Airborne glyoxal measurements in the marine and continental atmosphere: comparison with TROPOMI observations and EMAC simulations

We report on airborne limb and nadir measurements of vertical profiles and total vertical column densities (VCDs) of glyoxal (C2H2O2) in the troposphere, which were performed aboard the German research aircraft HALO (High Altitude and LOng Range) in different regions and seasons around the globe between 2014 and 2019. The airborne nadir and integrated limb profiles agree excellently among each other. Our airborne observations are further compared to collocated glyoxal measurements of the TROPOspheric Monitoring Instrument (TROPOMI), with good agreement between both data sets for glyoxal observations in (1) pristine terrestrial, (2) pristine marine, (3) mixed polluted, and (4) biomass-burning-affected air masses with high glyoxal concentrations. Exceptions to the overall good agreement are observations of (1) faint and aged biomass burning plumes over the oceans and (2) of low-lying biomass burning or anthropogenic plumes in the terrestrial or marine boundary layer, both of which contain elevated glyoxal that is mostly not captured by TROPOMI. These differences in airborne and satellite-detected glyoxal are most likely caused by the overall small contribution of plumes of a limited extent to the total glyoxal absorption in the atmosphere and the difficulty in remotely detecting weak absorbers located close to low reflective surfaces (e.g. the ocean in the visible wavelength range) or within dense aerosol layers. Observations of glyoxal in aged biomass burning plumes (e.g. observed over the tropical Atlantic off the coast of West Africa in summer 2018, off the coast of Brazil by the end of the dry season 2019, and the East China Sea in spring 2018) could be traced back to related wildfires, such as a plume crossing over the Drake Passage that originated from the Australian bushfires in late 2019. Our observations of glyoxal in such aged biomass burning plumes confirm recent findings of enhanced glyoxal and presumably secondary organic aerosol (SOA) formation in aged wildfire plumes from yet-to-be-identified, longer-lived organic precursor molecules (e.g. aromatics, acetylene, or aliphatic compounds) co-emitted in the fires. Furthermore, elevated glyoxal (median 44 ppt – parts per trillion), as compared to other marine regions (median 10–19 ppt), is observed in the boundary layer over the tropical oceans, which is well in agreement with previous reports. The airborne data sets are further compared to glyoxal simulations performed with the global atmosphere chemistry model EMAC (ECHAM/MESSy Atmospheric Chemistry). When using an EMAC set up that resembles recent EMAC studies focusing on complex chemistry, reasonable agreement is found for pristine air masses (e.g. the unperturbed free and upper troposphere), but a notable glyoxal overestimation of the model exists for regions with high emissions of glyoxal and glyoxal-producing volatile organic compounds (VOCs) from the biosphere (e.g. the Amazon). In all other investigated regions, the model underpredicts glyoxal to varying degrees, in particular when probing mixed emissions from anthropogenic activities (e.g. over continental Europe, the Mediterranean, and East China Sea) and potentially from the sea (e.g. the tropical oceans). Also, the model tends to largely underpredict glyoxal in city plumes and aged biomass burning plumes. The potential causes for these differences are likely to be multifaceted, but they all point to missing glyoxal sources from the degradation of the mixture of potentially longer-chained organic compounds emitted from anthropogenic activities, biomass burning, and from the organic microlayer of the sea surface.</p

Oxidation of low-molecular weight organic compounds in cloud droplets: development of the JAMOC chemical mechanism in CAABA/MECCA (version 4.5.0gmdd)

The Jülich Aqueous-phase Mechanism of Organic Chemistry (JAMOC) is developed and implemented in the Module Efficiently Calculating the Chemistry of the Atmosphere (MECCA, version 4.5.0gmdd1). JAMOC is an explicit in-cloud oxidation scheme for oxygenated volatile organic compounds (OVOCs), suitable for global model applications. It is based on a subset of the comprehensive CLoud Explicit Physico-chemical Scheme (CLEPS, version 1.0). The phase transfer of species containing up to ten carbon atoms is included, and a selection of species containing up to four carbon atoms reacts in the aqueous-phase. In addition, the following main advances are implemented: (1) simulating hydration and dehydration explicitly, (2) taking oligomerisation of formaldehyde, glyoxal and methylglyoxal into account, (3) adding further photolysis reactions, and (4) considering gas-phase oxidation of new outgassed species. The implementation of JAMOC in MECCA makes a detailed in-cloud OVOC oxidation model readily available for box as well as for regional and global simulations that are affordable with modern supercomputing facilities. The new mechanism is tested inside the box-model Chemistry As A Boxmodel Application (CAABA), yielding reduced gas-phase concentrations of most oxidants and OVOCs except for the nitrogen oxides

Influence of weather situation on non-CO₂ aviation climate effects: the REACT4C climate change functions

Emissions of aviation include CO2, H2O, NOx, sulfur oxides, and soot. Many studies have investigated the annual mean climate impact of aviation emissions. While CO2 has a long atmospheric residence time and is almost uniformly distributed in the atmosphere, non-CO2 gases and particles and their products have short atmospheric residence times and are heterogeneously distributed. The climate impact of non-CO2 aviation emissions is known to vary with different meteorological background situations. The aim of this study is to systematically investigate the influence of characteristic weather situations on aviation climate effects over the North Atlantic region, to identify the most sensitive areas, and to potentially detect systematic weather-related similarities. If aircraft were re-routed to avoid climate-sensitive regions, the overall aviation climate impact might be reduced. Hence, the sensitivity of the atmosphere to local emissions provides a basis for the assessment of weather-related, climate-optimized flight trajectory planning. To determine the climate change contribution of an individual emission as a function of location, time, and weather situation, the radiative impact of local emissions of NOx and H2O to changes in O3, CH4, H2O and contrail cirrus was computed by means of the ECHAM5/MESSy Atmospheric Chemistry model. From this, 4-dimensional climate change functions (CCFs) were derived. Typical weather situations in the North Atlantic region were considered for winter and summer. Weather-related differences in O3, CH4, H2O, and contrail cirrus CCFs were investigated. The following characteristics were identified: enhanced climate impact of contrail cirrus was detected for emissions in areas with large-scale lifting, whereas low climate impact of contrail cirrus was found in the area of the jet stream. Northwards of 60∘ N, contrails usually cause climate warming in winter, independent of the weather situation. NOx emissions cause a high positive climate impact if released in the area of the jet stream or in high-pressure ridges, which induces a south- and downward transport of the emitted species, whereas NOx emissions at, or transported towards, high latitudes cause low or even negative climate impact. Independent of the weather situation, total NOx effects show a minimum at ∼250 hPa, increasing towards higher and lower altitudes, with generally higher positive impact in summer than in winter. H2O emissions induce a high climate impact when released in regions with lower tropopause height, whereas low climate impact occurs for emissions in areas with higher tropopause height. H2O CCFs generally increase with height and are larger in winter than in summer. The CCFs of all individual species can be combined, facilitating the assessment of total climate impact of aircraft trajectories considering CO2 and spatially and temporally varying non-CO2 effects. Furthermore, they allow for the optimization of aircraft trajectories with reduced overall climate impact. This also facilitates a fair evaluation of trade-offs between individual species. In most regions, NOx and contrail cirrus dominate the sensitivity to local aviation emissions. The findings of this study recommend considering weather-related differences for flight trajectory optimization in favour of reducing total climate impact

Influence of the actual weather situation on non-CO2 aviation climate effects: The REACT4C Climate Change Functions

The influence of different weather situations on non-CO2 aviation climate impact is investigated. The aim is to identify systematic weather related sensitivities. If aircraft trajectories avoid the most sensitive areas, the overall climate impact might be reduced. An enhanced significance of the position of emission release is identified in relation to high pressure systems, in relation to the jet stream, in relation to polar night, and in relation to the altitude of the tropopause. The results of this study represent a comprehensive dataset for studies aiming at weather dependent flight trajectory optimization reducing total climate impact

Assessing the climate impact of formation flights

Emissions of aviation include CO2, H2O, NOx and particles. While CO2 has a long atmospheric residence time and is uniformly distributed in the atmosphere, non-CO2 gases, particles and their products have short atmospheric residence times and are heterogeneously distributed. Their climate effects depend on chemical and meteorological background conditions during emission, which vary with geographic location, altitude, time, local insolation, actual weather, etc. This spatial and temporal variability can be utilized for aviation climate impact mitigation by identifying aircraft trajectories which avoid climate-sensitive regions. To determine the climate change contribution of individual emissions as function of 3-dimensional position, time and weather situation, contributions of local emissions to changes in O3, CH4, H2O and contrail-cirrus were computed by means of the ECHAM5/MESSy Atmospheric Chemistry model and four-dimensional climate change functions (CCFs) were derived thereof. Typical weather situations in the North Atlantic region were considered for winter and summer. For all non-CO2 species included in the study, we found distinct weather related differences with respect to their climate impact. Depending on the species, we found enhanced significance of the position of emission release in relation to high pressure systems, in relation to the jet stream, in relation to polar night and in relation to the tropopause altitude. The dominating parameters were found to be contrail-cirrus and total NOx. The results of this study represent a comprehensive basis for weather dependent flight trajectory optimization studies. Furthermore it constitutes the groundwork for the development of more generally applicable algorithmic CCFs.Aircraft Noise and Climate Effect

Mitigating the Climate Impact from Aviation: Achievements and Results of the DLR WeCare Project

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.Aircraft Noise and Climate Effect

Ubiquitous atmospheric production of organic acids mediated by cloud droplets

International audienceAtmospheric acidity is increasingly determined by carbon dioxide and organic acids1–3. Among the latter, formic acid facilitates the nucleation of cloud droplets4 and contributes to the acidity of clouds and rainwater1,5. At present, chemistry–climate models greatly underestimate the atmospheric burden of formic acid, because key processes related to its sources and sinks remain poorly understood2,6–9. Here we present atmospheric chamber experiments that show that formaldehyde is e ciently converted to gaseous formic acid via a multiphase pathway that involves its hydrated form, methanediol. In warm cloud droplets, methanediol undergoes fast outgassing but slow dehydration. Using a chemistry–climate model, we estimate that the gas-phase oxidation of methanediol produces up to four times more formic acid than all other known chemical sources combined. Our ndings reconcile model predictions and measurements of formic acid abundance. The additional formic acid burden increases atmospheric acidity by reducing the pH of clouds and rainwater by up to 0.3. The diol mechanism presented here probably applies to other aldehydes and may help to explain the high atmospheric levels of other organic acids that a ect aerosol growth and cloud evolution