Contribution of emissions to concentrations

Abstract

Questions such as “what is the contribution of road traffic emissions to climate change?” or “what is the impact of shipping emissions on local air quality?” require a quantification of the contribution of specific emissions sectors to the concentration of radiatively active species and air-quality-related species, respectively. Here, we present a diagnostics package, implemented in the Modular Earth Submodel System (MESSy), which keeps track of the contribution of source categories (mainly emission sectors) to various concentrations. The diagnostics package is implemented as a submodel (TAGGING) of EMAC (European Centre for Medium-Range Weather Forecasts – Hamburg (ECHAM)/MESSy Atmospheric Chemistry). It determines the contributions of 10 different source categories to the concentration of ozone, nitrogen oxides, peroxyacytyl nitrate, carbon monoxide, non-methane hydrocarbons, hydroxyl, and hydroperoxyl radicals ( =  tagged tracers). The source categories are mainly emission sectors and some other sources for completeness. As emission sectors, road traffic, shipping, air traffic, anthropogenic non-traffic, biogenic, biomass burning, and lightning are considered. The submodel obtains information on the chemical reaction rates, online emissions, such as lightning, and wash-out rates. It then solves differential equations for the contribution of a source category to each of the seven tracers. This diagnostics package does not feed back to any other part of the model. For the first time, it takes into account chemically competing effects: for example, the competition between NOx, CO, and non-methane hydrocarbons (NMHCs) in the production and destruction of ozone. We show that the results are in-line with results from other tagging schemes and provide plausibility checks for concentrations of trace gases, such as OH and HO2, which have not previously been tagged. The budgets of the tagged tracers, i.e. the contribution from individual source categories (mainly emission sectors) to, e.g., ozone, are only marginally sensitive to changes in model resolution, though the level of detail increases. A reduction in road traffic emissions by 5 % shows that road traffic global tropospheric ozone is reduced by 4 % only, because the net ozone productivity increases. This 4 % reduction in road traffic tropospheric ozone corresponds to a reduction in total tropospheric ozone by  ≈  0.3 %, which is compensated by an increase in tropospheric ozone from other sources by 0.1 %, resulting in a reduction in total tropospheric ozone of  ≈  0.2 %. This compensating effect compares well with previous findings. The computational costs of the TAGGING submodel are low with respect to computing time, but a large number of additional tracers are required. The advantage of the tagging scheme is that in one simulation and at every time step and grid point, information is available on the contribution of different emission sectors to the ozone budget, which then can be further used in upcoming studies to calculate the respective radiative forcing simultaneously.