Mounting evidence has highlighted the role of aviation non-CO2 emissions in anthropogenic climate change. Of particular importance is the impact of contrails, to which recent studies attribute over one-third of the total effective radiative forcing from aircraft operations. However, the relative importance of the aircraft-design-dependent and environmental factors that influence the formation of persistent contrails is not yet well understood. In this paper, we use ERA5 data from the 2010s to better understand the interplay between the factors on a climatological timescale. We identify ice supersaturation as the most limiting factor for all aircraft designs considered, underscoring the importance of accurately estimating ice supersaturated regions. We also develop climatological relationships that describe potential persistent contrail formation as a function of the pressure level and Schmidt-Appleman mixing line slope. We find that the influence of aircraft design on persistent contrail formation reduces with increasing altitude. Compared to a state-of-the-art conventional aircraft with an overall propulsion system efficiency of 0.37, water vapour extraction technologies envisioned for the future have the potential to reduce persistent contrail formation by up to 85.1 %. On the other hand, compared to the same reference, hydrogen combustion and fuel cell aircraft could increase globally averaged persistent contrail formation by 46.5 % and 54.7 % respectively. Due to differing contrail properties, further work is required to translate these changes into climate impacts. This study is a step towards the development of a new and computationally inexpensive method to analyse the contrail climate impact of novel aviation fuels and propulsion technologies.

While carbon dioxide emissions from aviation often dominate climate change discussions, non-CO₂ effects such as contrails and contrail cirrus must also be considered. Despite varying estimates of their radiative forcing, avoiding contrails is a reasonable strategy for reducing aviation’s climate effects. This study examines temperature and humidity, key atmospheric parameters for contrail formation, across different ECHAM/MESSy (European Centre Hamburg General Circulation Model/Modular Earth Submodel System) Atmospheric Chemistry (EMAC) model setups. EMAC, a general circulation model, is evaluated with various vertical resolutions and two nudging methods across seven specified dynamics setups. A higher vertical resolution aims to capture steep water vapour gradients near the tropopause, crucial for accurate contrail prediction. Comparisons with reanalysis data (March–April 2014) indicate a systematic cold bias (approximately 3–5 K in mid-latitudes), particularly in setups without mean temperature nudging. In the upper troposphere and lower stratosphere, all simulations exhibit a wet bias, while lower altitudes display a dry bias, both affecting contrail formation estimates. Point-by-point comparisons along aircraft trajectories confirm similar biases. Sensitivity experiments with varying thresholds of relative humidity over ice illustrate trade-offs between achieving high hit rates and minimising false alarms in contrail detection. A single-day case study integrating aircraft and satellite observations demonstrates that EMAC’s predicted contrail coverage aligns well with the observed formation. These results suggest that, despite existing temperature and humidity biases, EMAC generally captures regions favourable for contrail formation across diverse atmospheric conditions. Addressing model biases by refining temperature and humidity representation could significantly improve contrail prediction accuracy, strengthening contrail-avoidance strategies and supporting climate-optimised flight routing to mitigate aviation’s overall climate effect.

Commercial supersonic aircraft may return in the near future, offering reduced travel time while flying higher in the atmosphere than subsonic aircraft, thus displacing part of the passenger traffic and associated emissions to higher altitudes. For the first time since 2007, we present a comprehensive multi-model assessment of the atmospheric and radiative effect of this displacement. We use four models (EMAC, GEOS-Chem, LMDz–INCA, and MOZART-3) to evaluate three scenarios in which subsonic aviation is partially replaced with supersonic aircraft. Replacing 4 % of subsonic traffic with Mach 2 aircraft that have a NOx emissions index of 13.8 g (NO2) kg−1 leads to ozone column loss of −0.3 % (−0.9 DU; model range from −0.4 % to −0.1 %), and it increases radiative forcing by 19.1 mW m−2 (model range from 16.7 to 28.1). This forcing is driven by water vapor (18.2 mW m−2), ozone (11.4 mW m−2), and aerosol emissions (−10.5 mW m−2). The use of a Mach 2 concept with low-NOx emissions (4.6 g (NO2) kg−1) reduces the effect on forcing and ozone to 13.4 mW m−2 (model range from 2.4 to 23.4) and −0.1 % (−0.3 DU; model range from −0.2 % to +0.0 %), respectively. If a Mach 1.6 aircraft with a lower cruise altitude and NOx emissions of 4.6 g (NO2) kg−1 is used instead, we find a near-net-zero effect on the ozone column and an increase in the radiative forcing of 3.7 mW m−2 (model range from 0.5 to 7.1). The supersonic concepts have up to 185 % greater radiative effect per passenger kilometer from non-CO2 emissions compared to subsonic aviation (excluding contrail impacts).

The aviation industry and policymakers are advocating Sustainable Aviation Fuels (SAF) as one of the main pillars for making the aviation industry sustainable. However, regulatory frameworks like CORSIA and the EU Renewable Energy Directive often exclude the climate impact from in-flight non-CO2 emissions (e.g., NOx, H2O, and soot emissions), which is important in determining the effect of SAF in reducing the climate impact of aviation. To bridge this gap, we evaluate the total global warming effects of SAF from a well-to-wake analysis, which includes the climate effects from CO2 emissions of the well-to-wake combined with the non-CO2 emissions of the pump-to-wake (i.e., inflight). We quantify the climate impact of NOx, H2O and contrails and convert them to a CO2 equivalence (CO2e) factor based on a climate metric, for instance, the Average Temperature Response over a given time horizon (i.e., 20, 50 and 100 years). The resulting well-to-wake CO2e values for SAF vary from about 150 to 250 g/MJ, depending on the specific fuel pathways. Our analysis shows that the maximum reduction in CO2e emissions when using SAF is less than 50% compared to conventional jet fuel, mainly due to the inflight NOx and contrail effects.

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 (Formula presented.) 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 (Formula presented.), which leads to (Formula presented.) loss and has a cooling effect. The ozone column and climate are least sensitive to increases in (Formula presented.) emissions. We also show that interactions between (Formula presented.), (Formula presented.), and (Formula presented.) emissions lead to non-linear behavior in the atmospheric response. The effect of these interactions can lead to (Formula presented.) 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 (Formula presented.) emissions may effectively reduce the environmental footprint of supersonic aviation emissions.

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.

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.

Reliable prediction of aviation’s environmental impact, including the effect of nitrogen oxides on ozone, is vital for effective mitigation against its contribution to global warming. Estimating this climate impact however, in terms of the short-term ozone instantaneous radiative forcing, requires computationally-expensive chemistry-climate model simulations that limit practical applications such as climate-optimised planning. Existing surrogates neglect the large uncertainties in their predictions due to unknown environmental conditions and missing features. Relative to these surrogates, we propose a high-accuracy probabilistic surrogate that not only provides mean predictions but also quantifies heteroscedastic uncertainties in climate impact estimates. Our model is trained on one of the most comprehensive chemistry-climate model datasets for aviation-induced nitrogen oxide impacts on ozone. Leveraging feature selection techniques, we identify essential predictors that are readily available from weather forecasts to facilitate the implementation therein. We show that our surrogate model is more accurate than homoscedastic models and easily outperforms existing linear surrogates. We then predict the climate impact of a frequently-flown flight in the European Union, and discuss limitations of our approach.

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.

A growing body of research has highlighted the major contribution of aviation non-CO2 emissions and effects to anthropogenic climate change. Regulation of these emissions, for example in the EU Emissions Trading System, requires the use of a climate metric. However, choosing a suitable climate metric is challenging due to the high uncertainties of aviation non-CO2 climate impacts, their variability in atmospheric lifetimes and their dependence on emission location and altitude. Here we use AirClim to explore alternatives to the conventional Global Warming Potential (GWP) by analysing the neutrality, temporal stability, compatibility and simplicity of existing climate metrics and perform a trade-off. We find that using the temperature-based Average Temperature Response (ATR) or using an Efficacy-weighted GWP (EGWP) would enable a more accurate assessment of existing as well as future aircraft powered by novel aviation fuels

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.

Aviation aims to reduce its climate effect by adopting trajectories that avoid regions of the atmosphere where aviation emissions have a large impact. To that end, prototype algorithmic climate change functions (aCCFs) can be used, which provide spatially and temporally resolved information on aviation's climate effect in terms of future near-surface temperature change. These aCCFs can be calculated with meteorological input data obtained from, e.g., numerical weather prediction models. We present here the open-source Python library called CLIMaCCF, an easy-to-use and flexible tool which efficiently calculates both the individual aCCFs (i.e., aCCF of water vapor, nitrogen oxide (NOx)-induced ozone production and methane depletion, and contrail cirrus) and the merged non-CO2 aCCFs that combine all these individual contributions. To construct merged aCCFs all individual aCCFs are converted to the same physical unit. This unit conversion needs the technical specification of aircraft and engine parameters, i.e., NOx emission indices and flown distance per kilogram of burned fuel. These aircraft- and engine-specific values are provided within CLIMaCCF version V1.0 for a set of aggregated aircraft and engine classes (i.e., regional, single-aisle, wide-body). Moreover, CLIMaCCF allows the user to choose from a range of physical climate metrics (i.e., average temperature response for pulse or future scenario emissions over the time horizons of 20, 50, or 100 years). Finally, we demonstrate the abilities of CLIMaCCF through a series of example applications.

While efforts have been made to curb CO2 emissions from aviation, the more uncertain non-CO2 effects that contribute about two-thirds to the warming in terms of radiative forcing (RF), still require attention. The most important non-CO2 effects include persistent line-shaped contrails, contrail-induced cirrus clouds and nitrogen oxide (NOx) emissions that alter the ozone (O3) and methane (CH4) concentrations, both of which are greenhouse gases, and the emission of water vapour (H2O). The climate impact of these non-CO2 effects depends on emission location and prevailing weather situation; thus, it can potentially be reduced by advantageous re-routing of flights using Climate Change Functions (CCFs), which are a measure for the climate effect of a locally confined aviation emission. CCFs are calculated using a modelling chain starting from the instantaneous RF (iRF) measured at the tropopause that results from aviation emissions. However, the iRF is a product of computationally intensive chemistry-climate model (EMAC) simulations and is currently restricted to a limited number of days and only to the North Atlantic Flight Corridor. This makes it impossible to run EMAC on an operational basis for global flight planning. A step in this direction lead to a surrogate model called algorithmic Climate Change Functions (aCCFs), derived by regressing CCFs (training data) against 2 or 3 local atmospheric variables at the time of emission (features) with simple regression techniques and are applicable only in parts of the Northern hemisphere. It was found that in the specific case of O3 aCCFs, which provide a reasonable first estimate for the short-term impact of aviation NOx on O3 warming using temperature and geopotential as features, can be vastly improved [1]. There is aleatoric uncertainty in the full-order model (EMAC), stemming from unknown sources (missing features) and randomness in the known features, which can introduce heteroscedasticity in the data. Deterministic surrogates (e.g. aCCFs) only predict point estimates of the conditional average, thereby providing an incomplete picture of the stochastic response. Thus, the goal of this research is to build a new surrogate model for iRF, which is achieved by : 1. Expanding the geographical coverage of iRF (training data) by running EMAC simulations in more regions (North & South America, Eurasia, Africa and Australasia) at multiple cruise flight altitudes, 2. Following an objective approach to selecting atmospheric variables (feature selection) and considering the importance of local as well as non-local effects, 3. Regressing the iRF against selected atmospheric variables using supervised machine learning techniques such as homoscedastic and heteroscedastic Gaussian process regression. We present a new surrogate model that predicts iRF of aviation NOx-O3 effects on a regular basis with confidence levels, which not only improves our scientific understanding of NOx-O3 effects, but also increases the potential of global climate-optimised flight planning.

The climate impact of aviation is considerably different from that of other transport modes. The turbofan engine’s efficiency can be increased by increasing the Operating Pressure Ratio (OPR), bypass ratio (BPR) and Turbine Inlet Temperature (TIT), thereby reducing CO2 and H2O emissions. However, this may have an adverse effect on the secondary emissions, such as NOx, soot, etc. Taking a holistic view in evaluating the climate impact of engine development trends considering all the climate forcers is imperative for design trends in the future. This research investigates the impact of some key engine design parameters on climate. The emission changes due to design variations in the CFM56-5B are estimated using in-house engine performance and emission prediction tools. Accordingly, the changes in the species’ Average Temperature Response for 100 years (ATR100) are analyzed using a climate assessment tool, AirClim. The results show that the overall climate impact increases by 40% when increasing OPR from 25 to 40. Meanwhile, the Twin Annular Premixed Swirler (TAPS-II) combustor reduces the total ATR100 drastically, in the range of 52–58%, due to lean combustion.

The climate impact of non-CO2 emissions, which are responsible for two-thirds of aviation radiative forcing, highly depends on the atmospheric chemistry and weather conditions. Hence, by planning aircraft trajectories to reroute areas where the non-CO2 climate impacts are strongly enhanced, called climate-sensitive regions, there is a potential to reduce aviation-induced non-CO2 climate effects. Weather forecast is inevitably uncertain, which can lead to unreliable determination of climate-sensitive regions and aircraft dynamical behavior and, consequently, inefficient trajectories. In this study, we propose robust climate-optimal aircraft trajectory planning within the currently structured airspace considering uncertainties in standard weather forecasts. The ensemble prediction system is employed to characterize uncertainty in the weather forecast, and climate-sensitive regions are quantified using the prototype algorithmic climate change functions. As the optimization problem is constrained by the structure of airspace, it is associated with hybrid decision spaces. To account for discrete and continuous decision variables in an integrated and more efficient manner, the optimization is conducted on the space of probability distributions defined over flight plans instead of directly searching for the optimal profile. A heuristic algorithm based on the augmented random search is employed and implemented on graphics processing units to solve the proposed stochastic optimization computationally fast. An open-source Python library called ROOST (V1.0) is developed based on the aircraft trajectory optimization technique. The effectiveness of our proposed strategy to plan robust climate-optimal trajectories within the structured airspace is analyzed through two scenarios: a scenario with a large contrail climate impact and a scenario with no formation of persistent contrails. It is shown that, for a nighttime flight from Frankfurt to Kyiv, a 55ĝ€¯% reduction in climate impact can be achieved at the expense of a 4ĝ€¯% increase in the operating cost.

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.

A growing body of research has highlighted the major contribution of aviation non-CO2 emissions to anthropogenic climate change. Regulation of these emissions, for example in the EU Emissions Trading System (ETS), requires the use of a climate metric. However, choosing a suitable climate metric is challenging due to the high uncertainties of aviation non-CO2 climate impacts, their variability in atmospheric lifetimes and their dependence on emission location and altitude. In this study, we explore the neutrality, temporal stability, compatibility and transparency of existing, physical climate metrics and find the Average Temperature Response (ATR) to be most suitable for aviation policy and aircraft design. We show that the similarities of the total CO2-eq emissions calculated by the ATR and the Global Warming Potential (GWP) for current aircraft would enable a timely introduction of the ATR in aviation policy, allowing for a more accurate assessment of novel aviation fuels and aircraft designs.

Aviation produces a net climate warming contribution that comprises multiple forcing terms of mixed sign. Aircraft NOx emissions are associated with both warming and cooling terms, with the short-term increase in O3 induced by NOx emissions being the dominant warming effect. The uncertainty associated with the magnitude of this climate forcer is amongst the highest out of all contributors from aviation and is owed to the nonlinearity of the NOx-O3 chemistry and the large dependency of the response on space and time, i.e., on the meteorological condition and background atmospheric composition. This study addresses how transport patterns of emitted NOx and their climate effects vary with respect to regions (North America, South America, Africa, Eurasia and Australasia) and seasons (January-March and July-September in 2014) by employing global-scale simulations. We quantify the climate effects from NOx emissions released at a representative aircraft cruise altitude of 250 hPa (∼10400 m) in terms of radiative forcing resulting from their induced short-term contributions to O3. The emitted NOx is transported with Lagrangian air parcels within the ECHAM5/MESSy Atmospheric Chemistry (EMAC) model. To identify the main global transport patterns and associated climate impacts of the 14 000 simulated air parcel trajectories, the unsupervised QuickBundles clustering algorithm is adapted and applied. Results reveal a strong seasonal dependence of the contribution of NOx emissions to O3. For most regions, an inverse relationship is found between an air parcel's downward transport and its mean contribution to O3. NOx emitted in the northern regions (North America and Eurasia) experience the longest residence times in the upper midlatitudes (40 %-45 % of their lifetime), while those beginning in the south (South America, Africa and Australasia) remain mostly in the Tropics (45 %-50 % of their lifetime). Due to elevated O3 sensitivities, emissions in Australasia induce the highest overall radiative forcing, attaining values that are larger by factors of 2.7 and 1.2 relative to Eurasia during January and July, respectively. The location of the emissions does not necessarily correspond to the region that will be most affected - for instance, NOx over North America in July will induce the largest radiative forcing in Europe. Overall, this study highlights the spatially and temporally heterogeneous nature of the NOx-O3 chemistry from a global perspective, which needs to be accounted for in efforts to minimize aviation's climate impact, given the sector's resilient growth.

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
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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).