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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. [ABSTRACT FROM AUTHOR]

Civil supersonic aviation may return in the near future. Their emissions have been found to lead to changes in the composition of the stratosphere, affecting the ozone layer and climate. To keep up with the rapid developments in supersonic aircraft technology and alternative fuels there is an increasing need for the development of surrogate modeling methods, which requires knowledge of the sensitivities to these emissions. We present a parametric study which evaluates the first‐ and second‐order sensitivities of the ozone column and radiative forcing (RF) to supersonic emissions across two flight corridors and three altitudes. For a given increase in global fuel burn, we find that the increase in emission of NOx ${\text{NO}}_{x}$ is the main driver of both the changes in the global ozone column and RF, the latter of which is linked through changes in the ozone distribution. Followed by the increase in the emission of SOx ${\text{SO}}_{x}$, which leads to O3 ${\mathrm{O}}_{3}$ loss and has a cooling effect. The ozone column and climate are least sensitive to increases in H2O ${\mathrm{H}}_{2}\mathrm{O}$ emissions. We also show that interactions between NOx ${\text{NO}}_{x}$, SOx ${\text{SO}}_{x}$, and H2O ${\mathrm{H}}_{2}\mathrm{O}$ emissions lead to non‐linear behavior in the atmospheric response. The effect of these interactions can lead to < ${< } $5% differences in the ozone column impacts and up to 7.3% increases in RF. Our results demonstrate that the majority of second‐order sensitivities may be neglected in surrogate models for small errors, which could greatly simplify their development. Our results also indicate that reductions in flight altitude and fleetwide NOx ${\text{NO}}_{x}$ emissions may effectively reduce the environmental footprint of supersonic aviation emissions. Plain Language Summary: Supersonic civil aircraft may return in the next decade, and their emissions may cause long‐term changes to the climate and the ozone layer. To keep up with this rapidly developing sector we need fast surrogate models, which can be incorporated in design optimisation processes. In this work we evaluate how the ozone layer and climate respond to 26 different emission scenarios, to determine the sensitivity to common emission species and the location of emissions. We show that, for an increase in fuel burn, the ozone column and climate are most sensitive to the associated NOx ${\text{NO}}_{x}$ emissions, followed by SOx ${\text{SO}}_{x}$ and H2O ${\mathrm{H}}_{2}\mathrm{O}$. We also show that when two emissions are increased simultaneously, interactions between them lead to a different response than if they were considered individually. These interactions change the ozone response by up to 5%, and the climate response by up to 7.3%. Often their effect is smaller, which implies that we could neglect them to simplify model development. Key Points: NOx emissions are the main driver of global ozone loss and the climate impact of supersonic emissionsSupersonic emissions above the Arabian sea have almost twice the ozone and radiative forcing (RF) impact of equivalent over the AtlanticSecond‐order interactions between NOx, SOx, and H2O emissions affect ozone depletion and RF, albeit at a small scale [ABSTRACT FROM AUTHOR]

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 mWm-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 mWm-2 (+78 %) and 50 mWm-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. [ABSTRACT FROM AUTHOR]

The optimization of aircraft trajectories involves balancing operating costs and climate impact, which are often conflicting objectives. To achieve compromised optimal solutions, higher-level information such as preferences of decision-makers must be taken into account. This paper introduces the SolFinder 1.0 module, a decision-making tool designed to identify eco-efficient aircraft trajectories, which allow for the reduction of the flight's climate impact with limited cost penalties compared to cost-optimal solutions. SolFinder 1.0 offers flexible decision-making options that allow users to select trade-offs between different objective functions, including fuel use, flight time, NOx emissions, contrail distance, and climate impact. The module is included in the AirTraf 3.0 submodel, which optimizes trajectories under atmospheric conditions simulated by the ECHAM/MESSy Atmospheric Chemistry model. This paper focuses on the ability of the module to identify eco-efficient trajectories while solving a bi-objective optimization problem that minimizes climate impact and operating costs. SolFinder 1.0 enables users to explore trajectory properties at varying locations of the Pareto fronts without prior knowledge of the problem results and to identify solutions that limit the cost of reducing the climate impact of a single flight. [ABSTRACT FROM AUTHOR]

Hydrogen-powered hypersonic aircraft are designed to travel in the middle stratosphere at approximately 30–40 km. These aircraft can have a considerable impact on climate-relevant species like stratospheric water vapor, ozone, and methane and thus would contribute to climate warming. The impact of hypersonic aircraft emissions on atmospheric composition and, in turn, on radiation fluxes differs strongly depending on cruise altitude. However, in contrast to variations in the altitude of emission, differences from variations in the latitude of emission are currently unknown. Using an atmospheric chemistry general circulation model, we show that a variation in the latitude of emission can have a larger effect on perturbations and stratospheric-adjusted radiative forcing than a variation in the altitude of emission. Our results include the individual impacts of water vapor and nitrogen oxide emissions, as well as unburned hydrogen, on middle-atmospheric water vapor, ozone, and methane and the resulting radiative forcing. Water vapor perturbation lifetime continues the known tropospheric increase with altitude and reaches almost 6 years in the middle stratosphere. Our results demonstrate how atmospheric composition changes caused by emissions of hypersonic aircraft are controlled by large-scale processes like the Brewer–Dobson circulation and, depending on the latitude of emission, local phenomena like polar stratospheric clouds. The analysis includes a model evaluation of ozone and water vapor with satellite data and a novel approach to reduce simulated years by one-third. A prospect for future hypersonic research is the analysis of seasonal sensitivities and simulations with emissions from combustion of liquefied natural gas instead of liquid hydrogen. [ABSTRACT FROM AUTHOR]

Aviation aims to reduce its climate effect by exploiting the potential of identifying alternative climate optimized aircraft trajectories. Such climate-optimized trajectories require a dedicated meteorological service in order to inform on those regions of the atmosphere where aviation emissions have a large effect on climate, for example, by contrail formation or nitrogen-oxide (NOx)-induced ozone formation. With the algorithmic Climate Change Functions (aCCFs) prototypes of a mathematical formulation for the temporal and spatial climate effects of aviation emissions in the atmosphere is provided, which relies solely on numerical weather prediction at the time and location of emissions. Based on the recently published consistent set of aCCF-V1.0, we here introduce newly derived calibration factors for the individual non-CO2 effects of aviation (NOx, water vapour, contrail cirrus) and establish version V1.0A of aCCFs (aCCF-V1.0A). ACCF-V1.0A represents an updated formulation of aCCF while exploring the current level of scientific understanding of individual climate effects of aviation emissions by evaluating quantitative estimates of climate effects with the state-of-the-art climate-response model AirClim. Individual scaling factors (i.e. AirClim calibration factors) are provided for the respective non-CO2 effects comprising contrail cirrus, water vapour and NOx-induced climate effects on ozone and methane, resulting uniformly in lower estimates in aCCF-V1.0A for all species compared to the earlier version aCCF-V1.0. [ABSTRACT FROM AUTHOR]

Despite their proven importance for the atmospheric radiative energy budget, the effect of cirrus on climate and the magnitude of their modification by human activity is not well quantified. Besides anthropogenic pollution sources on the ground, aviation has a large local effect on cirrus microphysical and radiative properties via the formation of contrails and their transition to contrail cirrus. To investigate the anthropogenic influence on natural cirrus, we compare the microphysical properties of cirrus measured at mid-latitude (ML) regions (<60 ∘ N) that are often affected by aviation and pollution with cirrus measured in the same season in comparatively pristine high latitudes (HLs; ≥60 ∘ N). The number concentration, effective diameter, and ice water content of the observed cirrus are derived from in situ measurements covering ice crystal sizes between 2 and 6400 µm collected during the CIRRUS-HL campaign (Cirrus in High Latitudes) in June and July 2021. We analyse the dependence of cirrus microphysical properties on altitude and latitude and demonstrate that the median ice number concentration is an order of magnitude larger in the measured mid-latitude cirrus, with 0.0086 cm-3 , compared to the high-latitude cirrus, with 0.001 cm-3. Ice crystals in mid-latitude cirrus are on average smaller than in high-latitude cirrus, with a median effective diameter of 165 µm compared to 210 µm , and the median ice water content in mid-latitude cirrus is higher (0.0033 gm-3) than in high-latitude cirrus (0.0019 gm-3). In order to investigate the cirrus properties in relation to the region of formation, we combine the airborne observations with 10 d backward trajectories to identify the location of cirrus formation and the cirrus type, i.e. in situ or liquid origin cirrus, depending on whether there is only ice or also liquid water present in the cirrus history, respectively. The cirrus formed and measured at mid-latitudes (M–M) have a particularly high ice number concentration and low effective diameter. This is very likely a signature of contrails and contrail cirrus, which is often observed in the in situ origin cirrus type. In contrast, the largest effective diameter and lowest number concentration were found in the cirrus formed and measured at high latitudes (H–H) along with the highest relative humidity over ice (RHi). On average, in-cloud RHi was above saturation in all cirrus. While most of the H–H cirrus were of an in situ origin, the cirrus formed at mid-latitudes and measured at high latitudes (M–H) were mainly of liquid origin. A pristine Arctic background atmosphere with relatively low ice nuclei availability and the extended growth of few nucleated ice crystals may explain the observed RHi and size distributions. The M–H cirrus are a mixture of the properties of M–M and H–H cirrus (preserving some of the initial properties acquired at mid-latitudes and transforming under Arctic atmospheric conditions). Our analyses indicate that part of the cirrus found at high latitudes is actually formed at mid-latitudes and therefore affected by mid-latitude air masses, which have a greater anthropogenic influence. [ABSTRACT FROM AUTHOR]