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.@en

The resilient growth of air travel demands a comprehensive understanding of the climate effects from aviation emissions. The current level of knowledge of the environmental repercussions of CO2 emissions is considerably higher than that of non-CO2 emissions, which includes nitrogen oxides (NOx), sulfur oxides (SOx), other aerosols like black carbon (BC), water vapor and contrails. Aircraft NOx emissions not only possess a high degree of uncertainty because of the non-linearity of the NOx – O3 chemistry, but are also responsible for producing the second strongest net warming effect out of all non-CO2 climate forcers from aviation, right after contrails [1]. This study employs global-scale simulations to characterize the transport patterns of nitrogen oxides and assess their climate effects across several regions (North America, South America, Africa, Eurasia and Australasia) from January to March and July to September in 2014. Radiative forcing effects from the short-term increase in O3, which are triggered by NOx emissions, are estimated. These emissions, which are introduced at a typical cruising altitude, are modelled as Lagrangian air parcels that are transported within the ECHAM5/MESSy Atmospheric Chemistry (EMAC) model [2]. In order to summarize the dynamical and radiative forcing characteristics of more than 10,000 simulated trajectories, a clustering approach with an adapted distance metric is applied. The method itself is an unsupervised machine learning algorithm, called QuickBundles [3], that is most commonly used in the field of neuroscience. A strong seasonal dependence is found for the contribution of NOx emissions to O3. In terms of residence times, NOx emitted in Northern regions resides mainly in the upper mid-latitudes while those initiated in the South remain mostly in the Tropics. Due to pronounced zonal jets, the location of emission does not necessarily correspond to the region that will be most affected, i.e., an emission starting in N. America in July will induce the greatest warming in Europe. [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., Wilcox, L.J.: The contribution of global aviation to anthropogenic climate forcing for 2000 to 2018, Atmospheric Environment, Volume 244, 2021, 117834, ISSN 1352-2310, https://doi.org/10.1016/j.atmosenv.2020.117834. [2] Jöckel, P., Kerkweg, A., Pozzer, A., Sander, R., Tost, H., Riede, H., Baumgaertner, A., Gromov, S., Kern, B., Development cycle 2 of the Modular Earth Submodel System (MESSy2), Geoscientific Model Development, 3, 717-752, doi: 10.5194/gmd-3-717-2010, 2010. [3] Garyfallidis, E., Brett, M., Correia, M. M., Williams, G. B., Nimmo-Smith, I. QuickBundles, a Method for Tractography Simplification. Frontiers in neuroscience, 6, 175. https://doi.org/10.3389/fnins.2012.00175, 2012.@en

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.@en

A hard landing incident in Pico Aerodrome (LPPI) involving an Airbus A320-200 aircraft is investigated using airborne observations and forecasts of the AROME (Applications of Research to Operations at Mesoscale) model. A second flight is also analyzed. The severity of the wind shear during both flights is quantified using the intensity factor “I” that is based on aerial data and recommended by ICAO (International Civil Aviation Organization). During Flight 1, 36% of the landing phase (below 2100 ft) occurred under “severe” wind shear conditions and 16% occurred under “strong” conditions. Upstream characteristics included southwest winds, stable stratification and a Froude number close to 1. According to the AROME model, these circumstances triggered the development of vertically propagating mountain waves, with maximum vertical velocities above 400 ft/min and exceeding 200 ft/min in the flight path. These conditions, together with the severe wind shear, may have caused the incident. During the second flight, a wake with lee vortices and reversed flow developed in the region of the flight path, which is consistent with a low upstream Froude number and/or with the flow regime diagram of previous studies. During the approach phase of this flight, “severe” wind shear conditions were absent, with “strong” ones occurring 4% of the time. It predominantly displayed “light” conditions during 68% of this phase. As a result of the comparison between “I” and the AROME turbulence indicators, preliminary thresholds are proposed for these indexes. Lastly, this study provides an objective verification of AROME wind forecasts, showing a good agreement with airborne observations for wind speeds above 10 kt, but a poor skill for weaker winds.@en

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).@en

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).@en

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.@en

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.@en