Road traffic emits not only carbon dioxide (CO2) and particulate matter, but also other pollutants such as nitrogen oxides (NOx), volatile organic compounds (VOCs) and carbon monoxide (CO). These chemical species influence the atmospheric chemistry and produce ozone (O3) in the troposphere. Ozone acts as a greenhouse gas and thus contributes to anthropogenic global warming. Technological trends and political decisions can help to reduce the O3 effect of road traffic emissions on climate. In order to assess the O3 response of such mitigation options on climate, we developed a chemistry-climate response model called TransClim (Modelling the effect of surface Transportation on Climate). The current version considers road traffic emissions of NOx, VOC and CO and determines the O3 change and its corresponding stratosphere-adjusted radiative forcing. Using a tagging method, TransClim is further able to quantify the contribution of road traffic emissions to the O3 concentration. Thus, TransClim determines the contribution to O3 as well as the change in total tropospheric O3 of a road traffic emission scenario. Both quantities are essential when assessing mitigation strategies. The response model is based on lookup tables which are generated by a set of emission variation simulations performed with the global chemistry-climate model EMAC (ECHAM5 v5.3.02, MESSy v2.53.0). Evaluating TransClim against independent EMAC simulations reveals low deviations of all considered species (0.01%-10%). Hence, TransClim is able to reproduce the results of an EMAC simulation very well. Moreover, TransClim is about 6000 times faster in computing the climate effect of an emission scenario than the complex chemistry-climate model. This makes TransClim a suitable tool to efficiently assess the climate effect of a broad range of mitigation options for road traffic or to analyse uncertainty ranges by employing Monte Carlo simulations.

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To mitigate the human impact on climate change, it is essential to determine the contribution of emissions to the concentration of trace gases. In particular, the source attribution of short-lived species such as OH and HO₂ is important as they play a crucial role for atmospheric chemistry. This study presents an advanced version of a tagging method for OH and HO₂ (HO_x) which attributes HO_x concentrations to emissions. While the former version (V1.0) only considered 12 reactions in the troposphere, the new version (V1.1), presented here, takes 19 reactions in the troposphere into account. For the first time, the main chemical reactions for the HO_x chemistry in the stratosphere are also regarded (in total 27 reactions). To fully take into account the main HO₂ source by the reaction of H and O₂, the tagging of the H radical is introduced. In order to ensure the steady-state assumption, we introduce rest terms which balance the deviation of HO_x production and loss. This closes the budget between the sum of all contributions and the total concentration. The contributions to OH and HO₂ obtained by the advanced tagging method V1.1 deviate from V1.0 in certain source categories. For OH, major changes are found in the categories biomass burning, biogenic emissions and methane decomposition. For HO₂, the contributions differ strongly in the categories biogenic emissions and methane decomposition. As HO_x reacts with ozone (O₃), carbon monoxide (CO), reactive nitrogen compounds (NO_y), non-methane hydrocarbons (NMHCs) and peroxyacyl nitrates (PAN), the contributions to these species are also modified by the advanced HO_x tagging method V1.1. The contributions to NO_y, NMHC and PAN show only little change, whereas O₃ from biogenic emissions and methane decomposition increases in the tropical troposphere. Variations for CO from biogenic emissions and biomass burning are only found in the Southern Hemisphere.

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We quantify the contribution of land transport and shipping emissions to tropospheric ozone for the first time with a chemistry-climate model including an advanced tagging method (also known as source apportionment), which considers not only the emissions of nitrogen oxides (NOx, NO, and NO2), carbon monoxide (CO), and volatile organic compounds (VOC) separately, but also their non-linear interaction in producing ozone. For summer conditions a contribution of land transport emissions to ground-level ozone of up to 18% in North America and Southern Europe is estimated, which corresponds to 12 and 10nmolĝ€†mol-1, respectively. The simulation results indicate a contribution of shipping emissions to ground-level ozone during summer on the order of up to 30% in the North Pacific Ocean (up to 12nmolĝ€†mol-1) and 20% in the North Atlantic Ocean (12nmolĝ€†mol-1). With respect to the contribution to the tropospheric ozone burden, we quantified values of 8 and 6% for land transport and shipping emissions, respectively. Overall, the emissions from land transport contribute around 20% to the net ozone production near the source regions, while shipping emissions contribute up to 52% to the net ozone production in the North Pacific Ocean. To put these estimates in the context of literature values, we review previous studies. Most of them used the perturbation approach, in which the results for two simulations, one with all emissions and one with changed emissions for the source of interest, are compared. For a better comparability with these studies, we also performed additional perturbation simulations, which allow for a consistent comparison of results using the perturbation and the tagging approach. The comparison shows that the results strongly depend on the chosen methodology (tagging or perturbation approach) and on the strength of the perturbation. A more in-depth analysis for the land transport emissions reveals that the two approaches give different results, particularly in regions with large emissions (up to a factor of 4 for Europe). Our estimates of the ozone radiative forcing due to land transport and shipping emissions are, based on the tagging method, 92 and 62mWĝ€†m-2, respectively. Compared to our best estimates, previously reported values using the perturbation approach are almost a factor of 2 lower, while previous estimates using NOx-only tagging are almost a factor of 2 larger. Overall our results highlight the importance of differentiating between the perturbation and the tagging approach, as they answer two different questions. In line with previous studies, we argue that only the tagging approach (or source apportionment approaches in general) can estimate the contribution of emissions, which is important to attribute emission sources to climate change and/or extreme ozone events. The perturbation approach, however, is important to investigate the effect of an emission change. To effectively assess mitigation options, both approaches should be combined. This combination allows us to track changes in the ozone production efficiency of emissions from sources which are not mitigated and shows how the ozone share caused by these unmitigated emission sources subsequently increases.

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Emissions of road traffic crucially influence Earth’s climate. The vehicle fleet emits not only carbon dioxide (CO2), but also nitrogen oxides (NOx), volatile organic compounds (VOC) and carbon monoxide (CO) which produce ozone (O3) and destroy methane (CH4) in the troposphere. As the demand of mobility is expected to further increase in future, a reduction of the climate effect from road traffic emissions is indispensable. Therefore, it is essential to assess the climate impact of emission changes caused by technological trends and mitigation strategies for road traffic. Several studies have already quantified the impact of road traffic emissions on climate. But climate simulations with complex chemistry climate models are still computational expensive hampering the assessment of many road traffic emission scenarios. Consequently, an efficient method for quantifying the climate impact and contribution of mitigation options is required. Within the scope of this thesis, a unique chemistry-climate response model called TransClim (Modelling the effect of surface Transportation on Climate) was developed. Using an efficient interpolation algorithm, it assesses the impact and the contribution of road traffic emission scenarios on O3 and CH4 concentration as well as their corresponding radiative forcings. Comparing the results delivered by TransClim with simulations of the complex global chemistry climate model EMAC reveals very low deviations (0.02 – 6 %). To determine not only the impact but also the contribution of road traffic emissions to O3, OH and CH4 in TransClim, a so-called tagging method is applied. It attributes the concentrations of trace gases to emission sources such as road traffic. This thesis presents an improved tagging method for the short-lived species OH and HO2 as well as a new method for CH4. Within the scope of this thesis, TransClim enabled to assess the climate effect of two scientific questions: first, the effect of three prospective mitigation options of German road traffic and second, two scenarios describing the cases that European vehicles use fuel blends containing a low and a high proportion of biofuels. Summing up, TransClim offers a new method to quickly assess the climate impact and the contribution of mitigation strategies for road traffic in a sufficiently accurate manner. As TransClim simulates about 6000 times faster than a complex chemistry climate model, it enables to quantify the effect of many emission scenarios in different regions.@en