Rocket- and aircraft-borne trace gas measurements in the winter polar stratosphere

In January and February 1987 stratospheric rocket- and aircraft-borne trace gas measurements were done in the North Polar region using ACIMS (Active Chemical Ionization Mass Spectrometry) and PACIMS (PAssive Chemical Ionization Mass Spectrometry) instruments. The rocket was launched at ESRANGE (European Sounding Rocket Launching Range) (68 N, 21 E, Northern Sweden) and the twin-jet research aircraft operated by the DFVLR (Deutsche Forschungs- und Versuchs-anstalt fuer Luft- und Raumfahrt), and equipped with a mass spectrometer laboratory was stationed at Kiruna airport. Various stratospheric trace gases were measured including nitric acid, sulfuric acid, non-methane hydrocarbons (acetone, hydrogen cyanide, acetonitrile, methanol etc.), and ambient cluster ions. The experimental data is presented and possible implications for polar stratospheric ozone discussed

Distribution and origin of ozone in the eastern Mediterranean free troposphere during MINOS (August 2001)

International audienceA coupled tropospheric chemistry ? climate model is used to reproduce and analyze tropospheric ozone distributions observed during the MINOS campaign in the eastern Mediterranean region (August, 2001). Generally, regional atmospheric dynamics in summer 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 and containing up to 120 ppbv of ozone was present beneath. Ozone from stratospheric origin and from lightning NOx contributed to this layer. Additionally, pollutant ozone from North America was mixed in. Ozone in the lower troposphere originated mainly from the European continent. Modeled ozone profiles are in reasonable agreement with the observations. The stratospheric influence is sometimes overestimated by the model due to too strong vertical diffusion associated with the relatively coarse vertical resolution of the model, and specific convective events are not reproduced realistically. The modeled 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

Intercomparison of aircraft instruments on board the <i>C-130</i> and <i>Falcon 20</i> over southern Germany during EXPORT 2000

International audienceIn the summer 2000 Export aircraft campaign (European eXport of Precursors and Ozone by long-Range Transport), two comprehensively instrumented research aircraft measuring a variety of chemical species flew wing tip to wing tip for a period of one and a quarter hours. During this interval a comparison was undertaken of the measurements of nitrogen oxide (NO), odd nitrogen species (NOy), carbon monoxide (CO) and ozone (O3). The comparison was performed at two different flight levels, which provided a 10-fold variation in the concentrations of both NO (10 to 1000 parts per trillion by volume (pptv)) and NOy (200 to over 2500 pptv). Large peaks of NO and NOy observed from the Falcon 20, which were at first thought to be from the exhaust of the C-130, were also detected on the 4 channel NOx,y instrument aboard the C-130. These peaks were a good indication that both aircraft were in the same air mass and that the Falcon 20 was not in the exhaust plume of the C-130. Correlations and statistical analysis are presented between the instruments used on the two separate aircraft platforms. These were found to be in good agreement giving a high degree of correlation for the ambient air studied. Any deviations from the correlations are accounted for in the estimated inaccuracies of the instruments. These results help to establish that the instruments aboard the separate aircraft are reliably able to measure the corresponding chemical species in the range of conditions sampled and that data collected by both aircraft can be co-ordinated for purposes of interpretation

Depletion of Ozone and Reservoir Species of Chlorine and Nitrogen Oxide in the Lower Antarctic Polar Vortex Measured from Aircraft

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. ©2017. American Geophysical Union

Impact of the South Asian monsoon outflow on atmospheric hydroperoxides in the upper troposphere

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 (H$_{2}$O$_{2}$$^{obs}$) and organic hydroperoxides (ROOH$^{obs}$) as well as their precursors and loss processes. Observations are compared to photostationary-state (PSS) calculations of H$_{2}$O$_{2}$$^{PSS}$ and extended by a separation of ROOH$^{obs}$ into methyl hydroperoxide (MHP$^{PSS}$) and inferred unidentified hydroperoxide (UHP$^{PSS}$) 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 H$_{2}$O$_{2}$$^{obs}$ (45 %), MHP$^{PSS}$ (9 %), and UHPPSS (136 %) in the AMA relative to the northern hemispheric background. Highest concentrations for H$_{2}$O$_{2}$$^{obs}$ and MHP$^{PSS}$ of 211 and 152 ppb$_{V}$, respectively, were found in the tropics outside the AMA, while for UHP$^{PSS}$, with 208 ppt$_{V}$, 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 H$_{2}$O$_{2}$$^{EMAC}$ (medians: 71 ppt$_{V}$ vs. 164 ppt$_{V}$) and ROOHEMAC (medians: 25 ppt$_{V}$ vs. 278 ppt$_{V}$) mixing ratios. Longitudinal gradients indicate a pool of hydroperoxides towards the center of the AMA, most likely associated with upwind convection over India. This indicates main contributions of atmospheric transport to the local budgets of hydroperoxides along the flight track, explaining strong deviations from steady-state calculations which only account for local photochemistry. Underestimation of H$_{2}$O$_{2}$$^{EMAC}$ 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

Origin of aerosol particles in the mid-latitude and subtropical upper troposphere and lowermost stratosphere from cluster analysis of CARIBIC data

The origin of aerosol particles in the upper troposphere and lowermost stratosphere over the Eurasian continent was investigated by applying cluster analysis methods to in situ measured data. Number concentrations of submicrometer aerosol particles and trace gas mixing ratios derived by the CARIBIC (Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container) measurement system on flights between Germany and South-East Asia were used for this analysis. Four cluster analysis methods were applied to a test data set and their capability of separating the data points into scientifically reasonable clusters was assessed. The best method was applied to seasonal data subsets for summer and winter resulting in five cluster or air mass types: stratosphere, tropopause, free troposphere, high clouds, and boundary layer influenced. Other source clusters, like aircraft emissions could not be resolved in the present data set with the used methods. While the cluster separation works satisfactory well for the summer data, in winter interpretation is more difficult, which is attributed to either different vertical transport pathways or different chemical lifetimes in both seasons. The geographical distribution of the clusters together with histograms for nucleation and Aitken mode particles within each cluster are presented. Aitken mode particle number concentrations show a clear vertical gradient with the lowest values in the lowermost stratosphere (750–2820 particles/cm3 STP, minimum of the two 25% – and maximum of the two 75%-percentiles of both seasons) and the highest values for the boundary-layer-influenced air (4290–22 760 particles/cm3 STP). Nucleation mode particles are also highest in the boundary-layer-influenced air (1260–29 500 particles/cm3 STP), but are lowest in the free troposphere (0–450 particles/cm3 STP). The given submicrometer particle number concentrations represent the first large-scale seasonal data sets for the upper troposphere and lowermost stratosphere over the Eurasian continent

Aerosol-cirrus interactions: A number based phenomenon at all?

International audienceIn situ measurements of the partitioning of aerosol particles within cirrus clouds were used to investigate aerosol-cloud interactions in ice clouds. The number density of interstitial aerosol particles (non-activated particles in between the cirrus crystals) was compared to the number density of cirrus crystal residuals. The data was obtained during the two INCA (Interhemispheric Differences in Cirrus Properties form Anthropogenic Emissions) campaigns, performed in the Southern Hemisphere (SH) and Northern Hemisphere (NH) midlatitudes. Different aerosol-cirrus interactions can be linked to the different stages of the cirrus lifecycle. Cloud formation is linked to positive correlations between the number density of interstitial aerosol (Nint) and crystal residuals (Ncvi), whereas the correlations are smaller or even negative in a dissolving cloud. Unlike warm clouds, where the number density of cloud droplets is positively related to the aerosol number density, we observed a rather complex relationship when expressing Ncvi as a function of Nint for forming clouds. The data sets are similar in that they both show local maxima in the Nint range 100 to 200 cm-3, where the SH-maximum is shifted towards the higher value. For lower number densities Nint and Ncvi are positively related. The slopes emerging from the data suggest that a tenfold increase in the aerosol number density corresponds to a 3 to 4 times increase in the crystal number density. As Nint increases beyond the ca. 100 to 200 cm-3, the mean crystal number density decreases at about the same rate for both data sets. For much higher aerosol number densities, only present in the NH data set, the mean Ncvi remains low. The situation for dissolving clouds presents two alternative interactions between aerosols and cirrus. Either evaporating clouds are associated with a source of aerosol particles, or air pollution (high aerosol number density) retards evaporation rates

Transport and build-up of tropospheric trace gases during the MINOS campaign: comparision of GOME, in situ aircraft measurements and MATCH-MPIC-data

The MINOS (Mediterranean INtensive Oxidant Study) campaign was an international, multi-platform field campaign to measure long-range transport of air-pollution and aerosols from South East Asia and Europe towards the Mediterranean basin during August 2001. High pollution events were observed during this campaign. For the Mediterranean region enhanced tropospheric nitrogen dioxide (NO₂) and formaldehyde (HCHO), which are precursors of tropospheric ozone (O₃), were detected by the satellite based GOME (Global Ozone Monitoring Experiment) instrument and compared with airborne in situ measurements as well as with the output from the global 3D photochemistry-transport model MATCH-MPIC (Model of Atmospheric Transport and CHemistry - Max Planck Institute for Chemistry). The increase of pollution in that region leads to severe air quality degradation with regional and global implications