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The impact of monsoon outflow from India and Southeast Asia in the upper troposphere over the eastern Mediterranean

A major objective of the Mediterranean INtensive Oxidant Study (MINOS) was to investigate long-range transport of pollutants (notably ozone precursor species). Here we present trace gas measurements from the DLR (German Aerospace Organization) Falcon aircraft in the eastern Mediterranean troposphere. Ten day backward trajectories and a coupled chemistry-climate model (ECHAM4) were used to study the nature and origin of pollution observed in the upper troposphere between 6 and 13 km altitude. We focus on a large pollution plume encountered over the eastern Mediterranean between 1 and 12 August originating in South Asia (India and Southeast Asia), referred to as the Asian plume, associated with the Asian Summer Monsoon. Vertical as well as longitudinal gradients of methane, carbon monoxide, hydrocarbons including acetone, methanol, and acetonitrile, halocarbons, ozone and total reactive nitrogen (NOy) are presented, showing the chemical impact of the Asian plume compared to westerly air masses containing pollution from North America. The Asian plume is characterized by enhanced concentrations of biomass burning tracers (acetylene, methyl chloride, acetonitrile), notably from biofuel use. Concentrations of the new automobile cooling agent HFC-134a were significantly lower in the Asian plume than in air masses from North America. Relatively high levels of ozone precursors (CO, hydrocarbons) were found in both air masses, whereas lower ozone concentrations in the Asian plume suggest NOx-limited conditions. Consistently, ECHAM model simulations indicate that the expected future increase of NOx-emissions in Asia enhances the photochemical ozone production in the Asian plume. The size and location of the Asian plume near the tropopause provides an important potential for pollution transport into the lowermost stratosphere. We present observations indicative of Asian pollution transport into the lower stratosphere.
Evidence of impact of aviation on cirrus cloud formation

This work examines changes in cirrus cloud cover (CCC) in possible association with aviation activities at congested air corridors. The analysis is based on the latest version of the International Satellite Cloud Climatology Project D2 data set and covers the period 1984-1998. Over the studied areas, the effect of large-scale modes of natural climate variability such as ENSO, QBO and NAO as well as the possible influence of the tropopause variability, were first removed from the cloud data set in order to calculate long-term changes of observed cirrus cloudiness. The results show increasing trends in (CCC) between 1984 and 1998 over the high air traffic corridors of North America, North Atlantic and Europe. Of these upward trends, only in the summertime over the North Atlantic and only in the wintertime over North America are statistically significant (exceeding +2.0% per decade). Over adjacent locations with low air traffic, the calculated trends are statistically insignificant and in most cases negative both during winter and summer in the regions studied. These negative trends, over low air traffic regions, are consistent with the observed large scale negative trends seen in (CCC) over most of the northern middle latitudes and over the tropics. Moreover, further investigation of vertical velocities over high and low air traffic regions provide evidence that the trends of opposite signs in (CCC) over these regions, do not seem to be caused by different trends in dynamics. It is also shown that the longitudinal distribution of decadal changes in (CCC) along the latitude belt centered at the North Atlantic air corridor, parallels the spatial distribution of fuel consumption from highflying air traffic, providing an independent test of possible impact of aviation on contrail cirrus formation. The correlation between the fuel consumption and the longitudinal variability of (CCC) is significant (+0.7) over the middle latitudes but not over the tropics. This could be explained by the fact that over the tropics the variability of (CCC) is dominated by dynamics while at middle latitudes microphysics explain most of its variability. Results from this study are compared with other studies and for different periods of records and it appears that there exists general agreement as to the evidence of a possible aviation effect on high cloud positive trends over regions with congested air traffic.
An evaluation of the performance of chemistry transport models by comparison with research aircraft observations. Part 1: Concepts and overall model performance

A rigorous evaluation of five global Chemistry-Transport and two Chemistry-Climate Models operated by several different groups in Europe, was performed. Comparisons were made of the models with trace gas observations from a number of research aircraft measurement campaigns during the four-year period 1995-1998. Whenever possible the models were run over the same four-year period and at each simulation time step the instantaneous tracer fields were interpolated to all coinciding observation points. This approach allows for a very close comparison with observations and fully accounts for the specific meteorological conditions during the measurement flights. This is important considering the often limited availability and representativity of such trace gas measurements. A new extensive database including all major research and commercial aircraft measurements between 1995 and 1998, as well as ozone soundings, was established specifically to support this type of direct comparison. Quantitative methods were applied to judge model performance including the calculation of average concentration biases and the visualization of correlations and RMS errors in the form of so-called Taylor diagrams. We present the general concepts applied, the structure and content of the database, and an overall analysis of model skills over four distinct regions. These regions were selected to represent various atmospheric conditions and to cover large geographical domains such that sufficient observations are available for comparison. The comparison of model results with the observations revealed specific problems for each individual model. This study suggests the further improvements needed and serves as a benchmark for re-evaluations of such improvements. In general all models show deficiencies with respect to both mean concentrations and vertical gradients of important trace gases. These include ozone, CO and NOx at the tropopause. Too strong two-way mixing across the tropopause is suggested to be the main reason for differences between simulated and observed CO and ozone values. The generally poor correlations between simulated and measured NOx values suggest that in particular the NOx input by lightning and the convective transport from the polluted boundary layer are still not well described by current parameterizations, which may lead to significant differences in the spatial and seasonal distribution of NOx in the models. Simulated OH concentrations, on the other hand, were found to be in surprisingly good agreement with measured values.
Simulating gas-aerosol-cirrus interactions: Process-oriented microphysical model and applications

This work describes a process-oriented, microphysical-chemical model to simulate the formation and evolution of aerosols and ice crystals under the conditions prevailing in the upper troposphere and lower stratosphere. The model can be run as a box model or along atmospheric trajectories, and considers mixing, gas phase chemistry of aerosol precursors, binary homogeneous aerosol nucleation, homogeneous and heterogeneous ice nucleation, coagulation, condensation and dissolution, gas retention during particle freezing, gas trapping in growing ice crystals, and reverse processes. Chemical equations are solved iteratively using a second order implicit integration method. Gas-particle interactions and coagulation are treated over various size structures, with fully mass conserving and non-iterative numerical solution schemes. Particle types include quinternary aqueous solutions composed of H2SO4, HNO3, HCl, and HBr with and without insoluble components, insoluble aerosol particles, and spherical or columnar ice crystals deriving from each aerosol type separately. Three case studies are discussed in detail to demonstrate the potential of the model to simulate real atmospheric processes and to highlight current research topics concerning aerosol and cirrus formation near the tropopause. Emphasis is placed on how the formation of cirrus clouds and the scavenging of nitric acid in cirrus depends on small-scale temperature fluctuations and the presence of efficient ice nuclei in the tropopause region, corroborating and partly extending the findings of previous studies.
Preindustrial-to-present-day radiative forcing by tropospheric ozone from improved simulations with the GISS chemistry-climate GCM

Improved estimates of the radiative forcing from tropospheric ozone increases since the preindustrial have been calculated with the tropospheric chemistry model used at the Goddard Institute for Space Studies (GISS) within the GISS general circulation model (GCM). The chemistry in this model has been expanded to include simplified representations of peroxyacetylnitrates and non-methane hydrocarbons in addition to background NOx-HOx-Ox-CO-CH4 chemistry. The GCM has improved resolution and physics in the boundary layer, improved resolution near the tropopause, and now contains a full representation of stratospheric dynamics. Simulations of present-day conditions show that this coupled chemistry-climate model is better able to reproduce observed tropospheric ozone, especially in the tropopause region, which is critical to climate forcing. Comparison with preindustrial simulations gives a global annual average radiative forcing due to tropospheric ozone increases of 0.30 W/m2 with standard assumptions for preindustrial emissions. Locally, the forcing reaches more than 0.8 W/m2 in parts of the northern subtropics during spring and summer, and is more than 0.6 W/m2 through nearly all the Northern subtropics and mid-latitudes during summer. An alternative preindustrial simulation with soil NOx emissions reduced by two-thirds and emissions of isoprene, paraffins and alkenes from vegetation increased by 50% gives a forcing of 0.33 W/m2. Given the large uncertainties in preindustrial ozone amounts, the true value may lie well outside this range.
Effect of water addition and nitrogen fertilization on the fluxes of CH4, CO2, NOx, and N2O following five years of elevated CO2 in the Colorado Shortgrass Steppe

An open-top-chamber (OTC) CO2 enrichment (~720 mmol mol-1) study was conducted in the Colorado shortgrass steppe from April 1997 through October 2001. Aboveground plant biomass increased under elevated CO2 and soil moisture content was typically higher than under ambient CO2 conditions. Fluxes of CH4, CO2, NOx and N2O, measured weekly year round were not significantly altered by CO2 enrichment over the 55 month period of observation. During early summer of 2002, following the removal of the open-top-chambers from the CO2 enrichment sites in October 2001, we conducted a short term study to determine if soil microbial processes were altered in soils that had been exposed to double ambient CO2 concentrations during the growing season for the past five years. Microplots were established within each experimental site and 10 mm of water or 10 mm of water containing the equivalent of 10 g m-2 of ammonium nitrate-N was applied to the soil surface. Fluxes of CO2, CH4, NOx and N2O fluxes within control (unchambered), ambient CO2 and elevated CO2 OTC soils were measured at one to three day intervals for the next month. With water addition alone, CO2 and NO emission did not differ between ambient and elevated CO2 soils, while CH4 uptake rates were higher and N2O fluxes lower in elevated CO2 soils. Adding water and mineral N resulted in increased CO2 emissions, increased CH4 uptake and decreased NO emissions in elevated CO2 soils. The N addition study confirmed previous observations that soil respiration is enhanced under elevated CO2 and N immobilization is increased, thereby decreasing NO emission.
On the relationship between acetone and carbon monoxide in different air masses

Carbon monoxide and acetone measurements are presented for five aircraft measurement campaigns at mid-latitudes, polar and tropical regions in the northern hemisphere. Throughout all campaigns, free tropospheric air masses, which were influenced by anthropogenic emissions, showed a similar linear relation between acetone and CO, with a slope of 21-25 pptv acetone/ppbv CO. Measurements in the anthropogenically influenced marine boundary layer revealed a slope of 13-16 pptv acetone/ppbv CO. The different slopes observed in the marine boundary layer and the free troposphere indicate that acetone is emitted by the ocean in relatively clean air masses and taken up by the ocean in polluted air masses. In the lowermost stratosphere, a good correlation between acetone and CO was observed as well, however, with a much smaller slope (~5 pptv acetone/ppbv CO) compared to the troposphere. This is caused by the longer photochemical lifetime of CO compared to acetone in the lower stratosphere, due to the increasing photolytic loss of acetone and the decreasing OH concentration with altitude. No significant correlation between acetone and CO was observed over the tropical rain forest due to the large direct and indirect biogenic emissions of acetone. The common slopes of the linear acetone-CO relation in various layers of the atmosphere, during five field experiments, makes them useful for model calculations. Often a single observation of the acetone-CO correlation, determined from stratospheric measurements, has been used in box model applications. This study shows that different slopes have to be considered for marine boundary layer, free tropospheric and stratospheric air masses, and that the acetone-CO relation cannot be used for air masses which are strongly influenced by biogenic emissions.
On the accuracy of analysed low temperatures in the stratosphere

The accuracy of ECMWF (European Centre for Medium-Range Weather Forecasts) temperatures has been investigated by comparison to radiosonde temperatures. Particularly, the extent of temperatures below which Polar Stratospheric Clouds (PSCs) consisting of nitric acid trihydrate can exist (TNAT) has been studied. In the 1999/2000 winter analyses and in the 40 year reanalyses (ERA40) from the winter 1996/1997 the analysed extent agrees quite well with the radiosondes extent, whereas the 2002/2003 winter analyses considerably overestimate the extent from 40-11 hPa due to a general cold bias. Close to the frost point small-scale temperature variations, which ECMWF does not catch, substantially increase the extent of these low temperatures. Some of these small-scale variations are caused by lee-waves.
Assessment of possible airborne impact from nuclear risk sites – Part II: probabilistic analysis of atmospheric transport patterns in Euro-Arctic region

The probabilistic analysis of atmospheric transport patterns from most important nuclear risk sites in the Euro-Arctic region is performed employing the methodology developed within the "Arctic Risk" Project of the NARP Programme (Baklanov and Mahura, 2003). The risk sites are the nuclear power plants in the Northwest Russia, Finland, Sweden, Lithuania, United Kingdom, and Germany as well as the Novaya Zemlya test site of Russia. The geographical regions of interest are the Northern and Central European countries and Northwest Russia. In this study, the employed research tools are the trajectory model to calculate a multiyear dataset of forward trajectories that originated over the risk site locations, and a set of statistical methods (including exploratory, cluster, and probability fields analyses) for analysis of trajectory modelling results. The probabilistic analyses of trajectory modelling results for eleven sites are presented as a set of various indicators of the risk sites possible impact on geographical regions and countries of interest. The nuclear risk site possible impact (on a particular geographical region, territory, country, site, etc.) due to atmospheric transport from the site after hypothetical accidental release of radioactivity can be properly estimated based on a combined interpretation of the indicators (simple characteristics, atmospheric transport pathways, airflow and fast transport probability fields, maximum reaching distance and maximum possible impact zone, typical transport time and precipitation factor fields) for different time periods (annual, seasonal, and monthly) for any selected site (both separately for each site or grouped for several sites) in the Euro-Arctic region. Such estimation could be the useful input information for the decision-making process, risk assessment, and planning of emergency response systems for sites of nuclear, chemical, and biological danger.
The North Atlantic Oscillation controls air pollution transport to the Arctic

This paper studies the interannual variability of pollution pathways from northern hemisphere (NH) continents into the Arctic. Using a 15-year model simulation of the dispersion of passive tracers representative of anthropogenic emissions from NH continents, we show that the North Atlantic Oscillation (NAO) exerts a strong control on the pollution transport into the Arctic, particularly in winter and spring. For tracer lifetimes of 5 (30) days, surface concentrations in the Arctic winter are enhanced by about 70% (30%) during high phases of the NAO (in the following referred to as NAO+) compared to its low phases (NAO-). This is mainly due to great differences in the pathways of European pollution during NAO+ and NAO- phases, respectively, but reinforced by North American pollution, which is also enhanced in the Arctic during NAO+ phases. In contrast, Asian pollution in the Arctic does not significantly depend on the NAO phase. The model results are confirmed using remotely-sensed NO2 vertical atmospheric columns obtained from seven years of satellite measurements, which show enhanced northward NO2 transport and reduced NO2 outflow into the North Atlantic from Central Europe during NAO+ phases. Surface measurements of carbon monoxide (CO) and black carbon at high-latitude stations further corroborate the overall picture of enhanced Arctic pollution levels during NAO+ phases