Constraining CO emission estimates using atmospheric observations

Abstract

We apply a four-dimensional variational (4D-Var) data assimilation system to optimize carbon monoxide (CO) emissions and to reduce the uncertainty of emission estimates from individual sources using the chemistry transport model TM5. In the first study only a limited amount of surface network observations from the National Oceanic and Atmospheric Administration Earth System Research Laboratory (NOAA/ESRL) Global Monitoring Division (GMD) is used to test the 4D-Var system. Uncertainty reduction up to 60% in yearly emissions is observed over well-constrained regions and the inferred emissions compare well with recent studies for 2004. However, since the observations only constrain total CO emissions, the 4D-Var system has difficulties separating anthropogenic and biogenic sources in particular. The inferred emissions are validated with NOAA aircraft data over North America and the agreement is significantly improved from the prior to posterior simulation. Validation with the Measurements Of Pollution In The Troposphere (MOPITT) instrument shows a slight improved agreement over the well-constrained Northern Hemisphere and in the tropics (except for the African continent). However, the model simulation with posterior emissions underestimates MOPITT CO total columns on the remote Southern Hemisphere (SH) by about 10%. This is caused by a reduction in SH CO sources mainly due to surface stations on the high southern latitudes. In the second study, we compare two global inversions to estimate carbon monoxide (CO) emissions for 2004. Either surface flask observations from NOAA or CO total columns from the MOPITT instrument are assimilated in a 4D-Var framework. In the Southern Hemisphere (SH) three important findings are reported. First, due to their different vertical sensitivity, the stations-only inversion increases SH biomass burning emissions by 108 Tg CO/yr more than the MOPITT-only inversion. Conversely, the MOPITT-only inversion results in SH natural emissions (mainly CO from oxidation of NMVOCs) that are 185 Tg CO/yr higher compared to the stations-only inversion. Second, MOPITT-only derived biomass burning emissions are reduced with respect to the prior which is in contrast to previous (inverse) modeling studies. Finally, MOPITT derived total emissions are significantly higher for South America and Africa compared to the stations-only inversion. This is likely due to a positive bias in the MOPITT V4 product. This bias is also apparent from validation with surface stations and ground-truth FTIR columns. In the final study we present the first inverse modeling study to estimate CO emissions constrained by both surface (NOAA) and satellite (MOPITT) observations using a bias correction scheme. This approach leads to the identification of a positive bias of maximum 5 ppb in MOPITT column-averaged CO mixing ratios in the remote Southern Hemisphere (SH). The 4D-Var system is used to estimate CO emissions over South America in the period 2006-2010 and to analyze the interannual variability (IAV) of these emissions. We infer robust, high spatial resolution CO emission estimates that show slightly smaller IAV due to fires compared to the Global Fire Emissions Database (GFED3) prior emissions. Moreover, CO emissions probably associated with pre-harvest burning of sugar cane plantations are underestimated in current inventories by 50-100%