| 11. |
- Khosrawi, Farahnaz, 1971-, et al.
(författare)
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Evaluation of CLaMS, KASIMA and ECHAM5/MESSy1 simulations in the lower stratosphere using observations of Odin/SMR and ILAS/ILAS-II
- 2009
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 9:15, s. 5759-5783
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Tidskriftsartikel (refereegranskat)abstract
- 1-year data sets of monthly averaged nitrous oxide (N2O) and ozone (O3) derived from satellite measurements were used as a tool for the evaluation of atmospheric photochemical models. Two 1-year data sets, one solar occultation data set derived from the Improved Limb Atmospheric Spectrometer (ILAS and ILAS-II) and one limb sounding data set derived from the Odin Sub-Millimetre Radiometer (Odin/SMR) were employed. Here, these data sets are used for the evaluation of two Chemical Transport Models (CTMs), the Karlsruhe Simulation Model of the Middle Atmosphere (KASIMA) and the Chemical Lagrangian Model of the Stratosphere (CLaMS) as well as for one Chemistry-Climate Model (CCM), the atmospheric chemistry general circulation model ECHAM5/MESSy1 (E5M1) in the lower stratosphere with focus on the Northern Hemisphere. Since the Odin/SMR measurements cover the entire hemisphere, the evaluation is performed for the entire hemisphere as well as for the low latitudes, midlatitudes and high latitudes using the Odin/SMR 1-year data set as reference. To assess the impact of using different data sets for such an evaluation study we repeat the evaluation for the polar lower stratosphere using the ILAS/ILAS-II data set. Only small differences were found using ILAS/ILAS-II instead of Odin/SMR as a reference, thus, showing that the results are not influenced by the particular satellite data set used for the evaluation. The evaluation of CLaMS, KASIMA and E5M1 shows that all models are in agreement with Odin/SMR and ILAS/ILAS-II. Differences are generally in the range of ±20%. Larger differences (up to −40%) are found in all models at 500±25 K for N2O mixing ratios greater than 200 ppbv, thus in air masses of tropical character. Generally, the largest differences were found for the tropics and the lowest for the polar regions. However, an underestimation of polar winter ozone loss was found both in KASIMA and E5M1 both in the Northern and Southern Hemisphere.
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| 12. |
- Kulmala, M., et al.
(författare)
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Introduction: European Integrated Project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) : integrating aerosol research from nano to global scales
- 2009
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 9, s. 2825-2841
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Tidskriftsartikel (refereegranskat)abstract
- The European Aerosol Cloud Climate and Air Quality Interactions project EUCAARI is an EU Research Framework 6 integrated project focusing on understanding the interactions of climate and air pollution. EUCAARI works in an integrative and multidisciplinary way from nano-to global scale. EUCAARI brings together several leading European research groups, state-of-the-art infrastructure and some key scientists from third countries to investigate the role of aerosol on climate and air quality. Altogether 48 partners from 25 countries are participating in EUCAARI. During the first 16 months EUCAARI has built operational systems, e. g. established pan-European measurement network for Lagrangian studies and four stations in developing countries. Also an improved understanding of nanoscale processes (like nucleation) has been implemented in global models. Here we present the research methods, organisation, operations and first results of EUCAARI.
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| 13. |
- Lossow, Stefan, et al.
(författare)
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Middle atmospheric water vapour and dynamics in the vicinity of the polar vortex during the Hygrosonde-2 campaign
- 2009
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Ingår i: Atmospheric Chemistry And Physics. - 1680-7316 .- 1680-7324. ; 9, s. 4407-4417
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Tidskriftsartikel (refereegranskat)abstract
- The Hygrosonde-2 campaign took place on 16 December 2001 at Esrange/Sweden (68° N, 21° E) with the aim to investigate the small scale distribution of water vapour in the middle atmosphere in the vicinity of the Arctic polar vortex. In situ balloon and rocket-borne measurements of water vapour were performed by means of OH fluorescence hygrometry. The combined measurements yielded a high resolution water vapour profile up to an altitude of 75 km. Using the characteristic of water vapour being a dynamical tracer it was possible to directly relate the water vapour data to the location of the polar vortex edge, which separates air masses of different character inside and outside the polar vortex. The measurements probed extra-vortex air in the altitude range between 45 km and 60 km and vortex air elsewhere. Transitions between vortex and extra-vortex usually coincided with wind shears caused by gravity waves which advect air masses with different water vapour volume mixing ratios. From the combination of the results from the Hygrosonde-2 campaign and the first flight of the optical hygrometer in 1994 (Hygrosonde-1) a clear picture of the characteristic water vapour distribution inside and outside the polar vortex can be drawn. Systematic differences in the water vapour concentration between the inside and outside of the polar vortex can be observed all the way up into the mesosphere. It is also evident that in situ measurements with high spatial resolution are needed to fully account for the small-scale exchange processes in the polar winter middle atmosphere.
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| 14. |
- Orsolini, Y. J., et al.
(författare)
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Nitric acid in the stratosphere based on Odin observations from 2001 to 2009 – Part 2: High-altitude polar enhancements
- 2009
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 9:18, s. 7045-7052
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Tidskriftsartikel (refereegranskat)abstract
- The wintertime abundance of nitric acid (HNO3) in the polar upper stratosphere displays a strong inter-annual variability, and is known to be strongly influenced by energetic particle precipitation (EPP), primarily by protons during solar proton events (SPEs), but also by precipitating auroral or relativistic electrons. We analyse a multi-year record (August 2001 to April 2009) of middle atmospheric HNO3 measurements by the Sub-Millimeter Radiometer instrument aboard the Odin satellite, with a focus on the polar upper stratosphere. SMR observations show clear evidence of two different types of polar high-altitude HNO3 enhancements linked to EPP. In the first type, referred to as direct enhancements by analogy with the EPP/NOx direct effect, enhanced HNO3 mixing ratios are observed for a short period (1 week) after a SPE, upwards of a level typically in the mid-stratosphere. In a second type, referred to as indirect enhancements by analogy with the EPP/NOx indirect effect, the descent of mesospheric air triggers a stronger and longer-lasting enhancement. Each of the three major SPEs that occurred during the Northern Hemisphere autumn or winter, in November 2001, October–November 2003 and January 2005, are observed to lead to both direct and indirect HNO3 enhancements. On the other hand, indirect enhancements occur recurrently in winter, are stronger in the Southern Hemisphere, and are influenced by EPP at higher altitudes.
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| 15. |
- Rivera, Claudia, 1976, et al.
(författare)
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Tula industrial complex (Mexico) emissions of SO2 and NO2 during the MCMA 2006 field campaign using a mobile mini-DOAS system
- 2009
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 9, s. 6351-6361
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Tidskriftsartikel (refereegranskat)abstract
- The Mexico City Metropolitan Area (MCMA) has presented severe pollution problems for many years. There are several point and mobile emission sources inside and outside the MCMA which are known to affect air quality in the area. In particular, speculation has risen as to whether the Tula industrial complex, located 60 km northwest of the MCMA has any influence on high SO2 levels occurring on the northern part of the city, in the winter season mainly. As part of the MILAGRO Field Campaign, from 24 March to 17 April 2006, the differential vertical columns of sulfur dioxide (SO2) and nitrogen dioxide (NO2) were measured during plume transects in the neighborhood of the Tula industrial complex using mobile mini-DOAS instruments. Vertical profiles of wind speed and direction obtained from pilot balloons and radiosondes were used to calculate SO2 and NO2 emissions. According to our measurements, calculated average emissions of SO2 and NO2 during the field campaign were 384 ± 103 and 24 ± 7 tons day-1, respectively. The standard deviation of these estimations is due to actual variations in the observed emissions from the refinery and power plant, as well as to the uncertainty in the wind fields at the exact time of the measurements. Reported values in recent inventories were found to be in good agreement with calculated emissions during the field campaign. Our measurements were also found to be in good agreement with simulated plumes.
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| 16. |
- Sheesley, R.J., et al.
(författare)
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Source apportionment of elevated wintertime PAHs by compound-specific radiocarbon analysis
- 2009
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Ingår i: Atmospheric Chemistry And Physics. - 1680-7316 .- 1680-7324. ; 9:10, s. 3347-3356
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Tidskriftsartikel (refereegranskat)abstract
- Natural abundance radiocarbon analysis facilitates distinct source apportionment between contemporary biomass/biofuel (C-14 "alive") versus fossil fuel (C-14 "dead") combustion. Here, the first compound-specific radiocarbon analysis (CSRA) of atmospheric polycyclic aromatic hydrocarbons (PAHs) was demonstrated for a set of samples collected in Lycksele, Sweden a small town with frequent episodes of severe atmospheric pollution in the winter. Renewed interest in using residential wood combustion (RWC) means that this type of seasonal pollution is of increasing concern in many areas. Five individual/paired PAH isolates from three pooled fortnight-long filter collections were analyzed by CSRA: phenanthrene, fluoranthene, pyrene, benzo[b+k] fluoranthene and indeno[cd]pyrene plus benzo[ghi]perylene; phenanthrene was the only compound also analyzed in the gas phase. The measured Delta C-14 for PAHs spanned from -138.3% to 58.0%. A simple isotopic mass balance model was applied to estimate the fraction biomass (fbiomass) contribution, which was constrained to 71-87% for the individual PAHs. Indeno[cd]pyrene plus benzo[ghi]perylene had an fbiomass of 71%, while fluoranthene and phenanthrene (gas phase) had the highest biomass contribution at 87%. The total organic carbon (TOC, defined as carbon remaining after removal of inorganic carbon) fbiomass was estimated to be 77%, which falls within the range for PAHs. This CSRA data of atmospheric PAHs established that RWC is the dominating source of atmospheric PAHs to this region of the boreal zone with some variations among RWC contributions to specific PAHs
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| 17. |
- Struthers, Hamish, et al.
(författare)
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The simulation of the Antarctic ozone hole by chemistry-climate models
- 2009
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 9:17, s. 6363-6376
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Tidskriftsartikel (refereegranskat)abstract
- While chemistry-climate models are able to reproduce many characteristics of the global total column ozone field and its long-term evolution, they have fared less well in simulating the commonly used diagnostic of the area of the Antarctic ozone hole i.e. the area within the 220 Dobson Unit (DU) contour. Two possible reasons for this are: (1) the underlying Global Climate Model (GCM) does not correctly simulate the size of the polar vortex, and (2) the stratospheric chemistry scheme incorporated into the GCM, and/or the model dynamics, results in systematic biases in the total column ozone fields such that the 220DU contour is no longer appropriate for delineating the edge of the ozone hole. Both causes are examined here with a view to developing ozone hole area diagnostics that better suit measurement-model inter-comparisons. The interplay between the shape of the meridional mixing barrier at the edge of the vortex and the meridional gradients in total column ozone across the vortex edge is investigated in measurements and in 5 chemistry-climate models (CCMs). Analysis of the simulation of the polar vortex in the CCMs shows that the first of the two possible causes does play a role in some models. This in turn affects the ability of the models to simulate the large observed meridional gradients in total column ozone. The second of the two causes also strongly affects the ability of the CCMs to track the observed size of the ozone hole. It is shown that by applying a common algorithm to the CCMs for selecting a delineating threshold unique to each model, a more appropriate diagnostic of ozone hole area can be generated that shows better agreement with that derived from observations.
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| 18. |
- Szidat, S., et al.
(författare)
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Fossil and non-fossil sources of organic carbon (OC) and elemental carbon (EC) in Göteborg, Sweden
- 2009
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 9:5, s. 1521-1535
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Tidskriftsartikel (refereegranskat)abstract
- Particulate matter was collected at an urban site in Göteborg (Sweden) in February/March 2005 and in June/July 2006. Additional samples were collected at a rural site for the winter period. Total carbon (TC) concentrations were 2.1–3.6μgm−3, 1.8–1.9μgm−3, and 2.2– 3.0μgm−3 for urban/winter, rural/winter, and urban/summer conditions, respectively. Elemental carbon (EC), organic carbon (OC), water-insoluble OC (WINSOC), and watersoluble OC (WSOC) were analyzed for 14C in order to distinguish fossil from non-fossil emissions. As wood burning is the single major source of non-fossil EC, its contribution can be quantified directly. For non-fossil OC, the wood-burning fraction was determined independently by levoglucosan and 14C analysis and combined using Latin-hypercube sampling (LHS). For the winter period, the relative contribution of EC from wood burning to the total EC was >3 times higher at the rural site compared to the urban site, whereas the absolute concentrations of EC from wood burning were elevated only moderately at the rural compared to the urban site. Thus, the urban site is substantially more influenced by fossil EC emissions. For summer, biogenic emissions dominated OC concentrations most likely due to secondary organic aerosol(SOA) formation. During both seasons, a more pronounced fossil signal was observed for G¨oteborg than has previously been reported for Zurich, Switzerland. Analysis of air mass origin using back trajectories suggests that the fossil impact was larger when local sources dominated, whereas longrange transport caused an enhanced non-fossil signal. In comparison to other European locations, concentrations of levoglucosan and other monosaccharide anhydrides were low for the urban and the rural site in the area of G¨oteborg during winter.
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| 19. |
- Urban, Joachim, 1964, et al.
(författare)
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Nitric acid in the stratosphere based on Odin observations from 2001 to 2009 – Part 1: A global climatology
- 2009
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 9:18, s. 7031-7044
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Tidskriftsartikel (refereegranskat)abstract
- The Sub-Millimetre Radiometer (SMR) on board the Odin satellite, launched in February 2001, observes thermal emissions of stratospheric nitric acid (HNO3) originating from the Earth limb in a band centred at 544.6 GHz. Height-resolved measurements of the global distribution of nitric acid in the stratosphere were performed approximately on two observation days per week. An HNO3 climatology based on more than 7 years of observations from August 2001 to April 2009 covering the vertical range between typically ~19 and 45 km (~1.5–60 hPa or ~500–1800 K in terms of potential temperature) was created. The study highlights the spatial and seasonal variation of nitric acid in the stratosphere, characterised by a pronounced seasonal cycle at middle and high latitudes with maxima during late fall and minima during spring, strong denitrification in the lower stratosphere of the Antarctic polar vortex during winter (the irreversible removal of NOy by the sedimentation of cloud particles containing HNO3), as well as large quantities of HNO3 formed every winter at high-latitudes in the middle and upper stratosphere. A strong inter-annual variability is observed in particular at high latitudes. A comparison with a stratospheric HNO3 climatology, based on over 7 years of UARS/MLS (Upper Atmosphere Research Satellite/Microwave Limb Sounder) measurements from the 1990s, shows good consistency and agreement of the main morphological features in the potential temperature range ~465 to ~960 K, if the different characteristics of the data sets such as the better altitude resolution of Odin/SMR as well as the slightly different altitude ranges are considered. Odin/SMR reaches higher up and UARS/MLS lower down in the stratosphere. An overview from 1991 to 2009 of stratospheric nitric acid is provided (with a short gap between 1998 and 2001), if the global measurements of both experiments are taken together.
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| 20. |
- Yong, Yu, 1972, et al.
(författare)
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Observations of high rates of NO2-HONO conversion in the nocturnal atmospheric boundary layer in Kathmandu, Nepal
- 2009
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 9:17, s. 6401-6415
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Tidskriftsartikel (refereegranskat)abstract
- Nitrous acid (HONO) plays a significant role in the atmosphere, especially in the polluted troposphere. Its photolysis after sunrise is an important source of hydroxyl free radicals (OH). Measurements of nitrous acid and other pollutants were carried out in the Kathmandu urban atmosphere during January-February 2003, contributing to the sparse knowledge of nitrous acid in South Asia. The results showed average nocturnal levels of HONO (1.7+/-0.8 ppbv), NO2 (17.9+/-10.2 ppbv), and PM10(0.18+/-0.11 mg m(-3)) in urban air in Kathmandu. Surprisingly high ratios of chemically formed secondary [HONO] to [NO2] (up to 30%) were found, which indicates unexpectedly efficient chemical conversion of NO2 to HONO in Kathmandu. The ratios of [HONO]/[NO2] at night were found to be much higher than previously reported values from measurements in urban air in Europe, North America and Asia. The influences of aerosol surface, ground reactive surface, and relative humidity on NO2-HONO chemical conversion were discussed. The high humidity, strong and low inversion layer at night, and high aerosol pollution burden in Kathmandu may explain the particularly efficient conversion of NO2 to HONO.
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