On the wintertime low bias of Northern Hemisphere carbon monoxide found in global model simulations
Résumé
The uncertainties in the global budget of carbon monoxide (CO) are assessed to explain causes for the long-standing issue of Northern Hemispheric wintertime underestimation of CO concentrations in global models. With a series of MOZART sensitivity simulations for the year 2008, the impacts from changing a variety of surface sources and sinks were analyzed. The model results were evaluated with monthly averages of surface station observations from the global CO monitoring network as well as with total columns observed from satellites and with vertical profiles from measurements on passenger aircraft. Our basic simulation using MACCity anthropogenic emissions underestimated Northern Hemispheric near-surface CO concentrations on average by more than 20 ppb from December to April with the largest bias over Europe of up to 75 ppb in January. An increase in global biomass burning or biogenic emissions of CO or volatile organic compounds (VOC) is not able to reduce the annual course of the model bias and yields too high concentrations over the Southern Hemisphere. Raising global annual anthropogenic emissions results in overestimations of surface concentrations in most regions all-year-round. Instead, our results indicate that anthropogenic emissions in the MACCity inventory are too low for the industrialized countries during winter and spring. Thus we found it necessary to adjust emissions seasonally with regionally varying scaling factors. Moreover, exchanging the original resistance-type dry deposition scheme with a parameterization for CO uptake by oxidation from soil bacteria and microbes reduced the boreal winter dry deposition fluxes and could partly correct for the model bias. When combining the modified dry deposition scheme with increased wintertime road traffic emissions over Europe and North America (factors up to 4.5 and 2, respectively) we were able to optimize the match to surface observations and to reduce the model bias significantly with respect to the satellite and aircraft observations. A reason for the apparent underestimation of emissions may be an exaggerated downward trend in the RCP8.5 scenario in these regions between 2000 and 2010, as this scenario was used to extrapolate the MACCity emissions from their base year 2000. This factor is potentially amplified by a lack of knowledge about the seasonality of emissions. A methane lifetime of 9.7 yr for our basic model and 9.8 yr for the optimized simulation agrees well with current estimates of global OH, but we cannot exclude a potential effect from errors in the geographical and seasonal distribution of OH concentrations. Finally, underestimated emissions from anthropogenic VOCs can also account for a small part of the missing CO concentrations.
Domaines
Sciences de l'environnement
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