The chemical sink of atmospheric methane (CH₄) depends on the temperature and on the chemical composition. Here, we assess the feedback on atmospheric CH₄ induced by changes in the chemical sink in a warming climate using a CH₄-emission-flux-driven set-up of the chemistry-climate model EMAC (ECHAM/MESSy Atmospheric Chemistry), in which the chemical feedback of CH₄ mixing ratios can evolve explicitly. We perform idealized perturbation simulations driven either by increased carbon dioxide (CO₂) mixing ratios or by increased CH₄ emission fluxes. The CH₄ emission flux perturbation leads to a large increase of CH₄ mixing ratios. Remarkably, the factor by which the CH₄ mixing ratio increases is larger than the increase factor of the emission flux, because the atmospheric lifetime of CH₄ is extended. In contrast, the individual effect of the global surface air temperature (GSAT) increase is to shorten the CH₄ lifetime, which results in a significant reduction of CH₄ mixing ratios in our set-up. The corresponding radiative feedback is estimated at -0.041 and -0.089 W m^-2 K^-1 for the CO₂ and CH₄ perturbation, respectively. The explicit response of CH₄ mixing ratios leads to secondary feedbacks on the hydroxyl radical (OH) and ozone (O₃). Firstly, the OH response includes the CH₄-OH feedback, which enhances the CH₄ lifetime change, and, secondly, the formation of tropospheric O₃ is reduced.

We quantify the contributions of emissions from the transport sector to tropospheric ozone and the hydroxyl radical (OH) by means of model simulations with a global chemistry-climate model equipped with a source attribution method. For the first time we applied a method which also allows for quantifying contributions to OH which is invariant upon disaggregation or recombination and additive. Based on these quantified contributions, we analyse the ozone radiative forcing (RF) and methane lifetime reductions attributable to emissions from the transport sectors. The contributions were analysed for each transport sector separately and for 2015 as well as for 2050 under the Shared Socioeconomic Pathways (SSPs) SSP1-1.9, SSP2-4.5, and SSP3-7.0. In line with previous publications using the source attribution approach, we quantify ozone RF attributable to emissions from land transport, shipping, and aviation for the year 2015 of 121, 60, and 31 mW m−2, respectively. At the same time, we diagnose a relative reduction in methane lifetime due to transport emissions of 14.3 % (land transport), 8.5 % (shipping), and 3.8 % (aviation). These reductions are significantly larger than reported by previous studies due to the application of the source attribution method. Compared to 2015, only SSP1-1.9 shows a strong decrease in ozone RF and methane lifetime reduction attributable to the entire transport sector in 2050. For the projections of SSP2-4.5, we find similar effects of the total transport sector as for 2015, while the effects in SSP3-7.0 increase compared to 2015. This small change in the effects for the two projections compared to 2015 is caused by two main factors. Firstly, aviation emissions are projected to increase in SSP2-4.5 (increase of 107 %) and SSP3-7.0 (+86 %) compared to 2015, resulting in projected ozone RF of 55 mW m−2 (+78 %) and 50 mW m−2 (+61 %) for the year 2050 from aviation emissions. Secondly, the non-linear effects of atmospheric chemistry in polluted regions such as Europe and North America lead to rather small reductions in ozone and OH in response to emission reductions, especially from land transport emissions. In addition, the increase in emissions from land transport in other parts of the world, particularly in South Asia, leads to an increased contribution of ozone and OH. In particular, ozone formed by land transport emissions from South Asia causes strong RF that partially offsets the reductions in Europe and North America. Moreover, our results show that besides the non-linear response, lack of international cooperation, as in the SSP3-7.0 projection, hinders mitigation of ground-level ozone.

Flight altitude is relevant to the climate effects resulting from aircraft emissions. Other research has shown that flying higher within the troposphere leads to larger warming from O ₃ production. Aircraft NO _x emissions are of particular interest, as they lead to warming via the short-term production of O ₃, but also to reduced warming via processes like CH ₄ depletion. We focus on short-term O ₃ production, as it constitutes one of aviation’s largest warming components. Understanding how O ₃ formation varies altitudinally throughout the upper troposphere/lower stratosphere is essential for designing climate-compatible aircraft and routing. We quantify this variation by performing simulations with a global atmospheric chemistry model for three representative cruise altitudes, five regions and two seasons using three methods: Eulerian tagging, perturbation and Lagrangian tagging. This multi-method, regional approach overcomes limitations of previous studies that utilize only one of these methods and apply global emission inventories biased towards present-day flight distributions, thus limiting their applicability to future aviation scenarios. Our results highlight that underrepresenting emissions in areas with growing flight activity (e.g. Asia Pacific) may lead to significant, regional underestimations of the altitudinal sensitivity of short-term NO _x -related O ₃ warming effects in certain cases. We find that emitting in Southern regions, like Australasia, leads to warming larger by a factor of two when compared to global averages. Our findings also suggest that flying lower translates to lower warming from short-term O ₃ production and that this effect is strongest during the local summer. We estimate differences ranging from a factor of 1.2-2.6 between tagging and perturbation results that are attributable to non-linearities of NO _x -O ₃ chemistry, and derived regional correction factors for a widely-used sub-model. Overall, we stress that a combination of all three methods is necessary for a robust assessment of aviation climate effects as they address fundamentally different questions.

Emissions of land transport and anthropogenic non-traffic emissions (e.g. industry, households and power generation) are significant sources of nitrogen oxides, carbon monoxide and volatile organic compounds (VOCs). These emissions are important precursors of tropospheric ozone and affect air quality. The contribution of the emission sectors to ozone cannot be measured directly but can only be calculated using sophisticated atmospheric chemistry models. For this study we apply the MECO(n) model system (MESSy-fied ECHAM and COSMO models nested n times) equipped with a source attribution method to investigate the contribution of various sources to ground-level ozone in Europe. Compared to previous source apportionment studies for Europe, for the first time we apply a combined NOx–VOC tagging implemented in an online nested global–regional chemistry–climate model to achieve a finer resolution over central Europe (12 km) but concurrently incorporating the effect of long-range transport. We distinguish 10 different source sectors and 4 geographical source regions, analysing especially the contribution from the land transport sector. Our analysis focuses on large ozone events during summer in four different regions, two major polluted regions (Po Valley and Benelux) and two more remote regions (Iberian Peninsula and Ireland). The analysis concentrates on results for summer 2017, during which measurement campaign EMeRGe took place. Measurement data from this campaign are used for model evaluation. Our analysis shows that European land transport emissions contribute largely (42 % and 44 %, respectively) to ground-level NOy mixing ratios over Benelux and the Po Valley. Due to the overall lower ozone production efficiency over Benelux compared to the Po Valley, however, the contributions to ground-level ozone are larger in the Po Valley (12 %) compared to Benelux (8 %). In line with previous publications using different source apportionment methods, our results underline the large importance of long-range transport of ozone, especially from North America (Benelux, Ireland), but also from Africa (Iberian Peninsula), and provide additional information about the sectoral contribution not available before. Our analysis shows that the contributions of European emissions from land transport and anthropogenic non-traffic sectors strongly increase with increasing values of MDA8 (daily maximum 8 h average) ozone over the Po Valley and in the Benelux region. Accordingly, these two sectors drive large MDA8 values in these regions. Inter-comparisons of results for 2018 and with a coarser model resolution (50 instead of 12 km) show that these results are robust with respect to inter-annual variability and model resolution. Comparing our results with results from other source attribution methods we find that the contributions to ozone from individual sectors, which have large NOx but rather low VOC emissions, are estimated to be lower, if their emissions of NOx and VOCs are regarded concurrently.

We report on an inconsistency in the latitudinal distribution of aviation emissions between the data products of phases 5 and 6 of the Coupled Model Intercomparison Project (CMIP). Emissions in the CMIP6 data occur at higher latitudes than in the CMIP5 data for all scenarios, years, and emitted species. A comparative simulation with the chemistry-climate model ECHAM/MESSy Atmospheric Chemistry (EMAC) reveals that the difference in nitrogen oxide emission distribution leads to reduced overall ozone changes due to aviation in the CMIP6 scenarios because in those scenarios the distribution of emissions is partly shifted towards the chemically less active higher latitudes. The radiative forcing associated with aviation ozone is 7.6% higher, and the decrease in methane lifetime is 5.7% larger for the year 2015 when using the CMIP5 latitudinal distribution of emissions compared to when using the CMIP6 distribution. We do not find a statistically significant difference in the radiative forcing associated with aviation aerosol emissions. In total, future studies investigating the effects of aviation emissions on ozone and climate should consider the inconsistency reported here.

Aviation’s contribution to anthropogenic global warming is estimated to be between 3 – 5% [1]. This assessment comprises two contributions: the well understood atmospheric impact of carbon dioxide (CO2) and the more uncertain non-CO2 effects. The latter pertain to persistent contrails and pollutants like nitrogen oxides (NOx), water vapor (H2O), sulfur oxides (SOx) and soot particles. NOx emissions are involved in non-linear processes that result in the short-term production of ozone (O3) and longer-term destruction of methane (CH4), stratospheric water vapor (SWV), and primary mode ozone (PMO). The aviation-attributable impacts arising from this short-term increase in O3 can vary by more than a factor of 1.5 depending on the selected modelling approach. This O3 increase is associated with the second largest warming effect across aviation’s main climate forcers [1]. We therefore quantify this figure using three modelling approaches (an Eulerian and a Lagrangian tagging scheme as well as a perturbation approach) at three potential aircraft cruise altitudes (200, 250 and 300 hPa) at which NOx pulse emissions are introduced in the Americas, Africa, Eurasia and Australasia. In general, the tagging method computes the contribution by an emission source to the concentration of a chemical species while a perturbation approach consists in calculating the total impact of an emission to the concentration of a species by means of subtracting two simulations: one with all emissions and a second without the specific source’s emissions. We compare results from Eulerian and Lagrangian simulations using the same climate-chemistry code: the ECHAM5/MESSy Atmospheric Chemistry (EMAC) model. With the Eulerian setup, we are able to capture non-linear processes and feedback effects, but not track the transport of emitted species in detail. The Lagrangian setup [2], on the other hand, allows for the accompaniment of thousands of air parcel trajectories, but at the cost of assuming a simplified linear chemistry mechanism. We find that the Lagrangian tagging approach provides the largest estimates for O3 production and radiative forcing (RF), followed by the Eulerian tagging scheme and lastly by the perturbation method. We therefore investigate the appropriateness of each of these in quantifying aviation’s total and marginal climate effects by addressing the following research questions: 1) By how much are the estimates for the short-term NOx-induced O3 perturbation and consequent RF varying across the three modelling approaches and why? 2) How does this RF vary with emission altitude within the upper Troposphere/lower Stratosphere (UTLS)?

[1] Lee, D.S., Fahey, D.W., Skowron, A., Allen, M.R., Burkhardt, U., Chen, Q., Doherty, S.J., Freeman, S., Forster, P.M., Fuglestvedt, J., Gettelman, A., De León, R.R., Lim, L.L., Lund, M.T., Millar, R.J., Owen, B., Penner, J.E., Pitari, G., Prather, M.J., Sausen, R., and Wilcox, L.J.: The contribution of global aviation to anthropogenic climate forcing for 2000 to 2018, Atmos. Environ., 244, 117834, https://doi.org/10.1016/j.atmosenv.2020.117834, 2021.

[2] Maruhashi, J., Grewe, V., Frömming, C., Jöckel, P., and Dedoussi, I. C.: Transport patterns of global aviation NOx and their short-term O3 radiative forcing – a machine learning approach, Atmos. Chem. Phys., 22, 14253–14282, https://doi.org/10.5194/acp-22-14253-2022, 2022.

Aside from the climate impacts from carbon dioxide (CO2) emissions, civil aircraft currently in operation also emit nitrogen oxides (NOx), water vapor (H2O) and other non-CO2 pollutants whose combined primary and secondary effects account for almost 70% of aviation's net contribution towards anthropogenic global warming. NOx emissions, in the short-run, actuate the second largest aviation warming effect via indirect ozone (O3) formation [1], and, unlike CO2, the altitude, geographic location and time of emission are all significant drivers of their resulting climate impact. Past studies [2] have shown a positive correlation between emission altitude and warming from NOx emitted within the troposphere, but such analyses are frequently limited by emission inventories that largely focus on flights across the North Atlantic Flight Corridor (NAFC), thereby disregarding future shifts and alternate patterns in civil aviation traffic. We bridge this gap via global, Lagrangian and Eulerian simulations using the EMAC model wherein equal amounts of NO are released across five regions during two seasons, as was done in [3], but now for two additional flight levels that together cover typical subsonic cruise ranges of 10–12 km. The NOx-induced O3 production was calculated using two modelling methods, tagging and perturbation, as both are vastly used for climate effects estimations. The former is used to compute the contribution of a source to a whole while the latter is useful, for instance, in quantifying the total impact from variations in the strength of a source. We therefore characterize the relation between emission altitude and warming from short-term O3 on a global scale. These results and analyses then form an integral part of the development of next-generation surrogate models that will make climate-optimal routing a reality [4].

References
[1] Lee, D. S., Fahey, D. W., Skowron, A., Allen, M. R., Burkhardt, U., Chen, Q., Doherty, S. J., Freeman, S., Forster, P. M., Fuglestvedt, J., Gettelman, A., De León, R. R., Lim, L. L., Lund, M. T., Millar, R. J., Owen, B., Penner, J. E., Pitari, G., Prather, M. J., Sausen, R., and Wilcox, L. J.: The contribution of global aviation to anthropogenic climate forcing for 2000 to 2018, Atmos. Environ., 244, 117834, https://doi.org/10.1016/j.atmosenv.2020.117834, 2021.
[2] Matthes, S., Lim, L., Burkhardt, U., Dahlmann, K., Dietmüller, S., Grewe, V., Haslerud, A. S., Hendricks, J., Owen, B., Pitari, G., Righi, M., and Skowron, A.: Mitigation of Non-CO2 Aviation's Climate Impact by Changing Cruise Altitudes, Aerospace, 8, 36, https://doi.org/10.3390/aerospace8020036, 2021.
[3] Maruhashi, J., Grewe, V., Frömming, C., Jöckel, P., and Dedoussi, I. C.: Transport patterns of global aviation NOx and their short-term O3 radiative forcing – a machine learning approach, Atmos. Chem. Phys., 22, 14253–14282, https://doi.org/10.5194/acp-22-14253-2022, 2022.
[4] Rao, P., Dwight, R., Singh, D., Maruhashi, J., Dedoussi, I., Grewe, V., and Frömming, C.: Towards a new surrogate model for predicting short-term NOx-O3 effects from aviation using Gaussian processes, EGU General Assembly 2023, Vienna, Austria, 24–28 Apr 2023, EGU23-4337, https://doi.org/10.5194/egusphere-egu23-4337, 2023.

Acknowledgements
This research is part of the ACACIA (Advancing the Science for Aviation and Climate; http://www.acacia-project.eu) project, which is funded by the European Commission, Horizon 2020 Framework program under the grant agreement no. 875036.
This study used the Dutch national e-infrastructure with the support of the SURF Cooperative (grant nos. EINF-441 and EINF-2734).

During spring 2020, the COVID-19 pandemic caused massive reductions in emissions from industry and ground and airborne transportation. To explore the resulting atmospheric composition changes, we conducted the BLUESKY campaign with two research aircraft and measured trace gases, aerosols, and cloud properties from the boundary layer to the lower stratosphere. From 16 May to 9 June 2020, we performed 20 flights in the early COVID-19 lockdown phase over Europe and the Atlantic Ocean. We found up to 50% reductions in boundary layer nitrogen dioxide concentrations in urban areas from GOME-2B satellite data, along with carbon monoxide reductions in the pollution hot spots. We measured 20%-70% reductions in total reactive nitrogen, carbon monoxide, and fine mode aerosol concentration in profiles over German cities compared to a 10-yr dataset from passenger aircraft. The total aerosol mass was significantly reduced below 5 km altitude, and the organic aerosol fraction also aloft, indicative of decreased organic precursor gas emissions. The reduced aerosol optical thickness caused a perceptible shift in sky color toward the blue part of the spectrum (hence BLUESKY) and increased shortwave radiation at the surface. We find that the 80% decline in air traffic led to substantial reductions in nitrogen oxides at cruise altitudes, in contrail cover, and in resulting radiative forcing. The light extinction and depolarization by cirrus were also reduced in regions with substantially decreased air traffic. General circulation-chemistry model simulations indicate good agreement with the measurements when applying a reduced emission scenario. The comprehensive BLUESKY dataset documents the major impact of anthropogenic emissions on the atmospheric composition.

Aviation contributes to 3.5% of anthropogenic climate change in terms of Effective Radiative Forcing (ERF) and 5% in terms of temperature change. Aviation climate impact is expected to increase rapidly due to the growth of air transport sector in most regions of the world and the effects of the COVID-19 pandemic are expected to only have a temporary effect on this growth. While efforts have been made to curb CO2 emissions, non-CO2 effects that are at least equally significant according to recent research, require more attention. The EU Horizon 2020 project ClimOp considers a comprehensive approach to tackling the climate impact of aviation using novel operational measures. One such measure is climate-optimised flight planning, where small deviations can be made in aircraft trajectories to minimise their overall climate impact. Algorithmic Climate Change Functions (aCCFs) are used to estimate the climate impact of local non-CO2 effects such as nitrogen oxide (NOx) emissions (via ozone (O3) formation and methane (CH4) depletion), aviation water vapour (H2O) and contrails using weather variables directly as inputs. By using these functions in an air traffic optimisation module, climate sensitive regions are detected and avoided leading to climate-optimised trajectories. Here, we focus specifically on evaluating the effectiveness of reducing the aviation NOx induced climate impact via O3 formation, using only O3 aCCFs for the optimisation strategy. This is achieved using the chemistry climate model EMAC (ECHAM5/MESSy) and various submodels. A summer and winter day, characterised by high spatial variability of O3 aCCFs are selected, following which, air traffic over the European airspace is optimised with respect to climate as well as operating cost. The air traffic is laterally and vertically optimised separately to enable an evaluation of the horizontal and vertical pattern of O3 aCCFs. It is shown that despite the significant impact of the synoptic situation on the transport of emitted NOx, the climate-optimised flights lead to lower O3 Radiative Forcing (RF) compared to the cost-optimised flights. The study finds that while O3 aCCFs can reduce the climate impact, there are certain discrepancies in the prediction of O3 impact from aviation NOx emissions, as seen for the selected summer day. Although the aCCFs concept is a rough simplification in predicting future pathways of emissions and subsequent climate impact, we could show that it enables a reasonable first estimate. Further research is required to better describe the aCCFs allowing an improved estimate in O3-RF reduction for optimisation approaches.

One possibility to reduce the climate impact of aviation is the avoidance of climate-sensitive regions, which is synonymous with climate-optimised flight planning. Those regions can be identified by algorithmic Climate Change Functions (aCCFs) for nitrogen oxides (NOx), water vapour (H2O) as well as contrail cirrus, which provide a measure of climate effects associated with corresponding emissions. In this study, we evaluate the effectiveness of reducing the aviation-induced climate impact via ozone (O3) formation (resulting from NOx emissions), when solely using O3 aCCFs for the aircraft trajectory optimisation strategy. The effectiveness of such a strategy and the associated potential mitigation of climate effects is explored by using the chemistry–climate model EMAC (ECHAM5/MESSy) with various submodels. A summer and winter day, characterised by a large spatial variability of the O3 aCCFs, are selected. A one-day air traffic simulation is performed in the European airspace on those selected days to obtain both cost-optimised and climate-optimised aircraft trajectories, which more specifically minimised a NOx-induced climate effect of O3 (O3 aCCFs). The air traffic is laterally and vertically re-routed separately to enable an evaluation of the influences of the horizontal and vertical pattern of O3 aCCFs. The resulting aviation NOx emissions are then released in an atmospheric chemistry–climate simulation to simulate the contribution of these NOx emissions to atmospheric O3 and the resulting O3 change. Within this study, we use O3-RF as a proxy for climate impact. The results confirm that the climate-optimised flights lead to lower O3-RF compared to the cost-optimised flights, although the aCCFs cannot reproduce all aspects of the significant impact of the synoptic situation on the transport of emitted NOx. Overall, the climate impact is higher for the selected summer day than for the selected winter day. Lateral re-routing shows a greater potential to reduce climate impact compared to vertical re-routing for the chosen flight altitude. We find that while applying the O3 aCCFs in trajectory optimisation can reduce the climate impact, there are certain discrepancies in the prediction of O3 impact from aviation NOx emissions, as seen for the summer day. Although the O3 aCCFs concept is a rough simplification in estimating the climate impact of a local NOx emission, it enables a reasonable first estimate. Further research is required to better describe the O3 aCCFs allowing an improved estimate in the Average Temperature Response (ATR) of O3 from aviation NOx emissions. A general improvement in the scientific understanding of non-CO2 aviation effects could make climate-optimised flight planning practically feasible

The recent COVID-19 pandemic with its countermeasures, e.g. lock-downs, resulted in decreases in emissions of various trace gases. Here we investigate the changes of ozone over Europe associated with these emission reductions using a coupled global/regional chemistry climate model. We conducted and analysed a business as usual and a sensitivity (COVID19) simulation. A source apportionment (tagging) technique allows us to make a sector-wise attribution of these changes, e.g. to natural and anthropogenic sectors such as land transport. Our simulation results show a decrease of ozone of 8% over Europe in May 2020 due to the emission reductions. The simulated reductions are in line with observed changes in ground-level ozone. The source apportionment results show that this decrease is mainly due to the decreased ozone precursors from anthropogenic origin. Further, our results show that the ozone reduction is much smaller than the reduction of the total NO x emissions (around 20%), mainly caused by an increased ozone production efficiency. This means that more ozone is produced for each emitted NO x molecule. Hence, more ozone is formed from natural emissions and the ozone productivities of the remaining anthropogenic emissions increase. Our results show that politically induced emissions reductions cannot be transferred directly to ozone reductions, which needs to be considered when designing mitigation strategies.

Land transport is an important emission source of nitrogen oxides, carbon monoxide, and volatile organic compounds. The emissions of nitrogen oxides affect air quality directly. Further, all of these emissions serve as a precursor for the formation of tropospheric ozone, thus leading to an indirect influence on air quality. In addition, ozone is radiatively active and its increase leads to a positive radiative forcing. Due to the strong non-linearity of the ozone chemistry, the contribution of emission sources to ozone cannot be calculated or measured directly. Instead, atmospheric chemistry models equipped with specific source attribution methods (e.g. tagging methods) are required. In this study we investigate the contribution of land transport emissions to ozone and ozone precursors using the MECO(n) model system (MESSy-fied ECHAM and COSMO models nested n times). This model system couples a global and a regional chemistry climate model and is equipped with a tagging diagnostic. We investigate the combined effect of long-range-transported ozone and ozone which is produced by European emissions by applying the tagging diagnostic simultaneously and consistently on the global and regional scale. We performed two simulations each covering 3 years with different anthropogenic emission inventories for Europe. We applied two regional refinements, i.e. one refinement covering Europe (50&thinsp;<span classCombining double low line"inline-formula">km</span> resolution) and one covering Germany (12&thinsp;<span classCombining double low line"inline-formula">km</span> resolution). The diagnosed absolute contributions of land transport emissions to reactive nitrogen (<span classCombining double low line"inline-formula">NOy</span>) near ground level are in the range of 5 to 10&thinsp;<span classCombining double low line"inline-formula">nmol mol-1</span>. This corresponds to relative contributions of 50&thinsp;% to 70&thinsp;%. The largest absolute contributions appear around Paris, southern England, Moscow, the Po Valley, and western Germany. The absolute contributions to carbon monoxide range from 30&thinsp;<span classCombining double low line"inline-formula">nmol mol-1</span> to more than 75&thinsp;<span classCombining double low line"inline-formula">nmol mol-1</span> near emission hot-spots such as Paris or Moscow. The ozone which is attributed to land transport emissions shows a strong seasonal cycle with absolute contributions of 3&thinsp;<span classCombining double low line"inline-formula">nmol mol-1</span> during winter and 5 to 10&thinsp;<span classCombining double low line"inline-formula">nmol mol-1</span> during summer. This corresponds to relative contributions of 8&thinsp;% to 10&thinsp;% during winter and up to 16&thinsp;% during summer. The largest values during summer are confined to the Po Valley, while the contributions in western Europe range from 12&thinsp;% to 14&thinsp;%. Only during summer are the ozone contributions slightly influenced by the anthropogenic emission inventory, but these differences are smaller than the range of the seasonal cycle of the contribution to land transport emissions. This cycle is caused by a complex interplay of seasonal cycles of other emissions (e.g. biogenic) and seasonal variations of the ozone regimes. In addition, our results suggest that during events with large ozone values the ozone contributions of land transport and biogenic emissions increase strongly. Here, the contribution of land transport emissions peaks up to 28&thinsp;%. Hence, our model results suggest that land transport emissions are an important contributor during periods with large ozone values.

Anthropogenic and natural emissions influence the tropospheric ozone budget, thereby affecting air quality and climate. To study the influence of different emission sources on the ozone budget, often source apportionment studies with a tagged tracer approach are performed. Studies investigating air quality issues usually rely on regional models with a fine spatial resolution, while studies focusing on climaterelated questions often use coarsely resolved global models. It is well known that simulated ozone mixing ratios depend on the resolution of the model and the resolution of the emission inventory. Whether the contributions simulated using source apportionment approaches also depend on the model resolution, however, is still unclear. Therefore, this study attempts for the first time to analyse the impact of the model, the model resolution, and the emission inventory resolution on simulated ozone contributions using a diagnostic tagging method. The differences in the ozone contributions caused by these factors are compared with differences that arise from the usage of different emission inventories. To do so, we apply the MECO(n) (MESSy-fied ECHAM and COSMO models nested n times) model system which couples online a global chemistry-climate model with a regional chemistry-climate model equipped with a tagging scheme for source apportionment. The results of the global model (at 300 km horizontal resolution) are compared with the results of the regional model at 50 km (Europe) and 12 km (Germany) resolutions. Besides model-specific differences and biases that are discussed in detail, our results have important implications for other modelling studies and modellers applying source apportionment methods. First, contributions from anthropogenic emissions averaged over the continental scale are quite robust with respect to the model, model resolution, and emission inventory resolution. Second, differences on the regional scale caused by different models and model resolutions can be quite large, and regional models are indispensable for source apportionment studies on the subcontinental scale. Third, contributions from stratospheric ozone transported to the surface differ strongly between the models, mainly caused by differences in the efficiency of the vertical mixing. As stratospheric ozone plays an important role for ground level ozone, but the models show large differences in the amount of downward transported ozone, source apportionment methods should account for this source explicitly to better understand inter-model differences.

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.

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.