Airborne in-situ observations of ClO in the tropics were made during the TROCCINOX (Aracatuba, Brazil, February 2005) and SCOUT-O3 (Darwin, Australia, November/December 2005) field campaigns. While ...during most flights significant amounts of ClO (≈10–20 parts per trillion, ppt) were present only in aged stratospheric air, instances of enhanced ClO mixing ratios of up to 40 ppt – significantly exceeding those expected from gas phase chemistry – were observed in air masses of a more tropospheric character. Most of these observations are associated with low temperatures or with the presence of cirrus clouds (often both), suggesting that cirrus ice particles and/or liquid aerosol at low temperatures may promote significant heterogeneous chlorine activation in the tropical upper troposphere lower stratosphere (UTLS). In two case studies, particularly high levels of ClO observed were reproduced by chemistry simulations only under the assumption that significant denoxification had occurred in the observed air. However, to reproduce the ClO observations in these simulations, O3 mixing ratios higher than observed had to be assumed, and at least for one of these flights, a significant denoxification is in contrast to the observed NO levels, suggesting that the coupling of chlorine and nitrogen compounds in the tropical UTLS may not be completely understood.
Emissions from oil/gas extraction activities in the Arctic are already important in certain regions and may increase as global warming opens up new opportunities for industrial development. Emissions ...from oil/gas extraction are sources of air pollutants, but large uncertainties exist with regard to their amounts and composition. In this study, we focus on detailed investigation of emissions from oil/gas extraction in the Norwegian Sea combining measurements from the EU ACCESS aircraft campaign in July 2012 and regional chemical transport modeling. The goal is to (1) evaluate emissions from petroleum extraction activities and (2) investigate their impact on atmospheric composition over the Norwegian Sea. Numerical simulations include emissions for permanently operating offshore facilities from two datasets: the TNO-MACC inventory and emissions reported by Norwegian Environment Agency (NEA). It was necessary to additionally estimate primary aerosol emissions using reported emission factors since these emissions are not included in the inventories for our sites. Model runs with the TNO-MACC emissions are unable to reproduce observations close to the facilities. Runs using the NEA emissions more closely reproduce the observations although emissions from mobile facilities are missing from this inventory. Measured plumes suggest they are a significant source of pollutants, in particular NOx and aerosols. Sensitivities to NOx and NMVOC emissions show that, close to the platforms, O3 is sensitive to NOx emissions and is much less sensitive to NMVOC emissions. O3 destruction, via reaction with NO, dominates very close to the platforms. Far from the platforms, oil/gas facility emissions result in an average daytime O3 enhancement of +2% at the surface. Larger enhancements are predicted at noon ranging from +7% at the surface to +15% at 600 m. Black carbon is the aerosol species most strongly influenced by petroleum extraction emissions. The results highlight significant uncertainties in emissions related to petroleum extraction emissions in the Arctic.
During the TROCCINOX field experiments in February?March 2004 and February 2005, airborne in situ measurements of NO, NOy, CO, and O3 mixing ratios and the J(NO2) photolysis rate were carried out in ...the anvil outflow of thunderstorms over southern Brazil. Both tropical and subtropical thunderstorms were investigated, depending on the location of the South Atlantic convergence zone. Tropical air masses were discriminated from subtropical ones according to the higher equivalent potential temperature (?e) in the lower and mid troposphere, the higher CO mixing ratio in the mid troposphere, and the lower wind velocity in the upper troposphere within the Bolivian High (north of the subtropical jet stream). During thunderstorm anvil penetrations, typically at 20?40 km horizontal scales, NOx mixing ratios were distinctly enhanced and the absolute mixing ratios varied between 0.2?1.6 nmol mol?1 on average. This enhancement was mainly attributed to NOx production by lightning and partly due to upward transport from the NOx-richer boundary layer. In addition, CO mixing ratios were occasionally enhanced, indicating upward transport from the boundary layer. For the first time, the composition of the anvil outflow from a large, long-lived mesoscale convective system (MCS) advected from northern Argentina and Uruguay was investigated in more detail. Over a horizontal scale of about 400 km, NOx, CO and O3 absolute mixing ratios were significantly enhanced in these air masses in the range of 0.6?1.1, 110?140 and 60?70 nmol mol?1, respectively. Analyses from trace gas correlations and a Lagrangian particle dispersion model indicate that polluted air masses, probably from the Buenos Aires urban area and from biomass burning regions, were uplifted by the MCS. Ozone was distinctly enhanced in the aged MCS outflow, due to photochemical production and entrainment of O3-rich air masses from the upper troposphere ? lower stratosphere region. The aged MCS outflow was transported to the north, ascended and circulated, driven by the Bolivian High over the Amazon basin. In the observed case, the O3-rich MCS outflow remained over the continent and did not contribute to the South Atlantic ozone maximum.
The photochemical evolution of an anthropogenic plume from the New-York/Boston region during its transport at low altitudes over the North Atlantic to the European west coast has been studied using a ...Lagrangian framework. This plume, originally strongly polluted, was sampled by research aircraft just off the North American east coast on 3 successive days, and then 3 days downwind off the west coast of Ireland where another aircraft re-sampled a weakly polluted plume. Changes in trace gas concentrations during transport are reproduced using a photochemical trajectory model including deposition and mixing effects. Chemical and wet deposition processing dominated the evolution of all pollutants in the plume. The mean net photochemical O3 production is estimated to be −5 ppbv/day leading to low O3 by the time the plume reached Europe. Model runs with no wet deposition of HNO3 predicted much lower average net destruction of −1 ppbv/day O3, arising from increased levels of NOx via photolysis of HNO3. This indicates that wet deposition of HNO3 is indirectly responsible for 80% of the net destruction of ozone during plume transport. If the plume had not encountered precipitation, it would have reached Europe with O3 concentrations of up to 80 to 90 ppbv and CO between 120 and 140 ppbv. Photochemical destruction also played a more important role than mixing in the evolution of plume CO due to high levels of O3 and water vapour showing that CO cannot always be used as a tracer for polluted air masses, especially in plumes transported at low altitudes. The results also show that, in this case, an increase in O3/CO slopes can be attributed to photochemical destruction of CO and not to photochemical O3 production as is often assumed.
This paper presents results from a new method, ZooM‐CiTTy, that aims to accurately reproduce filamentation observed in profiles of chemically active species in the free troposphere. Lagrangian tracer ...reconstructions of aircraft measurements across pollutant plumes including a stochastic representation of mixing are coupled with photochemical trajectory simulations, initialized with global model fields. The results provide a high‐resolution simulation of trace gases along the flight track together with a detailed picture about the multiple air mass origins influencing chemical composition in the region where plume measurements were taken. This paper builds on results from Pisso et al. (2009) for the dynamic part of the model (the stochastic tracer reconstructions) and focuses on reconstruction of reactive species like O3. The model is evaluated for a case of long‐range transport of a forest fire plume from Alaska to Europe. Simulated trace species are compared with measurements made in the plume by the DLR Falcon aircraft flying over Europe, and the role of photochemistry in governing the chemical composition across the plume is evaluated. It is shown that the model reproduces well O3 and NOy concentrations and O3 production per CO in the plumes as well as gradients at plume edges. In particular, because ZooM‐CiTTy represents the contribution of several air masses to a measurement at a particular location, the model can reproduce so‐called mixing lines between air masses. Results show that photochemistry and mixing contributions vary in different parts of the plume and that resulting trace gas correlations are a combination of these different mixtures. One limitation of the method is the fact that mixing between air masses is only performed at the end of the trajectories. Errors on simulated O3 reconstruction from this formulation are evaluated. These errors seems to be negligible in this case (in the free troposphere, far from emission region) because strong gradients are maintained by large‐scale winds. Results from ZooM‐CiTTy are also used to evaluate errors due to nonlinearities in O3 photochemistry in coarse‐grid models. It is shown that in cases where strong gradients are maintained, errors in net O3 production can be as high as 50% at plumes edges. This new method is interesting to simulate relatively small layering structures observed in the free troposphere, but a more realistic treatment of mixing “en route” is needed if the model has to be used more extensively.
During the SCOUT-O3/ACTIVE field phase in November–December 2005, airborne in situ measurements were performed inside and in the vicinity of thunderstorms over northern Australia with several ...research aircraft (German Falcon, Russian M55 Geophysica, and British Dornier-228. Here a case study from 19 November is presented in detail on the basis of airborne trace gas measurements (NO, NOy, CO, O3) and stroke measurements from the German LIghtning Location NETwork (LINET), set up in the vicinity of Darwin during the field campaign. The anvil outflow from three different types of thunderstorms was probed by the Falcon aircraft: (1) a continental thunderstorm developing in a tropical airmass near Darwin, (2) a mesoscale convective system (MCS), known as Hector, developing within the tropical maritime continent (Tiwi Islands), and (3) a continental thunderstorm developing in a subtropical airmass ~200 km south of Darwin. For the first time detailed measurements of NO were performed in the Hector outflow. The highest NO mixing ratios were observed in Hector with peaks up to 7 nmol mol−1 in the main anvil outflow at ~11.5–12.5 km altitude. The mean NOx (=NO+NO2) mixing ratios during these penetrations (~100 km width) varied between 2.2 and 2.5 nmol mol−1. The NOx contribution from the boundary layer (BL), transported upward with the convection, to total anvil-NOx was found to be minor (<10%). On the basis of Falcon measurements, the mass flux of lightning-produced NOx (LNOx) in the well-developed Hector system was estimated to 0.6–0.7 kg(N) s−1. The highest average stroke rate of the probed thunderstorms was observed in the Hector system with 0.2 strokes s−1 (here only strokes with peak currents ≥10 kA contributing to LNOx were considered). The LNOx mass flux and the stroke rate were combined to estimate the LNOx production rate in the different thunderstorm types. For a better comparison with other studies, LINET strokes were scaled with Lightning Imaging Sensor (LIS) flashes. The LNOx production rate per LIS flash was estimated to 4.1–4.8 kg(N) for the well-developed Hector system, and to 5.4 and 1.7 kg(N) for the continental thunderstorms developing in subtropical and tropical airmasses, respectively. If we assume, that these different types of thunderstorms are typical thunderstorms globally (LIS flash rate ~44 s−1), the annual global LNOx production rate based on Hector would be ~5.7–6.6 Tg(N) a−1 and based on the continental thunderstorms developing in subtropical and tropical airmasses ~7.6 and ~2.4 Tg(N) a−1, respectively. The latter thunderstorm type produced much less LNOx per flash compared to the subtropical and Hector thunderstorms, which may be caused by the shorter mean flash component length observed in this storm. It is suggested that the vertical wind shear influences the horizontal extension of the charged layers, which seems to play an important role for the flash lengths that may originate. In addition, the horizontal dimension of the anvil outflow and the cell organisation within the thunderstorm system are probably important parameters influencing flash length and hence LNOx production per flash.
The detection of nitric acid trihydrate (NAT, HNO3×3H2O) particles in the tropical transition layer (TTL) harmonizes our understanding of polar stratospheric cloud formation. Large reactive nitrogen ...(NOy) containing particles were observed on 8 August 2006 by instruments onboard the high altitude research aircraft M55-Geophysica near and below the tropical tropopause. The particles, most likely NAT, have diameters less than 6 μm and concentrations below 10-4 cm−3. The NAT particle layer was repeatedly detected at altitudes between 15.1 and 17.5 km over extended areas of 9.5 to 17.2° N and 1.5° W to 2.7° E above the African continent. Satellite observations suggest that the NAT particles could have nucleated on ice fed by convective activity. Once nucleated, the NAT particles can slowly grow within the TTL for days, while being transported over long distances. Their in-situ detection combined with global model simulations of the NAT supersaturation near the tropical tropopause indicate the potential for a tropical tropopause NAT particle belt.
The Atmospheric Radionuclide Transport Model (ARTM) operates at the meso-γ scale and simulates the dispersion of radionuclides originating from nuclear facilities under routine operation within the ...planetary boundary layer. This study presents the extension and validation of this Lagrangian particle dispersion model and consists of three parts: (i) a sensitivity study that aims to assess the impact of key input parameters on the simulation results, (ii) the evaluation of the mixing properties of five different turbulence models using the well-mixed criterion, and (iii) a comparison of model results to airborne observations of carbon dioxide (CO2) emissions from a power plant and the evaluation of related uncertainties. In the sensitivity study, we analyse the effects of the stability class, roughness length, zero-plane displacement factor, and source height on the three-dimensional plume extent as well as the distance between the source and maximum concentration at the ground. The results show that the stability class is the most sensitive input parameter as expected. The five turbulence models are the default turbulence models of ARTM 2.8.0 and ARTM 3.0.0, one alternative built-in turbulence model of ARTM, and two further turbulence models implemented for this study. The well-mixed condition tests showed that all five turbulence models are able to preserve an initially well-mixed atmospheric boundary layer reasonably well. The models deviate only 6 % from the expected uniform concentration below 80 % of the mixing layer height, except for the default turbulence model of ARTM 3.0.0 with deviations of up to 18 %. CO2 observations along a flight path in the vicinity of the lignite power plant Bełchatów, Poland, measured by the Deutsches Zentrum für Luft- und Raumfahrt (DLR) Cessna aircraft during the Carbon Dioxide and Methane Mission (CoMet) campaign in 2018 allowed for evaluation of model performance for the different turbulence models under unstable boundary layer conditions. All simulated mixing ratios are of the same order of magnitude as the airborne in situ data. An extensive uncertainty analysis using probability distribution functions, statistical tests, and direct spatio-temporal comparisons of measurements and model results help to quantify the model uncertainties. With the default turbulence setups of ARTM versions 2.8.0 and 3.0.0, the plume widths are underestimated by up to 50 %, resulting in a strong overestimation of the maximum plume CO2 mixing ratios. The comparison of the three alternative turbulence models shows good agreement of the peak plume CO2 concentrations, the CO2 distribution within the plumes, and the plume width, with a 30 % deviation in the peak CO2 concentration and a less than 25 % deviation in the measured CO2 plume width. Uncertainties in the simulations may arise from the different spatial and temporal resolutions of simulations and measurements in addition to the turbulence parametrisation and boundary conditions. The results of this work may help to improve the accurate representation of real plumes in very unstable atmospheric conditions through the selection of distinct turbulence models. Further comparisons at different stability regimes are required for a final assessment of model uncertainties.
The retrieval of turbulence parameters with profiling Doppler wind lidars (DWLs) is of high interest for boundary layer meteorology and its applications. DWLs provide wind measurements above the ...level of meteorological masts while being easier and less expensive to deploy. Velocity-azimuth display (VAD) scans can be used to retrieve the turbulence kinetic energy (TKE) dissipation rate through a fit of measured azimuth structure functions to a theoretical model. At the elevation angle of 35.3∘ it is also possible to derive TKE. Modifications to existing retrieval methods are introduced in this study to reduce errors due to advection and enable retrievals with a low number of scans. Data from two experiments are utilized for validation: first, measurements at the Meteorological Observatory Lindenberg–Richard-Aßmann Observatory (MOL-RAO) are used for the validation of the DWL retrieval with sonic anemometers on a meteorological mast. Second, distributed measurements of three DWLs during the CoMet campaign with two different elevation angles are analyzed. For the first time, the ground-based DWL VAD retrievals of TKE and its dissipation rate are compared to in situ measurements of a research aircraft (here: DLR Cessna Grand Caravan 208B), which allows for measurements of turbulence above the altitudes that are in range for sonic anemometers. From the validation against the sonic anemometers we confirm that lidar measurements can be significantly improved by the introduction of the volume-averaging effect into the retrieval. We introduce a correction for advection in the retrieval that only shows minor reductions in the TKE error for 35.3∘ VAD scans. A significant bias reduction can be achieved with this advection correction for the TKE dissipation rate retrieval from 75∘ VAD scans at the lowest measurement heights. Successive scans at 35.3 and 75∘ from the CoMet campaign are shown to provide TKE dissipation rates with a good correlation of R>0.8 if all corrections are applied. The validation against the research aircraft encourages more targeted validation experiments to better understand and quantify the underestimation of lidar measurements in low-turbulence regimes and altitudes above tower heights.
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