Trapping, chemistry, and export of trace gases in the South Asian summer monsoon observed during CARIBIC flights in 2008

The CARIBIC (Civil Aircraft for the Regular Investigation of the Atmosphere Based on an Instrument Container) passenger aircraft observatory performed in situ measurements at 10–12 km altitude in the South Asian summer monsoon anticyclone between June and September 2008. These measurements enable us to investigate this atmospheric region (which so far has mostly been observed from satellites) using the broad suite of trace gases and aerosol particles measured by CARIBIC. Elevated levels of a variety of atmospheric pollutants (e.g. carbon monoxide, total reactive nitrogen oxides, aerosol particles, and several volatile organic compounds) were recorded. The measurements provide detailed information about the chemical composition of air in different parts of the monsoon anticyclone, particularly of ozone precursors. While covering a range of 3500 km inside the monsoon anticyclone, CARIBIC observations show remarkable consistency, i.e. with distinct latitudinal patterns of trace gases during the entire monsoon period. Using the CARIBIC trace gas and aerosol particle measurements in combination with the Lagrangian particle dispersion model FLEXPART, we investigated the characteristics of monsoon outflow and the chemical evolution of air masses during transport. The trajectory calculations indicate that these air masses originated mainly from South Asia and mainland Southeast Asia. Estimated photochemical ages of the air were found to agree well with transport times from a source region east of 90–95° E. The photochemical ages of the air in the southern part of the monsoon anticyclone were systematically younger (less than 7 days) and the air masses were mostly in an ozone-forming chemical mode. In its northern part the air masses were older (up to 13 days) and had unclear ozone formation or destruction potential. Based on analysis of forward trajectories, several receptor regions were identified. In addition to predominantly westward transport, we found evidence for efficient transport (within 10 days) to the Pacific and North America, particularly during June and September, and also of cross-tropopause exchange, which was strongest during June and July. Westward transport to Africa and further to the Mediterranean was the main pathway during July

Overview: On the transport and transformation of pollutants in the outflow of major population centres – observational data from the EMeRGe European intensive operational period in summer 2017

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

Stickoxidmessungen in der Tropopausenregion an Bord eines Linienflugzeugs: Großräumige Verteilung und Einfluss des Luftverkehrs

Als Vorläufergase von Ozon nehmen Stickoxide eine zentrale Rolle in der Atmosphärenchemie ein. Die großräumige Verteilung von Stickoxiden in der UTLS ist jedoch noch nicht hinreichend bekannt. In dieser Arbeit wurde die Verteilung von NO und NOy anhand von Stickoxidmessungen, die an Bord eines Linienflugzeugs durchgeführt werden, untersucht. Die NOy sowie die NO Mischungsverhältnisse zeigen klare saisonale und regionale Abhängigkeiten. Der Einfluss des Flugverkehrs auf die Stickoxide wird abgeschätzt. Ferner wurde das Messinstrument um einen NO2 Konverter erweitert

Nitrogen Oxides and Reactive Nitrogen in the UTLS: Long Term Observations from CARIBIC

Nitrogen oxides measurements in the UTLS region within the CARIBIC project

Experimental determination of the temperature dependence of water activities for a selection of aqueous organic solutions

This work presents experimental data of the temperature dependence of water activity in aqueous organic solutions relevant for tropospheric conditions (200–273 K). Water activity (aw) at low temperatures (T) is a crucial parameter for predicting homogeneous ice nucleation. We investigated temperature-dependent water activities, ice freezing and melting temperatures of solutions, and vapour pressures of a selection of atmospherically relevant aqueous organic systems. To measure aw over a wide composition range and with a focus on low temperatures, we use various aw measurement techniques and instruments: a dew point water activity meter, an electrodynamic balance (EDB), differential scanning calorimetry (DSC), and a setup to measure the total gas phase pressure at equilibrium over aqueous solutions. Water activity measurements were performed for aqueous multicomponent and multifunctional organic mixtures containing the functional groups typically found in atmospheric organic aerosols, such as hydroxyl, carboxyl, ketone, ether, ester, and aromatic groups. The aqueous organic systems studied at several fixed compositions over a considerable temperature range differ significantly in their temperature dependence. Aqueous organic systems of 1,4-butanediol and methoxyacetic acid show a moderate decrease in aw with decreasing temperature. The aqueous M5 system (a multicomponent system containing five different dicarboxylic acids) and aqueous 2-(2-ethoxyethoxy)ethanol solutions both show a strong increase of water activity with decreasing temperature at high solute concentrations for T < 270 K and T < 260 K, respectively. These measurements show that the temperature trend of aw can be reversed at low temperatures and that linear extrapolations of high-temperature data may lead to erroneous predictions. To avoid this, experimentally determined aw at low temperature are needed to improve thermodynamic models towards lower temperatures and for improved predictions of the ice nucleation ability of organic–water systems

Impact of acetone (photo)oxidation on HOx production in the UT/LMS based on CARIBIC passenger aircraft observations and EMAC simulations

Impact of acetone (photo)oxidation on HOx production in the UT/LMS based on CARIBIC passenger aircraft observations and EMAC simulation

Trace gas profiles and anthropogenic plumes from metropolitan areas in West Africa during DACCIWA - Airborne measurements on board the DLR Falcon 20

International audienceThe DACCIWA (Dynamics-Aerosol-Chemistry-Cloud Interactions over West Africa) airborne field campaign was conducted in Southern West Africa in June/July 2016. The atmosphere in South West Africa is exposed to numerous influences like the Monsoon, biomass burning and oil rigs. Its chemical composition is modified by urbanisation, a growing population, complex meteorological influences and air pollution. During DACCIWA, three European research aircraft (DLR - Falcon 20, SAFIRE - ATR 42 and BAS - Twin Otter) were deployed from Lomé/Togo and conducted research flights across Ivory Coast, Ghana, Togo and Benin. On board the DLR Falcon O3, SO2, CO, NO2 and aerosol fine mode particle number concentration and size distribution were measured during a total of 12 scientific flights. Distinct trace gas layers were found during vertical soundings. An O3 layer at 3000 m altitude was observed during 6 flights with concentrations up to 85 ppb compared to background concentrations of about 35 ppb due to southern hemispheric biomass burning products which were transported to the DACCIWA study area. Furthermore, enhanced trace gas and particle number concentrations were detected in city pollution plumes of Lomé/Togo, Accra/Ghana and Kumasi/Ghana. O3 enhancements of 5 - 10 ppb were measured downstream of the cities relative to the upstream observations. Measured SO2 pollution plumes with concentrations up to 0.9 ppb near Lomé are combined with HYPSLIT dispersion simulations and are compared to emission databases