| 1. |
- Bower, K. N., et al.
(författare)
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ACE-2 HILLCLOUD. An overview of the ACE-2 ground-based cloud experiment
- 2000
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Ingår i: Tellus. Series B: Chemical and Physical Meteorology. - : Stockholm University Press. - 0280-6509. ; 52:2, s. 750-778
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Tidskriftsartikel (refereegranskat)abstract
- The ACE-2 HILLCLOUD experiment was carried out on the island of Tenerife in June-July 1997 to investigate the interaction of the boundary layer aerosol with a hill cap cloud forming over a ridge to the north-east of the island. The cloud was used as a natural flow through reactor to investigate the dependence of the cloud microphysics and chemistry on the characteristics of the aerosols and trace gases entering cloud, and to simultaneously study the influence of the physical and chemical processes occurring within the cloud on the size distribution, chemical and hygroscopic properties of the aerosol exiting cloud. 5 major ground base sites were used, measuring trace gases and aerosols upwind and downwind of the cloud, and cloud microphysics and chemistry and interstitial aerosol and gases within the cloud on the hill. 8 intensive measurement periods or runs were undertaken during cloud events, (nocturnally for seven of the eight runs) and were carried out in a wide range of airmass conditions from clean maritime to polluted continental. Polluted air was characterised by higher than average concentrations of ozone (> 50 ppbv), fine and accumulation mode aerosols (> 3000 and > 1500 cm -3 , respectively) and higher aerosol mass loadings. Cloud droplet number concentrations N, increased from 50 cm -3 in background maritime air to > 2500 cm -3 in aged polluted continental air, a concentration much higher than had previously been detected. Surprisingly, N was seen to vary almost linearly with aerosol number across this range. The droplet aerosol analyser (DAA) measured higher droplet numbers than the corrected forward scattering spectrometer probe (FSSP) in the most polluted air, but at other times there was good agreement (FSSP = 0.95 DAA with an r 2 = 0.89 for N < 1200 cm -3 ). Background ammonia gas concentrations were around 0.3 ppbv even in air originating over the ocean, another unexpected but important result for the region. NO 2 was present in background concentrations of typically 15 pptv to 100 pptv and NO 3 . (the nitrate radical) was observed at night throughout. Calculations suggest NO 3 . losses were mainly by reaction with DMS to produce nitric acid. Low concentrations of SO 2 (~30 pptv), HNO 3 and HCl were always present. HNO 3 concentrations were higher in polluted episodes and calculations implied that these exceeded those which could be accounted for by NO 2 oxidation. It is presumed that nitric and hydrochloric acids were present as a result of outgassing from aerosol, the HNO 3 from nitrate rich aerosol transported into the region from upwind of Tenerife, and HCl from sea salt aerosol newly formed at the sea surface. The oxidants hydrogen peroxide and ozone were abundant (i.e., were well in excess over SO 2 throughout the experiment). Occasions of significant aerosol growth following cloud processing were observed, particularly in cleaner cases. Observations and modelling suggested this was due mainly to the take up of nitric acid, hydrochloric acid and ammonia by the smallest activated aerosol particles. On a few occasions a small contribution was made by the in-cloud oxidation of S(IV). The implications of these results from HILLCLOUD for the climatologically more important stratocumulus Marine Boundary Layer (MBL) clouds are considered.
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| 2. |
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| 3. |
- Brandefelt, Jenny, et al.
(författare)
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Anthropogenic and biogenic winter sources of Arctic CO2 - a model study
- 2001
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Ingår i: Tellus. Series B, Chemical and physical meteorology. - : Stockholm University Press. - 0280-6509 .- 1600-0889. ; 53:1, s. 10-21
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Tidskriftsartikel (refereegranskat)abstract
- Long-range transport of anthropogenic and biogenic CO2 to a remote site in the Arctic is studied. A limited area, off-line, Eulerian atmospheric transport model is used, and the results are compared to the observed CO2 concentration at the Ny-Alesund International Arctic Research and Monitoring Facility. Inventories of anthropogenic CO2 emissions and estimates of biogenic CO2 emissions are used to investigate the respective impact of these emissions on Arctic CO2 variations during 4 winter months. A direct comparison of the modelled and observed concentrations reveals remarkably good timing in the modelled variations as compared to the observed variations for most of the time. The correlation of observed versus modelled CO2 concentration is significant at the 95% confidence level. The biogenic and the anthropogenic CO2 emissions are shown to have approximately equal influence on Arctic CO2 variations during winter. Europe is found to be the dominant source of anthropogenic CO2 Lit the monitoring station, while Siberia and Northern America have little influence on Arctic CO2. during the months studied. These results contradict Engardt and Holmen whose results indicate that the lower-Ob region in western Siberia has a large impact on Arctic CO2.
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| 4. |
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| 5. |
- Delmas, RJ, et al.
(författare)
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Bomb-test Cl-36 measurements in Vostok snow (Antarctica) and the use of Cl-36 as a dating tool for deep ice cores
- 2004
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Ingår i: Tellus. Series B: Chemical and Physical Meteorology. - : Stockholm University Press. - 0280-6509. ; 56:5, s. 492-498
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Tidskriftsartikel (refereegranskat)abstract
- A large pulse of atmospheric Cl-36 generated by a limited number of nuclear tests peaked in the late 1950s to early 1960s. The corresponding enhanced Cl-36 deposition is seen in various glaciological archives in the Northern Hemisphere. The profile of the bomb spike recorded in firn layers at Vostok Station, central East Antarctica. has been measured by employing accelerator mass spectrometry (AMS). The records obtained front two well-dated data sets collected in snow pits in 1997 and 1998 show a broad Cl-36 peak, beginning as early as the 1940s and reaching its maximum in the 1960s. The signal is followed by a long-lasting tail up to the surface. This pattern is totally unexpected. We show that the results, unlike the Greenland data, can be explained by a mobility of HCl in the Antarctic firn. This experiment demonstrates the instability of gaseous Cl- deposits. a phenomenon which has important implications for the use of natural cosmogenic Cl-36 radionuclides as a reliable dating tool for deep ice cores from low-accumulation areas. However, during glacial times, under favourable atmospheric chemistry conditions this dating method may still be applicable. Snow metamorphism and ventilation are assumed to be the two main physical processes responsible for the observed patterns.
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| 6. |
- Flynn, Michael J., et al.
(författare)
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Modelling cloud processing of aerosol during the ACE-2 HILLCLOUD experiment
- 2000
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Ingår i: Tellus. Series B: Chemical and Physical Meteorology. - : Stockholm University Press. - 0280-6509. ; 52:2, s. 779-800
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Tidskriftsartikel (refereegranskat)abstract
- A numerical model has been used to simulate the conditions observed during the ACE-2 Hillcloud experiment and to study the processes which may be taking place. The model incorporates gas phase chemistry of sulphur and nitrogen compounds upstream of the cloud, and the interaction of aerosol, precursor trace gases and oxidants within the cloud. Gas phase and aerosol inputs to the model have been provided from measurements made in the field. Dynamics of the air flow over the hill consisted of simple prescribed dynamics based on wind speed measurements, and also for some cases modelled dynamics. In this modelling study, it was found that during clean case studies particles down to 40-55 nm diameter were activated to form cloud droplets, the total number of droplets formed ranging from 200 to 400 drops/cm3. Significant modification of the aerosol spectra due to cloud processing was observed. In polluted cases particles down to 65-80 nm diameter were activated to form cloud droplets, the total number of droplets ranging from 800 to 2800 drops/cm3. Modification of the aerosol spectra due to cloud processing was slight. In all cases, changes in the aerosol spectra were due to both the uptake of HNO3, HCl, NH3 and SO2 from the gas phase, (the SO2 being oxidised to sulphate) and the repartitioning of species such as HNO3, HCl, and NH3 from larger particles onto smaller ones. Modelling results have been compared with observations made. Modelled droplet numbers are typically within 20% of the best measured values. The mode of the droplet distribution typically around 10-20 μm for clean cases and 4-8 μm for polluted cases was found to be in good agreement with the measured values of 10-25 μm for clean cases, but not in such good agreement for polluted cases. Measurements of upwind and interstitial aerosol distributions showed that the smallest particles activated were 30 and 50 nm for clean and polluted cases respectively, slightly smaller than the model values quoted above. Measured upwind and downwind aerosol spectra showed similar modification to that predicted by the model in eight out of the eleven model runs carried out. Chemistry measurements also give general evidence for both the uptake of species from the gas phase, and repartitioning of species from large particles onto smaller ones, though comparisons for individual cases are more difficult. From this modelling study, it can be concluded that in general, in the remote environment the exchange of hydrochloric acid, nitric acid and ammonia between aerosol particles and take up from the gas phase in the vicinity of cloud may be a very important mechanism in regulating the evolution of the aerosol spectrum. Further, the much more linear relationship between cloud droplet and accumulation mode aerosol number, which was observed in the measurements made during the ACE-2 HILLCLOUD project is supported by these modelling results. The implications of this for the indirect effect will be explored in future work.
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| 7. |
- Johansson, Elisabeth, et al.
(författare)
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Nitrous oxide exchanges with the atmosphere of a constructed wetland treating wastewater - Parameters and implications for emission factors
- 2003
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Ingår i: Tellus Series B-Chemical and Physical Meteorology. - : Stockholm University Press. - 0280-6509 .- 1600-0889. ; 55:3, s. 737-750
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Tidskriftsartikel (refereegranskat)abstract
- Static chamber measurements of N2O fluxes were taken during the 1998 and 1999 growth seasons in a Swedish constructed wetland receiving wastewater. The dominating plant species in different parts of the wetland were Lemna minor L., Typha latifolia L., Spirogyra sp. and Glyceria maxima (Hartm.) and Phalaris arundinacea (L.), respectively. There were large temporal and spatial variations in N2O fluxes, which ranged from consumption at -350 to emissions at 1791 mug N2O m(-2) h(-1). The largest positive flux occurred in October 1999 and the lowest in the middle of July 1999. The average N2O flux for the two years was 130 mug N2O m(-2) h(-1) (SD = 220). No significant differences in N2O fluxes were found between the years, even though the two growing seasons differed considerably with respect to both air temperature and precipitation. 15% of the fluxes were negative, showing a consumption of N2O. Consumption occurred on a few occasions at most measurement sites and ranged from 1-350 mug N2O m(-2) h(-1). 13-43% of the variation in N2O fluxes was explained by multiple linear regression analysis including principal components. Emission factors were calculated according to IPCC methods from the N2O fluxes in the constructed wetland. The calculated emission factors were always lower (0.02-0.27%) compared to the default factor provided by the IPCC (0.75%). Thus, direct application of the IPCC default factor may lead to overestimation of N2O fluxes from constructed wastewater-treating wetlands.
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| 8. |
- Martinsson, Bengt G., et al.
(författare)
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Validation of very high cloud droplet number concentrations in air masses transported thousands of kilometres over the ocean
- 2000
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Ingår i: Tellus. Series B: Chemical and Physical Meteorology. - 0280-6509. ; 52:2, s. 801-814
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Tidskriftsartikel (refereegranskat)abstract
- The microstructure of orographic clouds related to the aerosol present was studied during the second Aerosol Characterisation Experiment (ACE-2). Very high cloud droplet number concentrations (almost 3000 cm -3 ) were observed. These high concentrations occurred when clouds formed on a hill slope at Tenerife in polluted air masses originating in Europe that had transported the order of 1000 km over the Atlantic Ocean. The validity of the measured droplet number concentrations was investigated by comparing with measurements of the aerosol upstream of the cloud and cloud interstitial aerosol. Guided by distributions of the ratios between the measurements, three criteria of typically 30% in maximum deviation were applied to the measurements to test their validity. Agreement was found for 88% of the cases. The validated data set spans droplet number concentrations of 150-3000 cm -3 . The updraught velocity during the cloud formation was estimated to 2.2 m s -1 by model calculations, which is typical of cumuliform clouds. The results of the present study are discussed in relation to cloud droplet number concentrations previously reported in the literature. The importance of promoting the mechanistic understanding of the aerosol/cloud interaction and the use of validation procedures of cloud microphysical parameters is stressed in relation to the assessment of the indirect climatic effect of aerosols.
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| 9. |
- Swietlicki, Erik, et al.
(författare)
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Hygroscopic properties of aerosol particles in the northeastern Atlantic during ACE-2
- 2000
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Ingår i: Tellus. Series B: Chemical and Physical Meteorology. - : Stockholm University Press. - 0280-6509 .- 1600-0889. ; 52:2, s. 201-227
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Tidskriftsartikel (refereegranskat)abstract
- Measurements of the hygroscopic properties of sub-micrometer atmospheric aerosol particles were performed with hygroscopic tandem differential mobility analysers (H-TDMA) at 5 sites in the subtropical north-eastern Atlantic during the second Aerosol Characterization Experiment (ACE-2) from 16 June to 25 July 1997. Four of the sites were in the marine boundary layer and one was, at least occasionally, in the lower free troposphere. The hygroscopic diameter growth factors of individual aerosol particles in the dry particle diameter range 10-440 nm were generally measured for changes in relative humidity (RH) from <10% to 90%. In the marine boundary layer, growth factors at 90% RH were dependent on location, air mass type and particle size. The data was dominated by a unimodal growth distribution of more-hygroscopic particles, although a bimodal growth distribution including less-hygroscopic particles was observed at times, most often in the more polluted air masses. In clean marine air masses the more-hygroscopic growth factors ranged from about 1.6 to 1.8 with a consistent increase in growth factor with increasing particle size. There was also a tendency toward higher growth factors as sodium to sulphate molar ratio increased with increasing sea-salt contribution at higher wind speeds. During outbreaks of European pollution in the ACE-2 region, the growth factors of the largest particles were reduced, but only slightly. Growth factors at all sizes in both clean and polluted air masses were markedly lower at the Sagres, Portugal site due to more proximate continental influences. The frequency of occurrence of less-hygroscopic particles with a growth factor of ca. 1.15 was greatest during polluted conditions at Sagres. The free tropospheric 50 nm particles were predominately less-hygroscopic, with an intermediate growth factor of 1.4, but more-hygroscopic particles with growth factors of about 1.6 were also frequent. While these particles probably originate from within the marine boundary layer, the less-hygroscopic particles are probably more characteristic of lower free tropospheric air masses. For those occasions when measurements were made at 90% and an intermediate 60% or 70% RH, the growth factor G(RH) of the more-hygroscopic particles could be modelled empirically by a power law expression. For the ubiquitous more-hygroscopic particles, the expressions G(RH) = (1 - RH/100)-0.210 for 50 nm Aitken mode particles and G(RH) = (1 - RH/100)-0.233 for 166 nm accumulation mode particles are recommended for clean marine air masses in the north-eastern Atlantic within the range 0 < RH < 95%, and for wind speeds for which the local sea-salt production is small (< ca. 8 m s-1).
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