Abstract. 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 10 nmol 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 12 nmol mol−1) and 20 % in the North Atlantic Ocean (12 nmol 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 62 mW 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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Abstract. 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, which considers not only the emissions of NO x (NO and NO 2 ), CO or non-methane hydrocarbons (NMHC) separately but the competing effects of all relevant ozone precursors. For summer conditions a contribution of land transport emissions to ground level ozone of up to 18 % in North America and South Europe is estimated, which corresponds to 12 nmol mol 10A 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 four for Europe). With respect to the contribution of land transport and ship traffic emissions to the tropospheric ozone burden we quantified values of 8 % and 6 % for the land transport and shipping emissions, respectively. Overall, the emissions from land transport contribute to around 20 % of the net ozone production near the source regions, while shipping emissions contribute up to 52 % to the net ozone production in the Northern Pacific. , respectively. Again these results are larger by a factor of 2-3 compared to previous studies using the perturbation approach, but largely agree with previous studies which investigated the difference between the tagging and the perturbation method. Overall our results highlight the importance of differing between the perturbation and the tagging approach, as they answer two different questions. We argue that only the tagging approach can estimate the contribution of emissions, while only 20 the perturbation approach investigates the effect of an emission change. To effectively asses mitigation options both approaches should be combined.

Abstract. 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 HO 2 is important as they play a crucial role for atmospheric chemistry. This study presents an advanced version of a tagging method for OH and HO 2 (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 HO 2 source by the reaction of H and O 2 , 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 HO 2 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 HO 2 , the contributions differ strongly in the categories biogenic emissions and methane decomposition. As HO x reacts with ozone (O 3 ), 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 O 3 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.