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Aviation NOx emissions have not only an impact on global climate by changing ozone and methane levels but also contribute to deteriorate local air quality. In order to properly assess the co-benefit with air quality improvement and the trade-off with the climate change associated with CO2, it appears essential to better quantify the climate impact of aircraft NOx emissions. A new version of the LMDZ-INCA global model, including both tropospheric and stratospheric chemistry and the sulfate-nitrate-ammonium cycle, is applied to re-evaluate the impact of aircraft NOx and aerosol emissions on climate. The results confirm that the efficiency of NOx to produce ozone is very much dependent on the injection height. For the baseline simulation and reference scenario this efficiency is 6.6 TgO3/TgN. The efficiency increases with the background methane and NOx concentrations and with decreasing aircraft NOx emissions. The same findings translate to the associated ozone radiative forcing which exhibits a fairly constant value per ozone mass change of 3.4 mW/m2/TgO3. The methane lifetime variation is less sensitive to the aircraft NOx emission location than the ozone change. The change in CH4 mixing ratio itself represents 75 % of the total methane forcing. The indirect changes through long-term tropospheric ozone, stratospheric water vapour and methane oxidation to CO2 contribute for 19 %, 4 % and 1 %, respectively. The net NOx radiative forcing (O3 + CH4) is largely affected by the revised CH4 radiative forcing formula which increases the total CH4 negative forcing by 15 %. As a consequence, the ozone positive forcing and the methane negative forcing largely offset each other resulting in a slightly positive forcing for the present-day. However, in the future, the net forcing turns to negative due essentially to higher methane background concentrations. Additional radiative forcings involving particle formation arise from aircraft NOx emissions since the increased OH concentrations are responsible for an enhanced conversion of SO2 to sulfate particles. Aircraft NOx emissions also increase the formation of nitrate particles in the lower troposphere. However, in the upper-troposphere, increased sulfate concentrations favor the titration of ammonia leading to lower ammonium nitrate concentrations. The total forcing from sulfate and nitrate aerosols associated with NOx emissions is negative and is estimated to -3.0 mW/m2/TgN for the present-day. When these aerosol radiative forcings are considered, the total NOx forcing turns from a positive value to a negative value even for present-day conditions. Hence, total radiative forcing from aircraft emissions associated with changes in atmospheric chemistry and direct aerosols forcings is negative for both present-day and future (2050) conditions. NOx emissions only cause a negative forcing representing about 45 % of the total forcing. The negative forcing associated with sulfates largely dominates the effect of the other particles. The sulfate direct radiative forcing is estimated to be associated for about 50 % with the direct SO2 and SO4 aircraft emissions and for about 50 % with the increased conversion of SO2 to SO4 at higher OH concentrations, and hence related to the NOx emissions. The net effect of decreasing (resp. increasing) the flight altitude by 2000 ft (about 610 m) is to increase (resp. decrease) the total negative forcing by 57 % (resp. 65 %). The variation of the total forcing with flight altitude is dominated by the high sensitivity of the ozone positive forcing to the altitude of the perturbation. Several mitigation options involving flight aircraft operation and cruise altitude changes, traffic growth, engine technology, and fuel type, exist to reduce the climate impact of aircraft NOx emissions. However, the climate forcing of aircraft NOx emissions is likely to be small or even switch to negative (cooling) depending on atmospheric NOx or CH4 future background concentrations or when the NOx impact on sulfate and nitrate particles is considered. There remain large uncertainties on the NOx net impact on climate effect calculation. Nevertheless, the results suggest that reducing aircraft NOx emissions is primarily beneficial for improving air quality. For climate consideration, one option to reduce uncertainties in mitigation strategies might be to prioritize the reduction of CO2 aircraft emissions which have a well-established and long-term impact on climate, however this reduces the overall mitigation potential.

Evaluating the global chemistry models in the upper troposphere – lower stratosphere (UTLS) is an important step toward a further understanding of its chemical composition. The latter is regularly sampled through in situ measurements based on passenger aircraft, in the framework of the In-service Aircraft for a Global Observing System (IAGOS) research infrastructure. This study focuses on the comparison of the IAGOS measurements in ozone, carbon monoxide (CO), nitrogen reactive species (NOy) and water vapour, with a 25-year simulation output from the LMDZ-OR-INCA chemistry-climate model. For this purpose, we present and apply an extension of the Interpol-IAGOS software that projects the IAGOS data onto any model grid, in order to derive a gridded IAGOS product and a masked model product that are directly comparable to one another. Climatologies are calculated in the upper troposphere (UT) and in the lower stratosphere (LS) separately, but also in the UTLS as a whole, as a demonstration for the models that do not sort out the physical variables necessary to distinguish between the UT and the LS. In the northern extratropics, the comparison in the UTLS layer suggests that the geographical distribution in the tropopause height is well reproduced by the model. In the separated layers, the model simulates well the water vapour climatologies in the UT, and the ozone climatologies in the LS. The opposite biases in CO in both UT and LS suggest that the cross-tropopause transport is overestimated. The NOy observations highlight the difficulty of the model in parameterizing the lightning emissions. In the tropics, the upper-tropospheric climatologies are remarkably well simulated for water vapour, as the observed CO peaks due to biomass burning in the most convective systems, and the ozone latitudinal variations. Ozone is more sensitive to lightning emissions than to biomass burning emissions, whereas the CO sensitivity to biomass burning emissions strongly depends on the location and on the season. Through this evaluation, the present study demonstrates that the Interpol-IAGOS software is a tool facilitating the assessment of the global model simulations in the UTLS, potentially useful for any modelling experiment involving chemistry-climate and chemistry-transport models.

Aircraft emissions consist of carbon dioxide (CO2), nitrogen oxides (NOx), sulfur dioxide (SO2) and particulate matter (black carbon, sulfate) and water vapour. The non-CO2 effects have been recently evaluated as twice the CO2 effects regarding their radiative forcing of climate in 2018 [1]. Among the non-CO2 effects, nitrogen oxides emissions impact several greenhouse gases concentrations. Increased tropospheric ozone production results in a positive radiative forcing (climate impact), but the subsequent increased OH concentrations enhance methane chemical destruction, thus decreasing stratospheric water vapour and the methane-linked background ozone levels in the troposphere. The net radiative forcing caused by the aircraft NOx emissions is evaluated as a net positive forcing but still shows important uncertainties.In order to investigate representation of key mechanisms involved for climate forcing, in the framework of the ACACIA (Advancing the Science for Aviation and Climate) EU project, six global chemistry-climate models have been used to reevaluate the climate effects of NOx and aerosol aircraft emissions on atmospheric composition following a common protocol. As a first step, the standard runs have been assessed regarding ozone, carbon monoxide (CO), water vapour and reactive nitrogen (NOy) against the IAGOS airborne measurements during 1994-2018, separately in the upper troposphere and in the lower stratosphere.As a second step, the models have been used to assess the impact of NOx and aerosol emissions on atmospheric composition. The subsonic aircraft perturbations are calculated based on the CEDS aircraft emission inventories [2] for the present-day conditions and based on different socioeconomic scenarios [3] for future (2050) conditions. Several sensitivity simulations will be presented in order to investigate the sensitivity of the results to background atmospheric conditions (present, future) and to lightning emissions. The changes in atmospheric composition will be presented and compared for the different models and scenarios. Acknowledgement:This study was supported by the European Union’s Horizon 2020 research and innovation programme under grant agreement No 875036 within the Aeronautics project ACACIA. References:[1] D.S. Lee, D.W. Fahey, A. Skowron, M.R. Allen, U. Burkhardt, Q. Chen, S.J. Doherty, S. Freeman, P.M. Forster, J. Fuglestvedt, A. Gettelman, R.R. De León, L.L. Lim, M. T. Lund, R.J. Millar, B. Owen, J.E. Penner, G. Pitari, M.J. Prather, R. Sausen, and L. J. Wilcox, Atmospheric Environment 244, 117834 (2021)[2] R. M. Hoesly, S. J. Smith, L. Feng, Z. Klimont, G. Janssens-Maenhout, T. Pitkanen, J. J. Seibert, L. Vu, R. J. Andres, R. M. Bolt, T. C. Bond, L. Dawidowski, N. Kholod, J. Kurokawa, M. Li, L. Liu, Z. Lu, M. C. P. Moura, P. R. O’Rourke, and Q. Zhang, Geosci. Model Develop. 11, 369-408 (2018)[3] M. J. Gidden, K. Riahi, S. J. Smith, S. Fujimori, G. Luderer, E. Kriegler, D. P. van Vuuren, M. van den Berg, L. Feng, D. Klein, K. Calvin, J. C. Doelman, S. Frank, O.Fricko, M. Harmsen, T. Hasegawa, P. Havlik, J. Hilaire, R. Hoesly, J. Horing, A. Popp, E. Stehfest, and K. Takahashi, Geosci. Model Develop. 12, 1443-1475 (2019)

A wide variety of observation data sets are used to assess long-term simulations provided by chemistry-climate models (CCMs) and chemistry-transport models (CTMs). However, the upper troposphere – lower stratosphere (UTLS) is hardly assessed in the models because of uncertainties in remote measurements, a limited area for balloon-borne observations and a limited period for aircraft campaigns. Observations performed in the framework of the IAGOS program (In-service Aircraft for a Global Observing System) combine the advantages of in situ measurements in the UTLS with an almost global-scale area, a ~20-year monitoring period and a high sampling frequency. Few model assessments have been made using the IAGOS database, and none of them involved the whole cruise data set.Cohen et al. (2021, GMD) proposed a method to project all the IAGOS data onto a model monthly grid, in order to make them ready for assessing global climatologies and seasonal cycles above several well-sampled regions in the North Hemisphere. This work has been extended to a daily resolution for an accurate separation between the upper troposphere and the lower stratosphere, and to other chemical species. In this study, we apply this method to a set of simulations generated by the following CTMs or CCMs: Oslo-CTM3, MOZART3, EMAC, UKESM, and LMDZ-OR-INCA, all involved into the ACACIA European Union program (Advancing the Science for Aviation and Climate) that focuses on the climate impact of the subsonic aviation emissions. The runs are generated following a common protocol, notably regarding the boundary conditions (e.g. emission inventories) and the chemical configurations, the latter including gaseous tropospheric and stratospheric chemistry, and heterogeneous chemistry. The multi-model assessment concerns the 1994 – 2017 period, and focuses on ozone, carbon monoxide, water vapour and reactive nitrogen (NOy) fields.

A wide variety of observation data sets are used to assess long-term simulations provided by chemistry-climate models (CCMs) and chemistry-transport models (CTMs). However, the upper troposphere – lower stratosphere (UTLS) has hardly been assessed in the models yet. Observations performed in the framework of IAGOS (In-service Aircraft for a Global Observing System) combine the advantages of in situ airborne measurements in the UTLS with an almost global-scale sampling, a ~ 20-year monitoring period and a high frequency. If a few model assessments have been made using IAGOS database, none of them took advantage of the dense and high-resolution cruise data in their whole ensemble yet. The present study proposes a method to compare this large IAGOS data set to long-term simulations used for chemistry-climate studies. For this purpose, a new software (named Interpol-IAGOS) projects all IAGOS data on the 3D grid of the chosen model with a monthly resolution, since generally chemistry-climate models provide 3D outputs as monthly means. This provides a new IAGOS data set (IAGOS-DM) mapped at the model's grid and time resolution. As a first application, the REF-C1SD simulation generated by MOCAGE CTM in the framework of CCMI phase-I has been evaluated during the 1994–2013 period for ozone and the 2002–2013 period for carbon monoxide. This comparison is exclusively based on the grid cells sampled by IAGOS, thus the assessed model output (MOCAGE-M) is obtained by applying a corresponding mask onto the grid. First, climatologies are derived from the IAGOS-DM product. Good correlations are reported between IAGOS-DM and MOCAGE-M spatial distributions. As an attempt to analyse MOCAGE-M behaviour in the upper troposphere (UT) and the lower stratosphere (LS) separately, UT and LS data in IAGOS-DM were sorted according to potential vorticity. From this, we derived O3 and CO seasonal cycles in eight regions well sampled by IAGOS flights in the northern mid-latitudes. They are remarkably well-reproduced by the model for lower-stratospheric O3 and also good for upper-tropospheric CO. The data projection onto the model's grid is a necessary step for a more accurate assessment, as it allows to filter out biases only due to either spatial or temporal resolution. Beyond the MOCAGE REF-C1SD evaluation presented in this paper, the method could be used by CCMI models for individual assessments in the UTLS and for model intercomparisons with respect to IAGOS data set.

International audience; Climatology and long-term evolution of ozone and carbon monoxide in the upper troposphere-lower stratosphere (UTLS) at northern midlatitudes, as seen by IAGOS from Abstract. In situ measurements in the upper troposphere-lower stratosphere (UTLS) have been performed in the framework of the European research infrastructure IAGOS (In-service Aircraft for a Global Observing System) for ozone since 1994 and for carbon monoxide (CO) since 2002. The flight tracks cover a wide range of longitudes in the northern extratropics, extending from the North American western coast (125 • W) to the eastern Asian coast (135 • E) and more recently over the northern Pacific Ocean. Several tropical regions are also sampled frequently, such as the Brazilian coast, central and southern Africa, southeastern Asia, and the western half of the Maritime Continent. As a result, a new set of climatologies for O 3 (in the upper troposphere (UT), tropopause layer, and lower stratosphere (LS) are made available, including gridded horizontal distributions on a semi-global scale and seasonal cycles over eight well-sampled regions of interest in the northern extratropics. The seasonal cycles generally show a summertime maximum in O 3 and a springtime maximum in CO in the UT, in contrast to the systematic springtime maximum in O 3 and the quasi-absence of a seasonal cycle of CO in the LS. This study highlights some regional variabilities in the UT, notably (i) a west-east difference of O 3 in boreal summer with up to 15 ppb more O 3 over central Russia compared with northeast America, (ii) a systematic west-east gradient of CO from 60 to 140 • E, especially noticeable in spring and summer with about 5 ppb by 10 degrees longitude, (iii) a broad spring/summer maximum of CO over northeast Asia, and (iv) a spring maximum of O 3 over western North Amer-ica. Thanks to almost 20 years of O 3 and 12 years of CO measurements, the IAGOS database is a unique data set to derive trends in the UTLS at northern midlatitudes. Trends in O 3 in the UT are positive and statistically significant in most regions, ranging from +0.25 to +0.45 ppb yr −1 , characterized by the significant increase in the lowest values of the distribution. No significant trends of O 3 are detected in the LS. Trends of CO in the UT, tropopause, and LS are almost all negative and statistically significant. The estimated slopes range from −1.37 to −0.59 ppb yr −1 , with a nearly homogeneous decrease in the lowest values of the monthly distribution (5th percentile) contrasting with the high interregional variability in the decrease in the highest values (95th percentile).

The overall objective of the thesis is to characterize the geographical distribution, seasonal cycles and recent trends of ozone and carbon monoxide in the upper troposphere- lower stratosphere (UT-LS) over eight regions of interest, in the northern mid-latitudes. For this purpose, we first analyzed the IAGOS airborne observations. We have shown a positive trend in ozone in the UT over 1994-2013, and a negative trend in carbon monoxide, the latter being linked to the decrease in surface emissions. We then compared the observations to the recent climate chemical composition simulation performed by the MOCAGE model in the CCMI intercomparison exercise. To do this, we have developed a new method to project IAGOS measurements onto the model grid, allowing us to process long observation periods. This method has proven to be relevant for evaluating the simulation and could be extended to other simulations and models.; L'objectif général de la thèse est de caractériser la distribution géographique, les cycles saisonniers et l'évolution récente de l'ozone et du monoxyde de carbone dans la haute troposphère - basse stratosphère (UT - LS) au-dessus de huit régions d'intérêt, aux moyennes latitudes de l'hémisphère Nord. Pour cela, nous avons analysé les observations aéroportées IAGOS. Nous avons montré une tendance positive de l'ozone dans l'UT sur 1994 - 2013, et une tendance négative du monoxyde de carbone liée à la décroissance des émissions en surface. Nous avons comparé les mesures à la simulation de composition chimique sur le climat récent issue du modèle MOCAGE dans l'exercice d'intercomparaison CCMI. Pour ce faire, nous avons développé une nouvelle méthode permettant de projeter les mesures IAGOS sur le maillage du modèle et de traiter ainsi 20 ans d'observations. Cette méthode s'est révélée pertinente pour évaluer la simulation et pourrait être étendue à d'autres simulations et d'autres modèles.

In situ measurements in the upper troposphere – lower stratosphere (UTLS) are performed in the framework of the European research infrastructure IAGOS (In-service Aircraft for a Global Observing System) for ozone since 1994 and for carbon monoxide since 2002. The flight tracks cover a wide range of longitudes in the northern extratropics, extending from the North American western coast (125° W) to the eastern Asian coast (135° E), and more recently over the northern Pacific ocean. Different tropical regions are also sampled frequently, such as the Brazilian coast, central and southern Africa, southeastern Asia and the western Maritime Continent. As a result, a new set of climatologies for O3 (Aug. 1994–Dec. 2013) and CO (Dec. 2001–Dec. 2013) in the upper troposphere (UT), tropopause layer and lower stratosphere (LS) are made available, including quasi-global gridded horizontal distributions, and seasonal cycles over eight well sampled regions of interest in the northern extratropics. The seasonal cycles generally show a summertime maximum in O3 and a springtime maximum in CO in the UT, in contrast with the systematic springtime maximum in O3 and the quasi-absence of seasonal cycle of CO in the LS. This study highlights some regional variabilities in the UT notably (i) a west-east difference of O3 in boreal summer with up to 15 ppb more O3 over central Russia compared with northeast America, (ii) a systematic west-east gradient of CO from 60° E to 140° E (especially noticeable in spring and summer with about 5 ppb by 10 degrees longitude), (iii) a broad spring/summer maximum of CO over North East Asia, and (iv) a spring maximum of O3 over Western North America. Thanks to almost 20 years of O3 and 12 years of CO measurements, the IAGOS database is a unique data set to derive trends in the UTLS. Trends in O3 in the UT are positive and statistically significant in most regions, ranging from +0.25 to +0.45 ppb yr−1, characterized by the significant increase of the lowest values of the distribution. No significant trends of O3 are detected in the LS. Trends of CO in the UT, tropopause and LS are all negative and statistically significant. The estimated slopes range from −1.37 to −0.59 ppb yr−1 , with a nearly homogeneous decrease of the lowest values of the monthly distribution (fifth percentile) contrasting with the high inter-regional variability of the highest values (95th percentile).