating the CO profiles and the surface layer retrievals from June 2004 to May 2005. Because the surface layer retrievals are less sensitive to CO in the free troposphere, it is expected that they should provide constraints in the CO source estimates that are less sensitive to the vertical structure of CO in the free troposphere. The inferred source estimates all suggest a reduction in CO emissions in the tropics and subtropics, and an increase in the extratropics over the a priori estimates. The tropical decreases were particularly pronounced for regions where the biogenic source of CO was dominant, suggesting an overestimate of the a priori isoprene source of CO in the model. We found that the differences between the regional source estimates inferred from the profile and surface layer retrievals for 2004–2005 were small, generally less than 10% for the main continental regions, except for estimates for southern Asia, North America, and Europe. Because of discrepancies in convective transport in the model, the CO source estimates for India and southeastern Asia inferred from the CO profiles were significantly higher than those estimated from the surface layer retrievals during June–August 2004. On the other hand, the profile inversion underestimated the CO emissions from North America and Europe compared to the assimilation of the surface layer retrievals. We showed that vertical transport of air from the North American and European boundary layers is slower than from other continental regions, and thus air in the free troposphere from North America and Europe in the model is more chemically aged, which could explain the discrepancy between the source estimates inferred from the profile and surface layer retrievals. We also examined the impact of the OH distribution on the source estimates and found that the discrepancies between the source estimates obtained with two OH fields were larger when using the profile data, which is consistent with greater sensitivity to the more chemically aged air in the free troposphere. Our findings indicate that regional CO source estimates are sensitive to the vertical CO structure. They suggest that diagnostics to assess the age of air from the continental source regions should help interpret the results from CO source inversions. Our results also suggest that assimilating a broader range of composition measurements to provide better constraint on tropospheric OH and the biogenic sources of CO is essential for reliable quantification of the regional CO budget.
Revised: 05 Jan 2015 – Accepted: 08 Jan 2015 – Published: 11 Feb 2015
Jiang, Z., Jones, D. B. A., Worden, H. M., and Henze, D. K.: Sensitivity of top-down CO source estimates to the modeled vertical structure in atmospheric CO, Atmos. Chem. Phys., 15, 1521-1537, doi:10.5194/acp-15-1521-2015, 2015.