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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.

The Arctic winter 2015/2016 was characterized by extremely low temperatures in the stratosphere and by a very strong polar vortex, accompanied by extended fields of Polar Stratospheric Clouds. During this winter, aircraft-based measurements were carried out with the research aircraft HALO (High Altitude and Long-Range Research Aircraft) from Kiruna/Sweden and Oberpfaffenhofen/Germany.Total reactive nitrogen and its distribution between the gas and particle phases are key parameters for understanding processes controlling the ozone budget in the polar winter stratosphere. Tracer-tracer correlations were applied to study the vertical redistribution of gas-phase total reactive nitrogen. The extended observation period from December to March provided the opportunity to study the changing distribution of reactive nitrogen in the lowermost Arctic stratosphere during the course of the winter. In early winter, during December, the lowermost Arctic stratosphere did not show any indications for disturbed conditions.The situation changed during the observational period in January and February. Tracer-tracer correlations showed elevated levels of total reactive nitrogen of up to 6 nmol/mol. These observations could be interpreted by evaporation of polar stratospheric particles falling down from the stratosphere above and leading to a nitrification of the lowermost stratosphere. During some periods up to 60 % of the observed total reactive nitrogen can be attributed to evaporating particles. The observation of gas phase nitrification was accompanied by the occurrence of particulate nitrate in extended regions at altitudes between about 10 and 14 km. Usually, the occurrence of particulate nitrate is rare at such altitudes. The diameter of these particles was estimated to range between about 9 and 18 µm.During the late-winter observation period, no indications for polar stratospheric cloud particles at flight altitude were found. However, extended regions with elevated gas-phase concentrations of total reactive nitrogen were still observed. In late winter, the subsidence of air masses from the polar vortex became increasingly important for the distribution of total reactive nitrogen in the lowermost stratosphere. Air masses with substantial denitrification of up to 5 nmol/mol were observed. In these cases, up to 50 % of the undisturbed total reactive nitrogen was missing. Concurrently lower ozone concentrations were observed, indicating destruction of ozone at higher altitudes.Nitrification and denitrification of the lowermost stratosphere during the course of the winter are linked by heterogeneous processes in the above-lying stratosphere. Simulations with the CLaMS model confirm and complement the findings of the in-situ observations. They also suggest that the observations have been representative of the vortex-wide redistribution of total reactive nitrogen. The aircraft-based in-situ measurements provided a comprehensive picture of the temporal evolution of the distribution of total reactive nitrogen over the entire winter period 2015/2016.

Aviation is concerned by its climate effects which results from CO2 and non-CO2 effects, comprising NOx-induced changes of atmospheric ozone and methane. Here climate-chemistry models are required to advance our understanding on induced changes of reactive species and the associated radiative forcing associated to aviation emissions. Evaluation of such comprehensive models is key in order to be able to investigate associated uncertainties can use observational datasets from research infrastructures like IAGOS and DLR aircraft measurement campaign data.We use the MECO(n) system which is a “MESSy-fied ECHAM and COSMO nested n-times”, relying on the Modular Earth Submodel System (MESSy) framework. For this purpose, both models have been equipped with the MESSy infrastructure, implying that the same process formulations (MESSy submodels) are available for both models. Modelled atmospheric distributions from the multi-scale model system MECO(n) are systematically compared to observational data from aircraft measurements in the upper troposphere and lower stratosphere. Nudging of meteorology to reanalysis data, and special diagnostics available within the modular MESSy infrastructure are implemented in the numerical simulations. Online sampling along aircraft trajectories allows to extract model data with a high temporal resolution (MESSy submodel S4D), in order to evaluate model representation and key processes. Beyond systematic evaluation with IAGOS scheduled aircraft measurements, particular focus on those episodes where dedicated measurements from aircraft campaigns are available. We present an analysis of reactive species, NOy and ozone, which also identifies those weather pattern and synoptic situations where aviation contributes strong signals. We evaluate model representation of the NOx-induces effect on radiatively active species ozone and hydroxyl radical in both model instances, ECHAM5 and COSMO. This is key for advancing the scientific understanding of NOx-induced effects from aviation non-CO2 effects required in order to quantify potential compensation and trade-offs and eventually in order to identify robust mitigation options for sustainable aviation.This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 875036 (ACACIA, Advancing the Science for Aviation and Climate) and has been supported by the DLR-Projekt Eco2Fly. This work uses measurement data from the European Research Infrastructure CARIBIC/IAGOS. High-Performance Super Computing simulations have been performed by the Deutsches Klima-Rechenzentrum (DKRZ, Hamburg) and the Leibniz-Rechenzentrum (LRZ, München).

Recent atmospheric methane concentrations show an accelerated increase, but the contributions of the underlying emitters are poorly understood. Recording the stable carbon isotope ratio of methane (δ13C(CH4)) is a powerful tool for CH4 source attribution and the understanding of the global methane budget. The airborne measurement of δ13C(CH4) provides the advantages of reaching remote areas and covering large-scale regions, but is challenging regarding sufficient precision while maintaining high spatial measurement density. The state of the art technique is to collect airborne gas samples for subsequent laboratory analysis by isotope ratio mass spectrometry, with high δ13C(CH4) precision of 0.05 ‰. Here we present an innovative in situ airborne system for the measurement of δ13C(CH4), called MIRACLE. MIRACLE consists of a conventional Picarro cavity ring down greenhouse gas analyzer (G2210-i) for the measurement of CH4 and δ13C(CH4), and a sampler unit. The sampler enables the collection of six gas samples in 2 l stainless steel tanks, in a short time (20 s each) via a metal bellows pump, which allows for the specific sampling of small-scale features, such as point source emissions. The sampling is followed by an extended period of subsequent analysis (up to 10 min). Using this setup, we achieve sufficient δ13C(CH4) precision (1σ uncertainty of 0.34 ‰) and an average of five samples per flight hour, allowing for a large number of samples for long flights. Due to the resulting dense coverage with sufficient precision, this novel approach allows for airborne δ13C(CH4) characterization of small-scale methane emitters and large-scale gradients. We employed MIRACLE aboard the research aircraft HALO during the CoMet 2.0 Arctic campaign in summer 2022, which focused on characterizing natural and anthropogenic methane sources in Canada. In this presentation, a proof of concept for the instrument is elaborated, including the investigation of sample purity and measurement comparisons with other instruments. Additionally, we show δ13C(CH4) signatures revealed by the method of Keeling analysis of measurements obtained during CoMet 2.0 and compare them to previous studies. The airborne operation of the MIRACLE instrument combines the advantages of increased precision δ13C(CH4) measurements, typically only possible under stable laboratory conditions, with the in situ, near real time data analysis and the large-scale sampling of secluded areas. MIRACLE will be deployed during the DLR GHGMon campaign (June 2023) to investigate the δ13C(CH4) ratio of agricultural sources of methane in the Netherlands.

The Indochina biomass burning (BB) season in springtime has a substantial environmental impact on the surrounding areas in Asia. In this study, we evaluated the environmental impact of a major long-range BB transport event on 19 March 2018 (a flight of the High Altitude and Long Range Research Aircraft (HALO; https://www.halo-spp.de, last access: 14 February 2023) research aircraft, flight F0319) preceded by a minor event on 17 March 2018 (flight F0317). Aircraft data obtained during the campaign in Asia of the Effect of Megacities on the transport and transformation of pollutants on the Regional to Global scales (EMeRGe) were available between 12 March and 7 April 2018. In F0319, results of 1 min mean carbon monoxide (CO), ozone (O3), acetone (ACE), acetonitrile (ACN), organic aerosol (OA), and black carbon aerosol (BC) concentrations were up to 312.0, 79.0, 3.0, and 0.6 ppb and 6.4 and 2.5 µg m−3, respectively, during the flight, which passed through the BB plume transport layer (BPTL) between the elevation of 2000–4000 m over the East China Sea (ECS). During F0319, the CO, O3, ACE, ACN, OA, and BC maximum of the 1 min average concentrations were higher in the BPTL by 109.0, 8.0, 1.0, and 0.3 ppb and 3.0 and 1.3 µg m−3 compared to flight F0317, respectively. Sulfate aerosol, rather than OA, showed the highest concentration at low altitudes ( m) in both flights F0317 and F0319 resulting from the continental outflow in the ECS. The transport of BB aerosols from Indochina and its impacts on the downstream area were evaluated using a Weather Research Forecasting with Chemistry (WRF-Chem) model. The modeling results tended to overestimate the concentration of the species, with examples being CO (64 ppb), OA (0.3 µg m−3), BC (0.2 µg m−3), and O3 (12.5 ppb) in the BPTL. Over the ECS, the simulated BB contribution demonstrated an increasing trend from the lowest values on 17 March 2018 to the highest values on 18 and 19 March 2018 for CO, fine particulate matter (PM2.5), OA, BC, hydroxyl radicals (OH), nitrogen oxides (NOx), total reactive nitrogen (NOy), and O3; by contrast, the variation of J(O1D) decreased as the BB plume's contribution increased over the ECS. In the lower boundary layer ( m), the BB plume's contribution to most species in the remote downstream areas was %. However, at the BPTL, the contribution of the long-range transported BB plume was as high as 30 %–80 % for most of the species (NOy, NOx, PM2.5, BC, OH, O3, and CO) over southern China (SC), Taiwan, and the ECS. BB aerosols were identified as a potential source of cloud condensation nuclei, and the simulation results indicated that the transported BB plume had an effect on cloud water formation over SC and the ECS on 19 March 2018. The combination of BB aerosol enhancement with cloud water resulted in a reduction of incoming shortwave radiation at the surface in SC and the ECS by 5 %–7 % and 2 %–4 %, respectively, which potentially has significant regional climate implications.

Contrail cirrus constitute the largest radiative forcing (RF) component of the aviation effect on climate. However, the difference of microphysical properties and radiative effects between contrails, contrail cirrus and natural cirrus clouds are still not completely resolved. Motivated by these uncertainties, we investigate the cirrus perturbed by aviation in the North Atlantic Region on 26 March 2014 during the Mid Latitude Cirrus (ML-CIRRUS) experiment. In the synoptic context of a ridge cirrus cloud, an extended thin ice cloud with many persistent contrails can be observed for many hours with the geostationary Meteosat Second Generation (MSG)/Spinning Enhanced Visible and InfraRed Imager (SEVIRI) from the morning hours until dissipation close to 14 UTC. Airborne lidar observations aboard the German High Altitude and LOng Range Research Aircraft (HALO) suggest that this cloud is mainly of anthropogenic origin. We develop a new method to distinguish between contrails, contrail cirrus and natural cirrus based on in situ measurements of ice number and NO gas concentrations. It turns out that effective radii (Reff) of contrail cirrus and contrails are in the range of 3 to 53 µm and about 18 % smaller than that of natural cirrus, hence a difference in Reff is still present. Ice particle sizes in contrail cirrus are on average 114 % larger than in contrails. The optical thickness of natural cirrus, contrail cirrus and contrails derived from satellite data has similar distributions with average values of 0.21, 0.24 and 0.15 for these three cloud types, respectively. As for radiative effects, a new method to estimate top-of-atmosphere instantaneous RF in the solar and thermal range is developed based on radiative transfer model simulations exploiting in situ and lidar measurements, satellite observations and ERA5 reanalysis data for both cirrus and cirrus-free regions. Broadband irradiances estimated from our simulations compare well with satellite observations from MSG and the Geostationary Earth Radiation Budget (GERB), indicating that our method provides a good representation of the real atmosphere and can thus be used to determine RF of ice clouds probed during this flight. Contrails net RF is smaller by a factor of 4 compared to contrail cirrus. On average, the net RF of contrails and contrail cirrus is more strongly warming than that of natural cirrus. For a larger spatial area around the flight path, the RF is well related to that along the flight track. We find warming contrail cirrus and cirrus in the early morning and cooling contrail cirrus and cirrus during the day. The results will be valuable for research to constrain uncertainties in the assessment of climate impacts of natural cirrus and contrail cirrus and for the formulation and evaluation of contrail mitigation options.

Megacities and other major population centres (MPCs) worldwide are major sources of air pollution, both locally as well as downwind. The overall assessment and prediction of the impact of MPC pollution on tropospheric chemistry are challenging. The present work provides an overview of the highlights of a major new contribution to the understanding of this issue based on the data and analysis of the EMeRGe (Effect of Megacities on the transport and transformation of pollutants on the Regional to Global scales) international project. EMeRGe focuses on atmospheric chemistry, dynamics, and transport of local and regional pollution originating in MPCs. Airborne measurements, taking advantage of the long range capabilities of the High Altitude and LOng Range Research Aircraft (HALO, https://www.halo-spp.de, last access: 22 March 2022), are a central part of the project. The synergistic use and consistent interpretation of observational data sets of different spatial and temporal resolution (e.g. from ground-based networks, airborne campaigns, and satellite measurements) supported by modelling within EMeRGe provide unique insight to test the current understanding of MPC pollution outflows. In order to obtain an adequate set of measurements at different spatial scales, two field experiments were positioned in time and space to contrast situations when the photochemical transformation of plumes emerging from MPCs is large. These experiments were conducted in summer 2017 over Europe and in the inter-monsoon period over Asia in spring 2018. The intensive observational periods (IOPs) involved HALO airborne measurements of ozone and its precursors, volatile organic compounds, aerosol particles, and related species as well as coordinated ground-based ancillary observations at different sites. Perfluorocarbon (PFC) tracer releases and model forecasts supported the flight planning, the identification of pollution plumes, and the analysis of chemical transformations during transport. This paper describes the experimental deployment and scientific questions of the IOP in Europe. The MPC targets - London (United Kingdom; UK), the Benelux/Ruhr area (Belgium, the Netherlands, Luxembourg and Germany), Paris (France), Rome and the Po Valley (Italy), and Madrid and Barcelona (Spain) - were investigated during seven HALO research flights with an aircraft base in Germany for a total of 53 flight hours. An in-flight comparison of HALO with the collaborating UK-airborne platform Facility for Airborne Atmospheric Measurements (FAAM) took place to assure accuracy and comparability of the instrumentation on board. Overall, EMeRGe unites measurements of near- and far-field emissions and hence deals with complex air masses of local and distant sources. Regional transport of several European MPC outflows was successfully identified and measured. Chemical processing of the MPC emissions was inferred from airborne observations of primary and secondary pollutants and the ratios between species having different chemical lifetimes. Photochemical processing of aerosol and secondary formation or organic acids was evident during the transport of MPC plumes. Urban plumes mix efficiently with natural sources as mineral dust and with biomass burning emissions from vegetation and forest fires. This confirms the importance of wildland fire emissions in Europe and indicates an important but discontinuous contribution to the European emission budget that might be of relevance in the design of efficient mitigation strategies. The present work provides an overview of the most salient results in the European context, with these being addressed in more detail within additional dedicated EMeRGe studies. The deployment and results obtained in Asia will be the subject of separate publications., The HALO deployment during EMeRGe was funded by a consortium comprising the German Research Foundation (DFG) Priority Program HALO-SPP 1294, the Institute of Atmospheric Physics of DLR, the Max Planck Society (MPG), and the Helmholtz Association. Flora Kluge, Benjamin Schreiner, and Klaus Pfeilsticker acknowledge the support given by the DFG through the project nos. PF 384-16, PF 384-17, and PG 385-19. Ralf Koppmann and Marc Krebsbach acknowledge DFG funding through project no. KR3861_1-1. Katja Bigge acknowledges additional funding from the Heidelberg Graduate School for Physics. Johannes Schneider, Katharina Kaiser, and Stephan Borrmann acknowledge funding through the DFG (project no. 316589531). Lisa Eirenschmalz and Hans Schlager acknowledge support by DFG through project MEPOLL (SCHL1857/4-1). Anna B. Kalisz Hedegaard would like to thank DAAD and DLR for a Research Fellowship. Hans Schlager acknowledge financial support by the DLR TraK (Transport and Climate) project. Michael Sicard acknowledges support from the EU (GA nos. 654109, 778349, 871115, and 101008004) and the Spanish Government (ref. nos. CGL2017-90884-REDT, PID2019-103886RB-I00, RTI2018-096548-B-I00, and MDM-2016-0600). Midhun George, Yangzhuoran Liu, M. Dolores Andrés Hernández, and John Phillip Burrows acknowledge financial support from the University of Bremen. FLEXPART simulations were performed on the HPC cluster Aether at the University of Bremen, financed by DFG within the scope of the Excellence Initiative. Anne-Marlene Blechschmidt was partly funded through the CAMS-84 project. Jennifer Wolf acknowledges support from the German Federal Ministry for Economic Affairs and Energy – BMWi (project Digitally optimized Engineering for Services – DoEfS; contract no. 20X1701B). Theresa Harlass thanks DLR VO-R for funding the young investigator research group “Greenhouse Gases”. Mariano Mertens, Patrick Jöckel, and Markus Kilian acknowledge resources of the Deutsches Klimarechenzentrum (DKRZ) granted by the WLA project ID bd0617 for the MECO(n) simulations and the financial support from the DLR projects TraK (Transport und Klima) and the Initiative and Networking Fund of the Helmholtz Association through the project “Advanced Earth System Modelling Capacity” (ESM). Bruna A. Holanda acknowledges the funding from Brazilian CNPq (process 200723/2015-4). The article processing charges for this open-access publication were covered by the University of Bremen.

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.

The impact of aviation on atmospheric aerosol, its processing, and its effects on climate is still associated with large uncertainties. We identified aircraft exhaust plumes observed during flights of the IAGOS-CARIBIC Flying Laboratory and performed a dedicated analysis of the aviation related atmospheric aerosol properties.The European Research Infrastructure IAGOS (www.iagos.org) is using in-service aircraft as observation platforms, equipped with instrumentation for measuring gaseous species, aerosols, and cloud particles. From July 2018 to March 2020 the IAGOS-CARIBIC Flying Laboratory (equipped with 15 scientific instruments) conducted 42 operational flights aboard a Lufthansa Airbus A340-600 passenger aircraft. These flights covered routes between Munich (Germany) and destinations in North America, South Africa, and East Asia.The IAGOS-CARIBIC data set resulting from these flights includes a wide variety of aerosol and trace gas measurements, which could be fully synchronised for a subset of 36 flights. An algorithm was developed and implemented to automatically identify unique aircraft exhaust plumes based on the 1 Hz resolved NOy and aerosol data sets. For the years 2018 to 2020, the algorithm detected about 1100 unique aircraft exhaust plumes. These exhaust plumes were further categorised as tropospheric (37 %) and stratospheric (63 %) as well as in-cloud (12 %) and clear sky (82 %) conditions, providing a solid statistical bases and global insight into the impact of aviation on aerosol and trace gas properties. For each plume the measured parameters were further divided into their respective background and plume excess values.The analysis of the plume excess characteristics (e.g., in terms of the fraction of accumulation mode particles or the non-volatile aerosol fraction) shows that the aerosol properties inside the plume are independent from their background environment in the upper troposphere, the tropopause region, and the lowermost stratosphere. This would allow a parameterization of the plume aerosol properties independent of the flight altitude. Furthermore, we discuss the evolution of the aerosols aging/processing for the encountered aircraft exhaust plumes.Acknowledgments: Part of this study is funded by the ACACIA project (EU Grant Agreement Number 875036). We thank all members of IAGOS-CARIBIC, in particular Deutsche Lufthansa and Lufthansa Technik for enabling the IAGOS-CARIBIC observatory. The German Federal Ministry of Education and Research (BMBF) is acknowledged for financing the instruments operation and data analysis as part of the joint project IAGOS-D under grants 01LK1301A and 01LK1301C.

In this study, airborne measurements of the sum of hydroperoxyl (HO2) and organic peroxy (RO2) radicals that react with NO to produce NO2, i.e. RO2*, coupled with actinometry and other key trace gases measurements, have been used to test the current understanding of the fast photochemistry in the outflow of major population centres (MPCs). All measurements were made during the airborne campaign of the EMeRGe (Effect of Megacities on the transport and transformation of pollutants on the Regional to Global scales) project in Europe on-board the High Altitude Long range research aircraft (HALO). The on-board measurements of RO2* were made using the in-situ instrument Peroxy Radical Chemical Enhancement and Absorption Spectrometer (PeRCEAS). RO2* mixing ratios up to 120 pptv were observed in air masses of different origins and composition under different local actinometrical conditions during seven HALO research flights in July 2017 over Europe. The range and variability of the RO2* measurements agree reasonably well with radical production rates estimated using photolysis frequencies and RO2* precursor concentrations measured on-board. RO2* is primarily produced following the photolysis of ozone (O3), formaldehyde (HCHO), glyoxal (CHOCHO), and nitrous acid (HONO) in the airmasses investigated. The suitability of photostationary steady-state (PSS) assumptions to estimate the mixing ratios and the variability of RO2* during the airborne observations is investigated. The PSS assumption is robust enough to calculate RO2* mixing rations for most conditions encountered in air masses measured. The similarities and discrepancies between measured and calculated RO2* mixing ratios are analysed stepwise. The parameters, which predominantly control the RO2* mixing ratios under different chemical and physical regimes, are identified during the analysis. The dominant removal processes of RO2* in the airmasses measured up to 2000 m are the loss of OH and RO through the reaction with NOx during the radical interconversion. Above 2000 m, HO2 – HO2 and HO2 – RO2 reactions dominate RO2* loss reactions. RO2* calculations underestimated (< 20 %) the measurements by the analytical expression inside the pollution plumes probed. The underestimation is attributed to the limitations of the PSS analysis to take into account the production of RO2* through oxidation and photolysis of the OVOCs not measured during EMeRGe.

The Indochina biomass burning (BB) season in springtime has a substantial environmental impact on the surrounding areas in Asia. In this study, we evaluated the environmental impact of a major long-range BB transport event on 19 March 2018 (a flight of the HALO research aircraft, flight F0319) preceded by a minor event on 17 March 2018 (flight F0317). Aircraft data obtained during the campaign in Asia of the Effect of Megacities on the transport and transformation of pollutants on the Regional to Global scales (EMeRGe) were available between 12 March and 7 April 2018. In the F0319, results of 1-min mean carbon monoxide (CO), ozone (O3), acetone (ACE), acetonitrile (ACN), organic aerosol (OA) and black carbon aerosol (BC) concentrations were up to 312.0 ppb, 79.0 ppb, 3.0 ppb, 0.6 ppb, 6.4 µg m−3, 2.5 µg m−3 respectively, during the flight, which passed through the BB plume transport layer (BPTL) between the elevation of 2000–4000 m over the East China Sea (ECS). During F0319, CO, O3, ACE, ACN, OA and BC maximum of the 1 minute average concentrations were higher in the BPTL by 109.0 ppb, 8.0 ppb, 1.0 ppb, 0.3 ppb, 3.0 µg m−3 and 1.3 µg m−3 compared to flight F0317, respectively. Sulfate aerosol, rather than OA, showed the highest concentration at low altitudes ( The transport of BB aerosols from Indochina and its impacts on the downstream area was evaluated using a WRF-Chem model. Over the ECS, the simulated BB contribution demonstrated an increasing trend from the lowest values on 17 March 2018 to the highest values on 18 and 19 March 2018 for CO, fine particulate matter (PM2.5), OA, BC, hydroxyl radicals (OH), nitrogen oxides (NOx), total reactive nitrogen (NOy), and O3; by contrast, the variation of J(O1D) decreased as the BB plume’s contribution increased over the ECS. In the low boundary layer (y, NOx, PM2.5, BC, OH, O3, and CO) over South China (SC), Taiwan, and the ECS. BB aerosols were identified as a potential source of cloud condensation nuclei, and the simulation results indicated that the transported BB plume had an effect on cloud water formation over SC and the ECS on 19 March 2018. The combination of BB aerosol enhancement with cloud water resulted in a reduction of incoming shortwave radiation at the surface in SC and the ECS which potentially has significant regional climate implications.

IAGOS (www.iagos.org) is a European Research Infrastructure using commercial aircraft (Airbus A340, A330, and soon A350) for automatic and routine measurements of atmospheric composition including reactive gases (ozone, carbon monoxide, nitrogen oxides, volatile organic compounds), greenhouse gases (water vapour, carbon dioxide, methane), aerosols and cloud particles along with essential thermodynamic parameters. The main objective of IAGOS is to provide the most complete set of high-quality essential climate variables (ECV) covering several decades for the long-term monitoring of climate and air quality. The observations are stored in the IAGOS data centre along with added-value products to facilitate the scientific interpretation of the data. IAGOS began as two European projects, MOZAIC and CARIBIC, in the early 1990s. These projects demonstrated that commercial aircraft are ideal platforms for routine atmospheric measurements. IAGOS then evolved as a European Research Infrastructure offering a mature and sustainable organization for the benefits of the scientific community and for the operational services in charge of air quality and climate change issues such as the Copernicus Atmosphere Monitoring Services (CAMS) and the Copernicus Climate Change Service (C3S). IAGOS is also a contributing network of the World Meteorological Organization (WMO). IAGOS provides measurements of numerous chemical compounds which are recorded simultaneously in the critical region of the upper troposphere – lower stratosphere (UTLS) and geographical regions such as Africa and the mid-Pacific which are poorly sampled by other means. The data are used by hundreds of groups worldwide performing data analysis for climatology and trend studies, model evaluation, satellite validation and the study of detailed chemical and physical processes around the tropopause. IAGOS data also play an important role in the re-assessment of the climate impact of aviation. Most important in the context of weather-related research, IAGOS and its predecessor programmes provide long-term observations of water vapour and relative humidity with respect to ice in the UTLS as well as throughout the tropospheric column during climb-out and descending phases around airports, now for more than 25 years. The high quality and very good resolution of IAGOS observations of relative humidity over ice are used to better understand the role of water vapour and of ice-supersaturated air masses in the tropopause region and to improve their representation in numerical weather and climate forecasting models. Furthermore, CAMS is using the water vapour vertical profiles in near real time for the continuous validation of the CAMS atmospheric models.

Aviation aims to reduce its climate impact by identifying promising mitigation options which are able to reduce the overall climate effects of aviation considering CO2 and non-CO2 effects. While aiming to identify fuel optimal trajectories, aviation also aims to reduce the non-CO2 effects comprising NOx-induced changes of atmospheric ozone and methane. Here climate-chemistry models are required which are able to quantify perturbations in atmospheric composition of reactive species (NOx, O3) and the associated radiative forcings of aviation emissions relying on advanced modelling capabilities, realistic emission inventory data and global-scale observational datasets from research infrastructures like IAGOS and DLR aircraft measurement campaign data. We use the multi-scale climate-chemistry MECO(n) system which is a “MESSy-fied ECHAM and COSMO nested n-times”, relying on the Modular Earth Submodel System (MESSy) framework. For this purpose, both models have been equipped with the MESSy infrastructure, implying that the same process formulations (MESSy submodels) are available for both models. Modelled atmospheric distributions are systematically compared to observational data from aircraft measurements in the upper troposphere and lower stratosphere. Nudging of meteorology to ERA5 interim data, and special diagnostics available within the modular MESSy infrastructure are implemented in the numerical simulations. Online sampling along aircraft trajectories allows to extract model data with a high temporal resolution (MESSy submodel S4D), in order to evaluate model representation and key processes. Beyond systematic evaluation with IAGOS scheduled aircraft measurements, episodes will be evaluated where dedicated measurements from aircraft campaigns are available, comprising Spring 2014 (ML-CIRRUS campaign), early summer 2020 (Blue Sky campaign) and summer 2021 (Cirrus-HL campaign). Our analysis of reactive species, NOy and ozone, identifies those weather pattern and synoptic situations where aviation contributes strong signals, resulting in recommendations on measurement strategies to detect aviation signal in the atmosphere. We evaluate model representation of the NOx-induces effect on radiatively active species ozone and methane in both model instances, ECHAM5 and COSMO. This is key for advancing the scientific understanding of NOx-induced effects from aviation which is required in order to quantify potential compensation and trade-offs when identifying robust mitigation options for sustainable aviation. This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 875036 (ACACIA, Advancing the Science for Aviation and Climate) and has been supported by the DLR-Projekt Eco2Fly. This work uses measurement data from the European Research Infrastructure IAGOS/CARIBIC. High-Performance Super Computing simulations have been performed by the Deutsches Klima-Rechenzentrum (DKRZ, Hamburg) and the Leibniz-Rechenzentrum (LRZ, München).

Sulfate is among the major components of atmospheric aerosols or fine particulate matters. Aerosols loaded with sulfate result in low air quality, damage to ecosystems, and influences on climate change. Sulfate aerosols could originate from that directly emitted to the atmosphere and that produced by atmospheric physicochemical processes. The latter is generated from sulfur dioxide (SO2) via oxidation either in the gas phase reactions or in the aqueous phase. Several mechanisms of SO2 oxidation have been proposed, but the differentiation of the various mechanisms and identification of the sources remain challenging. To meet this need, a new method to estimate the contribution of the gas-phase reaction between hydroxyl radical (OH) and SO2 to the sulfate aerosol is proposed and investigated. Briefly, we consider the OH-reaction rates of the respective trace gases that compete for OH radicals with SO2 in the troposphere, and estimate the fraction of SO2-OH reaction in the total OH reactivity. Then the relationship between sulfate concentration and the SO2-OH reaction is analyzed statistically to investigate the sources of sulfate in aerosols. We test this method using the data from ground-based observations and aircraft measurements made during the Effect of Megacities on the transport and transformation of pollutants on the Regional to Global scales in Asia (EMeRGe-Asia) over the western Taiwan and West Pacific regions. Our results show that the estimated SO2-OH reactivity fraction is well-correlated with sulfate concentration. The sulfate production from SO2-OH reaction accounts for approximately 30 % of the total sulfate in aerosols collected at the surface and near-surface (altitude 2-OH reaction regionally and globally.

During winter 2015/2016 the Arctic stratosphere was characterized by extraordinarily low temperatures in connection with the occurrence of extensive polar stratospheric clouds. From mid of December 2015 until mid of March 2016 the German research aircraft HALO (High Altitude and Long–Range Research Aircraft) was deployed to probe the lowermost stratosphere in the Arctic region within the POLSTRACC (Polar Stratosphere in a Changing Climate) mission. More than twenty flights have been conducted out of Kiruna/Sweden and Oberpfaffenhofen/Germany, covering the whole winter period. Besides total reactive nitrogen (NOy), observations of nitrous oxide, nitric acid, ozone and water were used for this study. Total reactive nitrogen and its partitioning between gas- and particle phase are key parameters for understanding processes controlling the ozone budget in the polar winter stratosphere. The redistribution of total reactive nitrogen was evaluated by using tracer–tracer correlations. In January air masses with extensive nitrification were encountered at altitudes between 12 and 15 km. The excess NOy amounted up to about 6 ppb. During several flights, along with gas–phase nitrification, indications for extensive occurrence of nitric acid containing particles at flight altitude were found. These observations support the assumption of sedimentation and subsequent evaporation of nitric acid containing particles leading to redistribution of total reactive nitrogen. Remnants of nitrified air masses have been observed until mid of March. Between end of February and mid of March also de-nitrified air masses have been observed in connection with high potential temperatures. Using tracer–tracer correlations, missing total reactive nitrogen was estimated to amount up to 6 ppb. This indicates the downward transport of air masses that have been denitrified during the earlier winter phase. Observations within POLSTRACC, at the bottom of the vortex, reflect heterogeneous processes from the overlying Arctic winter stratosphere. The comparison of the observations with CLaMS model simulations confirm and complete the picture arising from the present measurements. The simulations confirm, that the ensemble of all observations is representative for the vortex–wide vertical NOy-redistribution.

Comprehensive regional chemistry-climate or chemistry transport models are important tools to study the impact of emissions from major population centres (MPC) and/or investigate potential mitigation options for MPC emissions. Before such models can be employed it is important to investigate how well the models represent observed atmospheric conditions. This comparison helps not only in judging the performance of the models, but allows to test our understanding of chemical and physical processes in the atmosphere. A prerequisite for an extensive evaluation of models are the availability of temporally and spatially high resolved observational data. Such a data set was obtained during the EMeRGe-Europe campaign of the HALO research aircraft in July 2017, which targeted the outflow of different MPC in Europe.We used the data of the EMeRGe-EU campaign together with ground based observations to evaluate the representation of European MPC emissions in the MECO(n) model system. MECO(n) is a global/regional chemistry-climate model which couples the regional chemistry-climate model COSMO-CLM/MESSy on-line (i.e., during runtime) with the global chemistry climate-model EMAC. The dynamics of EMAC is nudged against ERA-Interim reanalysis data. We performed three nesting steps from 300 km on the global scale to 50 km, 12 km and 7 km on the regional scale. In our evaluation we focus on tropospheric ozone (O3) and related precursors, methane (CH4) and sulphur dioxide (SO2). Generally, the comparison between the measurements and the model results shows a good representation of European MPC emissions in MECO(n). In detail, however, the measured mixing ratios of carbon monoxide (CO) and reactive nitrogen (NOy) are underestimated, while O3 and SO2 are overestimated by the model. Potential reasons for these differences are too efficient vertical mixing, and underestimation of MPC emissions. To test hypotheses for potential model improvements we performed additional sensitivity studies with different nudging data for EMAC and an alternative anthropogenic emission inventory. The differences of the model results to the observations, however, are only slightly influenced by these changes. Accordingly, further hypotheses for potential model improvements needs to be investigated. While the simulated mixing ratios differ only slightly between the sensitivity studies, the ozone source apportionment results (using a tagging approach) show much larger differences. This indicates the large uncertainty of source apportionment analyses caused by uncertainties of emission inventories and model dynamics and requires further analysis in the future.

The biomass burning season in America was exceptionally intense during summer 2019. Particularly in the subtropics biomass burning potentially contributes significantly to the trace gas budget of the upper troposphere and can affect chemistry and composition far from the source.During the SOUTHTRAC mission, which took place in September and November 2019, several cross sections from the equator to the southern tip of south America were flown at typical altitudes of 13-14 km. During the northbound flight on October, 7th 2019 massive enhancements of pollutants were observed at these altitudes. Notably, in-situ observations show continuously elevated CO values exceeding 200 ppbv over a flight distance of more than 1000 km. These massive enhancements were accompanied by largely elevated NO and NOy as well as CO2 and could be attributed to the large fires in South America during this time. Observations of C2H2 and PAN from GLORIA show, that pollution covered a layer extending from 8-9 km to the flight level at 13 km.Comparing the tracer observations to previous flights in exactly the same region three weeks earlier, we could estimate the ozone production due to the biomass burning. Based on first results we estimate ozone production in the polluted air masses up to 30-40 ppbv in the UT which is almost 40% of the observed ozone mixing ratio. Given the large extent of the polluted area over 15 degrees of latitude this may have an impact on the local energy budget of the tropopause region.

Since peroxy radicals are closely involved in a number of tropospheric chemical processes like O3 budget, hydrocarbon oxidation and acid formation, the accurate measurement of these radicals can provide essential information to improve our understanding of processing and transformation of polluted outflows from megacities and Major Population Centres (MPCs).Airborne measurements of the total sum of peroxy radicals, RO2* = HO2 + ∑ RO2, where R is an organic group, were conducted in Europe in summer 2017 and in East Asia in spring 2018 within the EMeRGe (Effect of Megacities on the Transport and Transformation of Pollutants on the Regional to Global Scales) project by using the PeRCEAS instrument (Peroxy Radical Chemical Enhancement and Absorption Spectrometer), on board of the HALO research aircraft (www.halo.dlr.de).Over the course of both measurement campaigns different MPC outflows were investigated including among others, London, Rome, Manila and Taipei. Polluted air masses of different origin and composition were probed. Overall the peroxy radical mixing ratios were of the same order of magnitude in the air masses probed in Europe and in East Asia. The variations in the photochemical activity were studied by taking into account simultaneous observations of radical precursors and photolysis rates, while applying known oxidation mechanisms. Radical precursors, photolysis rates and aerosol load were generally higher in Asia, which might indicate higher radical loss reactions on the aerosol surface than in Europe. Moreover this study shows a clear deviation in the photostationary state for MPC outflows close to the emission sources. Based on this information, this presentation will focus on the actual understanding of the photochemical processing in the probed air masses.

Middle and long-term photo-chemical effects of local and regional pollution are not well quantified and are an area of active study. NOx (here defined as NO, NO2, and HONO) is a regional pollutant, which influences atmospheric oxidation capacity and ozone formation. Airborne measurements of atmospheric trace gases from the HALO (High Altitude Long Range) aircraft, particularly of NO, NO2, and HONO were performed as part of the EMeRGe (Effect of Megacities on the Transport and Transformation of Pollutants on the Regional to Global Scales) campaign over continental Europe and southeast Asia in July 2017 and April 2018, respectively. NO (and NOY), O3, and the photolysis frequencies of NO2 and HONO were measured in-situ. NO2 and HONO were inferred from Limb measurements of the mini-DOAS (Differential Optical Absorption Spectroscopy) instrument, using the novel scaling method (Hüneke et al., 2017). These measurements were compared with simulations of the MECO/EMAC models. In relatively polluted air-masses in the boundary layer and free troposphere, HONO measured in excess of model predictions (and previous measurements) suggests an in-situ formation and a significant source of OH as well as a pathway for re-noxification. Aerosol composition simultaneously measured by the C-Tof-AMS instrument may reveal potential reaction mechanisms to explain the discrepancy.

At the industrial revolution (1750-1800), the population of the earth was around 1 Billion and less than 5% of population lived in urban areas. In 1950, when the population reached about 2.9 billion, there were two megacities New York/Newark and Tokyo. In 2020, the earth’s population is around 7.8 Billion, more than 50% live in urban areas and there are now approximately 38 around the world. Since 2007, more than 50% of the population live in urban areas and the earth’s population has now reached 7.8 Billion. Anthropogenic activity to sustain and feed MPC is now one of the most important sources of pollution, modifying atmospheric chemistry, air quality and climate. To assess the impact of MPC emissions locally and regionally requires knowledge of the transport and transformation of the MPC plumes. The EMeRGe project was proposed to address this need and investigate the transport and transformation of the chemical composition of MPC plumes. Secondary objectives include the improvement of our understanding of the impact of biomass burning, which mixes with the plumes from MPC. EMeRGe selected European and Asian MPC as targets, where the regulations on emissions are significantly different.EMeRGe assumes that the nature of the local emissions, the meteorology and photochemistry/chemistry determines the transport and transformation of the plumes from MPCs. To test this hypothesis, the following scientific questions are addressed: a) which transport and dispersion processes dominate the MPC outflows in Europe and Asia during the selected measurement periods;b) which oxidation or other processes determine the chemical transformation of MPC emissions;c) what are the regional impacts of the emission by the selected European and Asian MPCs;d) what is the relevance of emission from European and Asian MPCs for radiative forcing and climate change;e) do our chemical models adequately simulate of transport and transformation processes of European and Asian MPC outflows.An integrating focus of EMeRGe were the measurement campaigns exploiting the capabilities of the German HALO research were undertaken during EMeRGe, which investigated the outflow from: i) European MPCs in July 2017; ii) MPCs in East and South East Asia during March and April 2018. In addition to the HALO aircraft measurements, the EMeRGe International scientists contributed studies of the measurement from instrumentation from ground based, airborne and satellite platforms. For example in EMeRGe in Europe the UK NERC FAAM (https://nerc.ukri.org/research/sites/facilities/aircraft/) "ERA - CNR - ISAFOM" (https://www.eufar.net/aircrafts/44) were deployed to make measurements around London and Rome respectively. In EMeRGe in Asia, measurement were made ground based and Lidar measurements were made by EMeRGe partners from Taiwan, Japan, the Philippines, Thailand and China. EMeRGe benefited from the support by iCACGP (international Commission on Atmospheric Chemistry and Global Pollution). This presentation will provide an overview of the objectives, the planning, the measurements and some highlights from the EMeRGe HALO campaigns.

During the OMO (Oxidation Mechanism Observation) mission, trace gas measurements were performed on board the HALO (High Altitude Long Range) research aircraft in summer 2015 in order to investigate the outflow of the South Asian summer monsoon and its influence on the composition of the Asian monsoon anticyclone (AMA) in the upper troposphere over the eastern Mediterranean and the Arabian Peninsula. This study focuses on in situ observations of hydrogen peroxide (H2O2obs) and organic hydroperoxides (ROOHobs) as well as their precursors and loss processes. Observations are compared to photostationary-state (PSS) calculations of H2O2PSS and extended by a separation of ROOHobs into methyl hydroperoxide (MHPPSS) and inferred unidentified hydroperoxide (UHPPSS) mixing ratios using PSS calculations. Measurements are also contrasted to simulations with the general circulation ECHAM–MESSy for Atmospheric Chemistry (EMAC) model. We observed enhanced mixing ratios of H2O2obs (45 %), MHPPSS (9 %), and UHPPSS (136 %) in the AMA relative to the northern hemispheric background. Highest concentrations for H2O2obs and MHPPSS of 211 and 152 ppbv, respectively, were found in the tropics outside the AMA, while for UHPPSS, with 208 pptv, highest concentrations were found within the AMA. In general, the observed concentrations are higher than steady-state calculations and EMAC simulations by a factor of 3 and 2, respectively. Especially in the AMA, EMAC underestimates the H2O2EMAC (medians: 71 pptv vs. 164 pptv) and ROOHEMAC (medians: 25 pptv vs. 278 pptv) mixing ratios. Longitudinal gradients indicate a pool of hydroperoxides towards the center of the AMA, most likely associated with upwind convection over India. This indicates main contributions of atmospheric transport to the local budgets of hydroperoxides along the flight track, explaining strong deviations from steady-state calculations which only account for local photochemistry. Underestimation of H2O2EMAC by approximately a factor of 2 in the Northern Hemisphere (NH) and the AMA and overestimation in the Southern Hemisphere (SH; factor 1.3) are most likely due to uncertainties in the scavenging efficiencies for individual hydroperoxides in deep convective transport to the upper troposphere, corroborated by a sensitivity study. It seems that the observed excess UHPPSS is excess MHP transported to the west from an upper tropospheric source related to convection in the summer monsoon over Southeast Asia.

We present measurements of ozone, water vapour and nitric acid in the upper troposphere/lower stratosphere (UTLS) over North Atlantic and Europe. The measurements were acquired with the Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) during the Wave Driven Isentropic Exchange (WISE) campaign in October 2017. GLORIA is an airborne limb imager capable of acquiring both 2-D data sets (curtains along the flight path) and, when the carrier aircraft is flying around the observed air mass, spatially highly resolved 3-D tomographic data. We show a case study of a Rossby wave (RW) breaking event observed during two subsequent flights two days apart. RW breaking is known to steepen tracer gradients and facilitate stratosphere-troposphere exchange (STE). Our measurements reveal complex spatial structures in stratospheric tracers (ozone and nitric acid) with multiple vertically stacked filaments. Backward trajectory analysis is used to demonstrate that these features are related to several previous Rossby wave breaking events and that the small-scale structure of the UTLS in the Rossby wave breaking region, which is otherwise very hard to observe, can be understood as stirring and mixing of air masses of tropospheric and stratospheric origin. It is also shown that a strong nitric acid enhancement observed just above the tropopause is likely a result of NOx production by lightning activity. The measurements showed signatures of enhanced mixing between stratospheric and tropospheric air near the polar jet with some transport of water vapour into the stratosphere. Some of the air masses seen in 3-D data were encountered again two days later, stretched to very thin filament (horizontal thickness down to 30 km at some altitudes) rich in stratospheric tracers. This repeated measurement allowed us to directly observe and analyse the progress of mixing processes in a thin filament over two days. Our results provide direct insight into small-scale dynamics of the UTLS in the Rossby wave breaking region, witch is of great importance to understanding STE and poleward transport in the UTLS.

South Asian monsoon and pollution Air pollution is growing fastest in monsoon-impacted South Asia. During the dry winter monsoon, the fumes disperse toward the Indian Ocean, creating a vast pollution haze. The fate of these fumes during the wet summer monsoon has been unclear. Lelieveld et al. performed atmospheric chemistry measurements by aircraft in the Oxidation Mechanism Observations campaign, sampling the summer monsoon outflow in the upper troposphere between the Mediterranean and the Indian Ocean. The measurements, supported by model calculations, show that the monsoon sustains a remarkably efficient cleansing mechanism in which contaminants are rapidly oxidized and deposited on Earth's surface. However, some pollutants are lofted above the monsoon clouds and chemically processed in a reactive reservoir before being redistributed globally, including to the stratosphere. Science , this issue p. 270

The Midlatitude Cirrus experiment (ML-CIRRUS) deployed the High Altitude and Long Range Research Aircraft (HALO) to obtain new insights into nucleation, life cycle, and climate impact of natural cirrus and aircraft-induced contrail cirrus. Direct observations of cirrus properties and their variability are still incomplete, currently limiting our understanding of the clouds’ impact on climate. Also, dynamical effects on clouds and feedbacks are not adequately represented in today’s weather prediction models. Here, we present the rationale, objectives, and selected scientific highlights of ML-CIRRUS using the G-550 aircraft of the German atmospheric science community. The first combined in situ–remote sensing cloud mission with HALO united state-of-the-art cloud probes, a lidar and novel ice residual, aerosol, trace gas, and radiation instrumentation. The aircraft observations were accompanied by remote sensing from satellite and ground and by numerical simulations. In spring 2014, HALO performed 16 flights above Europe with a focus on anthropogenic contrail cirrus and midlatitude cirrus induced by frontal systems including warm conveyor belts and other dynamical regimes (jet streams, mountain waves, and convection). Highlights from ML-CIRRUS include 1) new observations of microphysical and radiative cirrus properties and their variability in meteorological regimes typical for midlatitudes, 2) insights into occurrence of in situ–formed and lifted liquid-origin cirrus, 3) validation of cloud forecasts and satellite products, 4) assessment of contrail predictability, and 5) direct observations of contrail cirrus and their distinction from natural cirrus. Hence, ML-CIRRUS provides a comprehensive dataset on cirrus in the densely populated European midlatitudes with the scope to enhance our understanding of cirrus clouds and their role for climate and weather.

The Arctic winter 2015/16 was characterized by exceptionally cold stratospheric temperatures, favouring the formation of polar stratospheric clouds (PSCs) from mid-December until the end of February down to low stratospheric altitudes. Observations by GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) on HALO (High Altitude and LOng range research aircraft) during the PGS (POLSTRACC/GW-LCYLCE II/SALSA) campaign from December 2015 to March 2016 allow an investigation of the influence of denitrification on the lowermost stratosphere (LMS) with a high spatial resolution. For the first time vertical cross-sections of nitric acid (HNO3) along the flight track and tracer-tracer correlations derived from the GLORIA observations document detailed pictures of wide-spread nitrification of the Arctic LMS during the course of an entire winter. GLORIA observations show large-scale structures and local fine structures with strongly enhanced absolute HNO3 volume mixing ratios reaching up to 11 ppbv at altitudes of 11 km in January and nitrified filaments persisting until the middle of March. Narrow streaks of enhanced HNO3, observed in mid-January, are interpreted as regions recently nitrified by sublimating HNO3-containing particles. Overall, a nitrification of the LMS between 5.0 ppbv and 7.0 ppbv at potential temperature levels between 350 and 380 K is estimated. This extent of nitrification has never been observed before in the Arctic lowermost stratosphere. The GLORIA observations are compared with CLaMS (Chemical Lagrangian Model of the Stratosphere) simulations. The fundamental structures observed by GLORIA are well reproduced, but differences in the fine structures are diagnosed. Further, CLaMS predominantly underestimates the spatial extent of maximum HNO3 mixing ratios derived from the GLORIA observations as well as the enhancement at lower altitudes. Sensitivity simulations with CLaMS including (i) enhanced sedimentation rates in case of ice supersaturation (to resemble ice nucleation on NAT), (ii) a global temperature offset, (iii) modified growth rates (to resemble aspherical particles with larger surfaces) and (iv) temperature fluctuations (to resemble the impact of small-scale mountain waves) mostly improve the agreement with the GLORIA observations. The sensitivity simulations suggest that details of particle microphysics play a significant role for simulated LMS nitrification in January, while air subsidence, transport and mixing become increasingly important towards the end of the winter.

Nitrogen oxide (NO and NOy) measurements were performed onboard an in-service aircraft within the framework of CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container). A total of 330 flights were completed from May 2005 through April 2013 between Frankfurt/Germany and destination airports in Canada, the USA, Brazil, Venezuela, Chile, Argentina, Colombia, South Africa, China, South Korea, Japan, India, Thailand, and the Philippines. Different regions show differing NO and NOy mixing ratios. In the mid-latitudes, observed NOy and NO generally shows clear seasonal cycles in the upper troposphere with a maximum in summer and a minimum in winter. Mean NOy mixing ratios vary between 1.36 nmol/mol in summer and 0.27 nmol/mol in winter. Mean NO mixing ratios range between 0.05 nmol/mol and 0.22 nmol/mol. Regions south of 40°N show no consistent seasonal dependence. Based on CO observations, low, median and high CO air masses were defined. According to this classification, more data was obtained in high CO air masses in the regions south of 40°N compared to the midlatitudes. This indicates that boundary layer emissions are more important in these regions. In general, NOy mixing ratios are highest when measured in high CO air masses. This dataset is one of the most comprehensive NO and NOy dataset available today for the upper troposphere and is therefore highly suitable for the validation of atmosphere-chemistry-models.

During the ACRIDICON-CHUVA field project (September–October 2014; based in Manaus, Brazil) aircraft-based in-situ measurements of aerosol chemical composition were conducted in the tropical troposphere over the Amazon using the High Altitude and Long Range Research Aircraft (HALO), covering altitudes from the boundary layer height up to 14.4 km. The submicron non-refractory aerosol was characterized by flash-vaporization/electron impact-ionization aerosol particle mass spectrometry. The results show that significant secondary organic aerosol (SOA) formation by isoprene oxidation products occurs in the upper troposphere, leading to increased organic aerosol mass concentrations above 10 km altitude. The median organic mass concentrations in the upper troposphere above 10 km range between 1.0 and 2.1 μg m−3 (referring to standard temperature and pressure; STP) with interquartile ranges of 0.6 to 3.0 μg m−3 (STP), representing 70 % of the total submicron non-refractory aerosol particle mass. The presence of isoprene epoxydiol-derived isoprene secondary organic aerosol (IEPOX-SOA) was confirmed by marker peaks in the mass spectra. We estimate the contribution of IEPOX-SOA to the total organic aerosol in the upper troposphere to be about 20 %. After isoprene emission from vegetation, oxidation processes occur at low altitudes and/or during transport to higher altitudes, which may lead to the formation of IEPOX (one oxidation product of isoprene). Reactive uptake or condensation of IEPOX on pre-existing particles leads to IEPOX-SOA formation and subsequently increasing organic mass in the upper troposphere. This organic mass increase was accompanied by an increase of the nitrate mass concentrations, most likely due to NOx production by lightning. We further found that the ammonium contained in the aerosol particles is not sufficient to neutralize the particulate sulfate and nitrate. Analysis of the ion ratio of NO+ to NO2+ indicated that nitrate in the upper troposphere exists mainly in the form of organic nitrate. IEPOX-SOA and organic nitrates are coincident with each other, indicating that IEPOX-SOA forms in the upper troposphere either on acidic nitrate particles forming organic nitrates derived from IEPOX or on already neutralized organic nitrate aerosol particles.

The WeCare project (Utilizing Weather information for Climate efficient and eco efficient future aviation), an internal project of the German Aerospace Center (Deutsches Zentrum für Luft- und Raumfahrt, DLR), aimed at finding solutions for reducing the climate impact of aviation based on an improved understanding of the atmospheric impact from aviation by making use of measurements and modeling approaches. WeCare made some important contributions to advance the scientific understanding in the area of atmospheric and air transportation research. We characterize contrail properties, show that the aircraft type significantly influences these properties, and how contrail-cirrus interacts with natural cirrus. Aviation NOx emissions lead to ozone formation and we show that the strength of the ozone enhancement varies, depending on where within a weather pattern NOx is emitted. These results, in combination with results on the effects of aerosol emissions on low cloud properties, give a revised view on the total radiative forcing of aviation. The assessment of a fleet of strut-braced wing aircraft with an open rotor is investigated and reveals the potential to significantly reduce the climate impact. Intermediate stop operations have the potential to significantly reduce fuel consumption. However, we find that, if only optimized for fuel use, they will have an increased climate impact, since non-CO2 effects compensate the reduced warming from CO2 savings. Avoiding climate sensitive regions has a large potential in reducing climate impact at relatively low costs. Taking advantage of a full 3D optimization has a much better eco-efficiency than lateral re-routings, only. The implementation of such operational measures requires many more considerations. Non-CO2 aviation effects are not considered in international agreements. We showed that climate-optimal routing could be achieved, if market-based measures were in place, which include these non-CO2 effects. An alternative measure to foster climate-optimal routing is the closing of air spaces, which are very climate-sensitive. Although less effective than an unconstrained optimization with respect to climate, it still has a significant potential to reduce the climate impact of aviation. By combining atmospheric and air transportation research, we assess climate mitigation measures, aiming at providing information to aviation stakeholders and policy-makers to make aviation more climate compatible.

Novel airborne in situ measurements of inorganic chlorine, nitrogen oxide species, and ozone were performed inside the lower Antarctic polar vortex and at its edge in September 2012. We focus on one flight during the Transport and Composition of the LMS/Earth System Model Validation (TACTS/ESMVal) campaign with the German research aircraft HALO (High-Altitude LOng range research aircraft), reaching latitudes of 65°S and potential temperatures up to 405 K. Using the early winter correlations of reactive trace gases with N2O from the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS), we find high depletion of chlorine reservoir gases up to ∼40% (0.8 ppbv) at 12 km to 14 km altitude in the vortex and 0.4 ppbv at the edge in subsided stratospheric air with mean ages up to 4.5 years. We observe denitrification of up to 4 ppbv, while ozone was depleted by 1.2 ppmv at potential temperatures as low as 380 K. The advanced instrumentation aboard HALO enables high-resolution measurements with implications for the oxidation capacity of the lowermost stratosphere.

We present in situ measurements of the trace gas composition of the upper tropospheric (UT) Asian summer monsoon anticyclone (ASMA) performed with the High Altitude and Long Range Research Aircraft (HALO) in the frame of the Earth System Model Validation (ESMVal) campaign. Air masses with enhanced O3 mixing ratios were encountered after entering the ASMA at its southern edge at about 150 hPa on 18 September 2012. This is in contrast to the presumption that the anticyclone's interior is dominated by recently uplifted air with low O3 in the monsoon season. We also observed enhanced CO and HCl in the ASMA, which are tracers for boundary layer pollution and tropopause layer (TL) air or stratospheric in-mixing respectively. In addition, reactive nitrogen was enhanced in the ASMA. Along the HALO flight track across the ASMA boundary, strong gradients of these tracers separate anticyclonic from outside air. Lagrangian trajectory calculations using HYSPLIT show that HALO sampled a filament of UT air three times, which included air masses uplifted from the lower or mid-troposphere north of the Bay of Bengal. The trace gas gradients between UT and uplifted air masses were preserved during transport within a belt of streamlines fringing the central part of the anticyclone (fringe), but are smaller than the gradients across the ASMA boundary. Our data represent the first in situ observations across the southern part and downstream of the eastern ASMA flank. Back-trajectories starting at the flight track furthermore indicate that HALO transected the ASMA where it was just splitting into a Tibetan and an Iranian part. The O3-rich filament is diverted from the fringe towards the interior of the original anticyclone, and is at least partially bound to become part of the new Iranian eddy. A simulation with the ECHAM/MESSy Atmospheric Chemistry (EMAC) model is found to reproduce the observations reasonably well. It shows that O3-rich air is entrained by the outer streamlines of the anticyclone at its eastern flank. Back-trajectories and increased HCl mixing ratios indicate that the entrained air originates in the stratospherically influenced TL. Photochemical ageing of air masses in the ASMA additionally increases O3 in originally O3-poor, but CO-rich air. Simulated monthly mean trace gas distributions show decreased O3 in the ASMA centre only at the 100 hPa level in July and August, but at lower altitudes and in September the ASMA is dominated by increased O3. The combination of entrainment from the tropopause region, photochemistry and dynamical instabilities can explain the in situ observations, and might have a larger impact on the highly variable trace gas composition of the anticyclone than previously thought.

Until a decade ago, acetone was assumed to be a dominant HOx source in the dry extra-tropical upper troposphere (ex-UT). New photodissociation quantum yields of acetone and the lack of representative data from the ex-UT challenged that assumption. Regular mass spectrometric observations onboard the Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container (CARIBIC) passenger aircraft deliver the first representative distribution of acetone in the UT/LMS (UT/lowermost stratosphere). Based on diverse CARIBIC trace gas data and non-observed parameters taken from the model ECHAM5/MESSy for Atmospheric Chemistry, we quantify the HOx source in the UT/LMS from (photo)oxidation of acetone. The findings are contrasted to HOx production from ozone photolysis, overall the dominant tropospheric HOx source. It is shown that HOx production from acetone (photo)oxidation reaches up to 95% of the HOx source from ozone photolysis in autumn in the UT and on average ~61% in summer. That is, acetone is a significant source of HOx in the UT/LMS.

Between 1 September and 4 October 2014, a combined airborne and ground-based measurement campaign was conducted to study tropical deep convective clouds over the Brazilian Amazon rain forest. The new German research aircraft, High Altitude and Long Range Research Aircraft (HALO), a modified Gulfstream G550, and extensive ground-based instrumentation were deployed in and near Manaus (State of Amazonas). The campaign was part of the German–Brazilian Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems–Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (Global Precipitation Measurement) (ACRIDICON– CHUVA) venture to quantify aerosol–cloud–precipitation interactions and their thermodynamic, dynamic, and radiative effects by in situ and remote sensing measurements over Amazonia. The ACRIDICON–CHUVA field observations were carried out in cooperation with the second intensive operating period of Green Ocean Amazon 2014/15 (GoAmazon2014/5). In this paper we focus on the airborne data measured on HALO, which was equipped with about 30 in situ and remote sensing instruments for meteorological, trace gas, aerosol, cloud, precipitation, and spectral solar radiation measurements. Fourteen research flights with a total duration of 96 flight hours were performed. Five scientific topics were pursued: 1) cloud vertical evolution and life cycle (cloud profiling), 2) cloud processing of aerosol particles and trace gases (inflow and outflow), 3) satellite and radar validation (cloud products), 4) vertical transport and mixing (tracer experiment), and 5) cloud formation over forested/deforested areas. Data were collected in near-pristine atmospheric conditions and in environments polluted by biomass burning and urban emissions. The paper presents a general introduction of the ACRIDICON– CHUVA campaign (motivation and addressed research topics) and of HALO with its extensive instrument package, as well as a presentation of a few selected measurement results acquired during the flights for some selected scientific topics.

Understanding the role of climate-sensitive trace gas variabilities in the upper troposphere and lower stratosphere region (UTLS) and their impact on its radiative budget requires accurate measurements. The composition of the UTLS is governed by transport and chemistry of stratospheric and tropospheric constituents, such as chlorine, nitrogen oxide and sulfur compounds. The Atmospheric chemical Ionization Mass Spectrometer AIMS has been developed to accurately measure a set of these constituents on aircraft by means of chemical ionization. Here we present a setup using SF5− reagent ions for the simultaneous measurement of trace gas concentrations of HCl, HNO3 and SO2 in the pptv to ppmv (10−12 to 10−6 mol mol−1) range with in-flight and online calibration called AIMS-TG (Atmospheric chemical Ionization Mass Spectrometer for measurements of trace gases). Part 1 of this paper (Kaufmann et al., 2016) reports on the UTLS water vapor measurements with the AIMS-H2O configuration. The instrument can be flexibly switched between two configurations depending on the scientific objective of the mission. For AIMS-TG, a custom-made gas discharge ion source has been developed for generation of reagent ions that selectively react with HCl, HNO3, SO2 and HONO. HNO3 and HCl are routinely calibrated in-flight using permeation devices; SO2 is continuously calibrated during flight adding an isotopically labeled 34SO2 standard. In addition, we report on trace gas measurements of HONO, which is sensitive to the reaction with SF5−. The detection limit for the various trace gases is in the low 10 pptv range at a 1 s time resolution with an overall uncertainty of the measurement of the order of 20 %. AIMS has been integrated and successfully operated on the DLR research aircraft Falcon and HALO (High Altitude LOng range research aircraft). As an example, measurements conducted during the TACTS/ESMVal (Transport and Composition of the LMS/UT and Earth System Model Validation) mission with HALO in 2012 are presented, focusing on a classification of tropospheric and stratospheric influences in the UTLS region. The combination of AIMS measurements with other measurement techniques yields a comprehensive picture of the sulfur, chlorine and reactive nitrogen oxide budget in the UTLS. The different trace gases measured with AIMS exhibit the potential to gain a better understanding of the trace gas origin and variability at and near the tropopause.

Airborne lidar and in-situ measurements of aerosols and trace gases were performed in volcanic ash plumes over Europe between Southern Germany and Iceland with the Falcon aircraft during the eruption period of the Eyjafjalla volcano between 19 April and 18 May 2010. Flight planning and measurement analyses were supported by a refined Meteosat ash product and trajectory model analysis. The volcanic ash plume was observed with lidar directly over the volcano and up to a distance of 2700 km downwind, and up to 120 h plume ages. Aged ash layers were between a few 100 m to 3 km deep, occurred between 1 and 7 km altitude, and were typically 100 to 300 km wide. Particles collected by impactors had diameters up to 20 μm diameter, with size and age dependent composition. Ash mass concentrations were derived from optical particle spectrometers for a particle density of 2.6 g cm−3 and various values of the refractive index (RI, real part: 1.59; 3 values for the imaginary part: 0, 0.004 and 0.008). The mass concentrations, effective diameters and related optical properties were compared with ground-based lidar observations. Theoretical considerations of particle sedimentation constrain the particle diameters to those obtained for the lower RI values. The ash mass concentration results have an uncertainty of a factor of two. The maximum ash mass concentration encountered during the 17 flights with 34 ash plume penetrations was below 1 mg m−3. The Falcon flew in ash clouds up to about 0.8 mg m−3 for a few minutes and in an ash cloud with approximately 0.2 mg m−3 mean-concentration for about one hour without engine damage. The ash plumes were rather dry and correlated with considerable CO and SO2 increases and O3 decreases. To first order, ash concentration and SO2 mixing ratio in the plumes decreased by a factor of two within less than a day. In fresh plumes, the SO2 and CO concentration increases were correlated with the ash mass concentration. The ash plumes were often visible slantwise as faint dark layers, even for concentrations below 0.1 mg m−3. The large abundance of volatile Aitken mode particles suggests previous nucleation of sulfuric acid droplets. The effective diameters range between 0.2 and 3 μm with considerable surface and volume contributions from the Aitken and coarse mode aerosol, respectively. The distal ash mass flux on 2 May was of the order of 500 (240–1600) kg s−1. The volcano induced about 10 (2.5–50) Tg of distal ash mass and about 3 (0.6–23) Tg of SO2 during the whole eruption period. The results of the Falcon flights were used to support the responsible agencies in their decisions concerning air traffic in the presence of volcanic ash.

An airfreight container with automated instruments for measurement of atmospheric gases and trace compounds was operated on a monthly basis onboard a Boeing 767-300 ER of LTU International Airways during long-distance flights from 1997 to 2002 (CARIBIC, Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container, http://www.caribic-atmospheric.com). Subsequently a more advanced system has been developed, using a larger capacity container with additional equipment and an improved inlet system. CARIBIC phase #2 was implemented on a new long-range aircraft type Airbus A340-600 of the Lufthansa German Airlines (Star Alliance) in December 2004, creating a powerful flying observatory. The instrument package comprises detectors for the measurement of O3, total and gaseous H2O, NO and NOy, CO, CO2, O2, Hg, and number concentrations of sub-micrometer particles (>4 nm, >12 nm, and >18 nm diameter). Furthermore, an optical particle counter (OPC) and a proton transfer mass spectrometer (PTR-MS) are incorporated. Aerosol samples are collected for analysis of elemental composition and particle morphology after flight. Air samples are taken in glass containers for laboratory analyses of hydrocarbons, halocarbons and greenhouse gases (including isotopic composition of CO2) in several laboratories. Absorption tubes collect oxygenated volatile organic compounds. Three differential optical absorption spectrometers (DOAS) with their telescopes mounted in the inlet system measure atmospheric trace gases such as BrO, HONO, and NO2. A video camera mounted in the inlet provides information about clouds along the flight track. The flying observatory, its equipment and examples of measurement results are reported.

International audience; During the Mediterranean Intensive Oxidant Study (MINOS) in August 2001 a total of 14 measurement flights were performed with the DLR Falcon aircraft from Heraklion, Crete. One objective of this campaign was to investigate the role of long-range transport of pollutants into the Mediterranean area. An analysis of 5-day back trajectories indicates that in the lower troposphere (0?4 km) air masses originated from eastern and western Europe, in the mid-troposphere (4?8 km) from the Atlantic Ocean region and in the upper troposphere (8?14 km) from North Artlantic Ocean/North America (NAONA) as well as South Asia. We allocated all back trajectories to clusters based on their ending height and source region. The mixing ratios of ozone, nitrogen oxide, total reactive oxidized nitrogen (NOy), formaldehyde, methanol, acetonitrile, acetone, peroxyacetyl nitrate (PAN), carbon dioxide, carbon monoxide and methane measured along the flight tracks are examined in relation to the different cluster trajectories. In the lower troposphere the mean gas mixing ratios of the eastern Europe cluster trajectories were significantly higher than that from western Europe. Considering 2-day instead of 5-day trajectories the relative differences between the concentrations of these two clusters increased. In the upper troposphere relatively high concentrations of O3 and NOy, combined with low CO of the NAONA trajectories indicate mixing with stratospheric air masses.

A coupled tropospheric chemistry-climate model is used to analyze tropospheric ozone distributions observed during the MINOS campaign in the eastern Mediterranean region (August, 2001). Modeled ozone profiles are generally in good agreement with the observations. Our analysis shows that the atmospheric dynamics in the region are strongly influenced by the occurrence of an upper tropospheric anti-cyclone, associated with the Asian summer monsoon and centered over the Tibetan Plateau. The anti-cyclone affects the chemical composition of the upper troposphere, where ozone concentrations of about 50 ppbv were measured, through advection of boundary layer air from South-East Asia. A layer between 4-6 km thickness was present beneath, containing up to 120 ppbv of ozone with substantial contributions by transport from the stratosphere and through lightning NOx. Additionally, pollutant ozone from North America was mixed in. Ozone in the lower troposphere originated mainly from the European continent. The stratospheric influence may be overestimated due to too strong vertical diffusion associated with the relatively coarse vertical resolution. The estimated tropospheric ozone column over the eastern Mediterranean is ~50 DU in summer, to which ozone from recent stratospheric origin contributes about 30%, ozone from lightning 13%, and from South-East Asia, North America and Europe about 7%, 8% and 14%, respectively, adding to a long-term hemispheric background of 25% of the column.