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  • 1
    Electronic Resource
    Electronic Resource
    Springer
    Journal of atmospheric chemistry 28 (1997), S. 319-337 
    ISSN: 1573-0662
    Keywords: convection ; free troposphere ; ozone ; oxides of nitrogen ; three-dimensional model
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract The fluxes of ozone and NOx out of the atmospheric boundary layer (ABL) over Europe are calculated in a mesoscale chemical transport model (MCT) and compared with the net chemical production or destruction of ozone and the emissions of precursors within the ABL for two 10 days' periods which had quite different synoptic situations and levels of photochemical activity (1–10 July 1991 (JUL91) and 26 October–4 November 1994 (ON94)). Over the European continent, about 8% of the NOx emissions were brought from the ABL to the free troposphere as NOx, while about 15% of the NOx emissions were brought to the free troposphere as NOy–NOx, i.e. as PAN or HNO3. The convection dominates over the synoptic scale vertical advection as a transport mechanism both for NOx and NOy out of the boundary layer in the summertime high pressure situation (JUL91), while in the fall situation (ON94) the convective part was calculated to be the smallest. NOx was almost completely transformed to NOy–NOx or removed within the ABL. Also for NOy the major part of the atmospheric cycle is confined to the ABL both for JUL91 and ON94. The vertical transport time out of the ABL is of the order of 100h both for the total model domain and over the European continent. The net convective exchange of ozone from the ABL is not a dominant process for the amount of ozone in the ABL averaged over 10 days and the whole domain, but convection reduces the maximum ozone concentration in episodes significantly. The ozone producing efficiency of NOx is calculated to increase with height to typically 15–20 in the upper half of the troposphere from around 5 in the ABL, but in the middle free troposphere the concentration of NOx is often too low to cause net chemical formation of ozone there.
    Type of Medium: Electronic Resource
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  • 2
    ISSN: 1573-0662
    Keywords: total nitrate ; total ammonium ; ozone ; filter pack ; denuder ; numerical modelling
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract Observations of the concentration of several nitrogen containing compounds at five rural Scandinavian sites during March–June 1993 are reported. Total nitrate (NO 3 - + HNO3) and total ammonium (NH 4 + + NH3) were measured by denuder and filter pack. In general the methods agree well. At all sites the particulate fraction dominated, with the largest fraction of NO 3 - and the lowest of NH 4 + at the sites which were closest to the emission sources. The fraction of NO 3 - of total nitrate increased with increasing NO2 concentrations, indicating that the nighttime conversion of NO2 to NO 3 - is an important route of formation for NO 3 - . A positive correlation was found between HNO3 and O3 in June at all sites, while no correlation was found early in the spring. Model calculations were made with a lagrangian boundary layer photooxidant model for the whole period, and compared to the measured concentrations. The calculated ratio between mean observed and modelled daily maximum concentrations of ozone over the measurement period were within +/−10% at all sites. The models ability to describe the daily ozone maximum concentration was satisfactory with an average deviation of 19–22% from the observed concentrations. HNO3 was underestimated by over 50% at all sites except the one closest to the emission sources. The correlation between modelled and observed concentrations was generally best for the sites with shortest transport distance from the sources of emission.
    Type of Medium: Electronic Resource
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