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  • 1
    Publication Date: 2002-11-05
    Description: We examine the effect of nanometer-sized aircraft-induced aqueous sulfuric acid (H2SO4/H2O) particles on atmospheric ozone as a function of temperature. Our calculations are based on a previously derived parameterization for the regional-scale perturbations of the sulfate surface area density due to air traffic in the North Atlantic Flight Corridor (NAFC) and a chemical box model. We confirm large scale model results that at temperatures T〉210 K additional ozone loss -- mainly caused by hydrolysis of BrONO2 and N2O5 -- scales in proportion with the aviation-produced increase of the background aerosol surface area. However, at lower temperatures (〈 210 K) we isolate two effects which efficiently reduce the aircraft-induced perturbation: (1) background particles growth due to H2O and HNO3 uptake enhance scavenging losses of aviation-produced liquid particles and (2) the Kelvin effect efficiently limits chlorine activation on the small aircraft-induced droplets by reducing the solubility of chemically reacting species. These two effects lead to a substantial reduction of heterogeneous chemistry on aircraft-induced volatile aerosols under cold conditions. In contrast we find contrail ice particles to be potentially important for heterogeneous chlorine activation and reductions in ozone levels. These features have not been taken into consideration in previous global studies of the atmospheric impact of aviation. Therefore, to parameterize them in global chemistry and transport models, we propose the following parameterisation: scale the hydrolysis reactions by the aircraft-induced surface area increase, and neglect heterogeneous chlorine reactions on liquid plume particles but not on ice contrails and aircraft induced ice clouds.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 2
    Publication Date: 2002-05-15
    Description: Polar stratospheric clouds (PSCs) of type 1a or 1a-enh containing high number densities of nitric acid trihydrate (NAT) particles, can act as mother clouds for extremely large NAT particles, termed NAT-rocks, provided the air below the clouds is supersaturated with respect to NAT. Individual NAT particles at the cloud base fall into undepleted gas phase and rapidly accelerate due to a positive feedback between their growth and sedimentation. The resulting reduction in number density is further enhanced by the strong HNO3 depletion within a thin layer below the mother cloud, which delays subsequent particles. This paper introduces the basic microphysical principles behind this mother cloud/NAT-rock mechanism, which produces 10-4 cm-3 NAT-rocks with radii around 10 mm some kilometers below the mother cloud. The mechanism does not require selective nucleation and works even for a monodisperse particle size distribution in the mother cloud.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 3
    Publication Date: 2002-10-28
    Description: The penetration of solar H Lyman-a radiation into the terrestrial middle atmosphere is studied in detail. The Lyman-a actinic flux is calculated with a Monte Carlo approach including multiple resonance scattering of Lyman-a photons within the terrestrial atmosphere and a temperature dependent absorption cross section of molecular oxygen. The dependence of the actinic flux on the temperature profile is significant for O2 column densities greater than about 1024 m-2. For column densities greater than about 5 · 1024 m-2 resonance scattering becomes important at solar zenith angles 〉 60°. The OD quantum yield of the O2 dissociation by Lyman-aphotons is found to decrease from 0.58 in the lower thermosphere to 0.48 in the lower mesosphere. Parameterisations for Lyman-a actinic flux, mean O2 absorption cross section and ODquantum yield including temperature dependence and resonance scattering are given valid up to a O2 column density of about 1025 m-2.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 4
    Publication Date: 2002-12-16
    Description: The physical state of tropospheric aerosol particles is largely unknown despite its importance for cloud formation and for the aerosols' radiative properties. Here we show the first systematic global modelling study of the physical state of the H2SO4/NH3/H2O aerosol, which constitutes an important class of aerosols in the free troposphere. The Aerosol Physical State Model (APSM) developed here is based on Lagrangian trajectories computed from ECMWF (European Centre for Medium Range Weather Forecasts) analyses, taking full account of the deliquescence/efflorescence hysteresis. As input APSM requires three data sets: (i) deliquescence and efflorescence relative humidities from laboratory measurements, (ii) ammonia-to-sulfate ratios (ASR) calculated by a global circulation model, and (iii) relative humidities determined from the ECMWF analyses. APSM results indicate that globally averaged a significant fraction (17-57%) of the ammoniated sulfate aerosol particles contain solids with the ratio of solid-containing to purely liquid particles increasing with altitude (between 2 and 10 km). In our calculations the most abundant solid is letovicite, (NH4)3H(SO4)2, while there is only little ammonium sulfate, (NH4)2SO4. Since ammonium bisulfate, NH4HSO4, does not nucleate homogeneously, it can only form via heterogeneous crystallization. As the ammonia-to-sulfate ratios of the atmospheric aerosol usually do not correspond to the stoichiometries of known crystalline substances, all solids are expected to occur in mixed-phase aerosol particles. This work highlights the global importance of letovicite, whose role as cloud condensation nucleus (CCN) and as scatterer of solar radiation remains to be scrutinized.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 5
    Publication Date: 2002-07-15
    Description: We examine the effect of nm-sized aircraft-induced aqueous sulfuric acid (H2SO4/H2O) particles on atmospheric ozone as a function of temperature. Our calculations are based on a previously derived parameterization for the regional-scale perturbations of the sulfate surface area density due to air traffic in the North Atlantic Flight Corridor (NAFC) and a chemical box model. We confirm large scale model results that at temperatures T 〉 210 K additional ozone loss -- mainly caused by hydrolysis of BrONO2 and N2O5 -- scales in proportion with the aviation-produced increase of the background aerosol surface area. However, at lower temperatures (〈 210 K) we isolate two effects which efficiently reduce the aircraft-induced perturbation: (1) background particles growth due to H2O and HNO3 uptake enhance scavenging losses of aviation-produced liquid particles and (2) the Kelvin effect efficiently limits chlorine activation on the small aircraft-induced droplets by reducing the solubility of chemically reacting species. These two effects lead to a substantial reduction of heterogeneous chemistry on aircraft-induced volatile aerosols under cold conditions. In contrast we find contrail ice particles to be potentially important for heterogeneous chlorine activation and ozone depletion. These features have not been taken into consideration in previous global studies of the atmospheric impact of aviation. Therefore, to parameterize them in global chemistry and transport models, we propose the following parameterisation: scale the hydrolysis reactions by the aircraft-induced surface area increase, and neglect heterogeneous chlorine reactions on liquid plume particles but not on ice contrails and aircraft induced ice clouds.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 6
    Publication Date: 2002-01-14
    Description: Polar stratospheric clouds (PSCs) of type 1a or 1a-enh containing high number densities of nitric acid trihydrate (NAT) particles, can act as mother clouds for extremely large NAT particles, termed NAT-rocks, provided the air below the clouds is supersaturated with respect to NAT. Individual NAT particles at the cloud base fall into undepleted gas phase and rapidly accelerate due to a positive feedback between their growth and sedimentation. The resulting reduction in number density is further enhanced by the strong HNO3 depletion within a thin layer below the mother cloud, which delays subsequent particles. This paper introduces the basic microphysical principles behind this mother cloud/NAT-rock mechanism, which produces 10-4 cm-3 NAT-rocks with radii around 10mm some kilometers below the mother cloud. The mechanism requires neither selective nucleation nor additional atmospheric dilution and works even for a monodisperse particle size distribution in the mother cloud.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 7
    Publication Date: 2002-08-31
    Description: Global geomagnetic activity has been suggested to be enhanced during weekends above the weekly average after 1930. Before the 1930s, weekends and weekdays were found to be equally active. This so-called "weekend effect" was suggested to be due to power line harmonic radiation (PLHR) in the VLF range emitted by electric power lines. Since the consumption of electric power is different on weekends and weekdays, leading to different PLHR intensities, this could possibly cause the "weekend effect" in global geomagnetic activity. In the present paper, we reanalyse the suggested "week-end effect" in global geomagnetic activity using the 69-year planetary geomagnetic Ap index and the 131-year antipodal aa index. We conclude that there is no statistically significant "weekend effect" during the interval covered by these geo-magnetic activity indices. Although global geomagnetic activity is slightly enhanced on weekends from the 1930s to the 1980s, the more recent data show rather a relative decrease in global geomagnetic activity on weekends, contrary to the expected increase in the "weekend effect", due to increasing power consumption. Moreover, the weekly distribution is fairly similar in solar wind speed and global geomagnetic activity during the last 35 years, further supporting the view that the "weekend effect" is only a statistical fluctuation.Key words. Geomagnetism and paleomagnetism (time variations, diurnal to secular) – Magnetospheric physics (planetary magnetospheres; storms and substorms)
    Print ISSN: 0992-7689
    Electronic ISSN: 1432-0576
    Topics: Geosciences , Physics
    Published by Copernicus on behalf of European Geosciences Union.
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  • 8
    Publication Date: 2002-12-31
    Description: Solar proton events and electron precipitation affect the concentrations of middle atmospheric constituents. Ionization caused by precipitating particles enhances the production of important minor neutral constituents, such as nitric oxide, through reaction chains in which ionic reactions play an important role. The Sodankylä Ion Chemistry model (SIC) has been modified and extended into a detailed ion and neutral chemistry model of the mesosphere. Our steady-state model (containing 55 ion species, 8 neutral species, and several hundred chemical reactions) is used to investigate the effect of the October 1989 solar proton event on odd nitrogen at altitudes between 50–90 km. The modelling results show that the NO concentration is significantly enhanced due to the proton precipitation, reaching 107 –108 cm-3 throughout the mesosphere on the 20 October when the proton forcing was most severe. A comparison between the chemical production channels of odd nitrogen indicates that ion chemical reactions are an important factor in the total odd nitrogen production during intense ionization. The modelled electron concentration for the 23 October is compared with EISCAT incoherent scatter radar measurements and a reasonable agreement is found.Key words. Atmospheric composition and structure (Middle atmosphere – composition and chemistry); Ionosphere (Particle precipitation)
    Print ISSN: 0992-7689
    Electronic ISSN: 1432-0576
    Topics: Geosciences , Physics
    Published by Copernicus on behalf of European Geosciences Union.
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