| 1. |
- Aas, W., et al.
(författare)
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Lessons learnt from the first EMEP intensive measurement periods
- 2012
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:17, s. 8073-8094
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Tidskriftsartikel (refereegranskat)abstract
- The first EMEP intensive measurement periods were held in June 2006 and January 2007. The measurements aimed to characterize the aerosol chemical compositions, including the gas/aerosol partitioning of inorganic compounds. The measurement program during these periods included daily or hourly measurements of the secondary inorganic components, with additional measurements of elemental- and organic carbon (EC and OC) and mineral dust in PM1, PM2.5 and PM10. These measurements have provided extended knowledge regarding the composition of particulate matter and the temporal and spatial variability of PM, as well as an extended database for the assessment of chemical transport models. This paper summarise the first experiences of making use of measurements from the first EMEP intensive measurement periods along with EMEP model results from the updated model version to characterise aerosol composition. We investigated how the PM chemical composition varies between the summer and the winter month and geographically. The observation and model data are in general agreement regarding the main features of PM10 and PM2.5 composition and the relative contribution of different components, though the EMEP model tends to give slightly lower estimates of PM10 and PM2.5 compared to measurements. The intensive measurement data has identified areas where improvements are needed. Hourly concurrent measurements of gaseous and particulate components for the first time facilitated testing of modelled diurnal variability of the gas/aerosol partitioning of nitrogen species. In general, the modelled diurnal cycles of nitrate and ammonium aerosols are in fair agreement with the measurements, but the diurnal variability of ammonia is not well captured. The largest differences between model and observations of aerosol mass are seen in Italy during winter, which to a large extent may be explained by an underestimation of residential wood burning sources. It should be noted that both primary and secondary OC has been included in the calculations for the first time, showing promising results. Mineral dust is important, especially in southern Europe, and the model seems to capture the dust episodes well. The lack of measurements of mineral dust hampers the possibility for model evaluation for this highly uncertain PM component. There are also lessons learnt regarding improved measurements for future intensive periods. There is a need for increased comparability between the measurements at different sites. For the nitrogen compounds it is clear that more measurements using artefact free methods based on continuous measurement methods and/or denuders are needed. For EC/OC, a reference methodology (both in field and laboratory) was lacking during these periods giving problems with comparability, though measurement protocols have recently been established and these should be followed by the Parties to the EMEP Protocol. For measurements with no defined protocols, it might be a good solution to use centralised laboratories to ensure comparability across the network. To cope with the introduction of these new measurements, new reporting guidelines have been developed to ensure that all proper information about the methodologies and data quality is given.
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| 2. |
- Angelbratt, Jon, 1981, et al.
(författare)
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A new method to detect long term trends of methane (CH4) and nitrous oxide (N2O) total columns measured within the NDACC ground-based high resolution solar FTIR network
- 2011
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:13, s. 6167-6183
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Tidskriftsartikel (refereegranskat)abstract
- Total columns measured with the ground-based solar FTIR technique are highly variable in time due to atmospheric chemistry and dynamics in the atmosphere above the measurement station. In this paper, a multiple regression model with anomalies of air pressure, total columns of hydrogen fluoride (HF) and carbon monoxide (CO) and tropopause height are used to reduce the variability in the methane (CH(4)) and nitrous oxide (N(2)O) total columns to estimate reliable linear trends with as small uncertainties as possible. The method is developed at the Harestua station (60 degrees N, 11 degrees E, 600 ma.s.l.) and used on three other European FTIR stations, i.e. Jungfraujoch (47 degrees N, 8 degrees E, 3600 ma.s.l.), Zugspitze (47 degrees N, 11 degrees E, 3000 ma.s.l.), and Kiruna (68 degrees N, 20 degrees E, 400 ma.s.l.). Linear CH(4) trends between 0.13 +/- 0.01-0.25 +/- 0.02% yr(-1) were estimated for all stations in the 1996-2009 period. A piecewise model with three separate linear trends, connected at change points, was used to estimate the short term fluctuations in the CH(4) total columns. This model shows a growth in 1996-1999 followed by a period of steady state until 2007. From 2007 until 2009 the atmospheric CH(4) amount increases between 0.57 +/- 0.22-1.15 +/- 0.17% yr(-1). Linear N(2)O trends between 0.19 +/- 0.01-0.40 +/- 0.02% yr(-1) were estimated for all stations in the 1996-2007 period, here with the strongest trend at Harestua and Kiruna and the lowest at the Alp stations. From the N(2)O total columns crude tropospheric and stratospheric partial columns were derived, indicating that the observed difference in the N(2)O trends between the FTIR sites is of stratospheric origin. This agrees well with the N(2)O measurements by the SMR instrument onboard the Odin satellite showing the highest trends at Harestua, 0.98 +/- 0.28% yr(-1), and considerably smaller trends at lower latitudes, 0.27 +/- 0.25% yr(-1). The multiple regression model was compared with two other trend methods, the ordinary linear regression and a Bootstrap algorithm. The multiple regression model estimated CH(4) and N(2)O trends that differed up to 31% compared to the other two methods and had uncertainties that were up to 300% lower. Since the multiple regression method were carefully validated this stresses the importance to account for variability in the total columns when estimating trend from solar FTIR data.
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| 3. |
- Angelbratt, Jon, 1981, et al.
(författare)
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Carbon monoxide (CO) and ethane (C2H6) trends from ground-based solar FTIR measurements at six European stations, comparison and sensitivity analysis with the EMEP model
- 2011
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:17, s. 9253-9269
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Tidskriftsartikel (refereegranskat)abstract
- Trends in the CO and C(2)H(6) partial columns (similar to 0-15 km) have been estimated from four European ground-based solar FTIR (Fourier Transform InfraRed) stations for the 1996-2006 time period. The CO trends from the four stations Jungfraujoch, Zugspitze, Harestua and Kiruna have been estimated to -0.45 +/- 0.16%yr(-1), -1.00 +/- 0.24%yr(-1), -0.62 +/- 0.19%yr(-1) and -0.61 +/- 0.16%yr(-1), respectively. The corresponding trends for C(2)H(6) are -1.51 +/- 0.23%yr(-1), -2.11 +/- 0.30%yr(-1), -1.09 +/- 0.25%yr(-1) and -1.14 +/- 0.18%yr(-1). All trends are presented with their 2-sigma confidence intervals. To find possible reasons for the CO trends, the global-scale EMEP MSC-W chemical transport model has been used in a series of sensitivity scenarios. It is shown that the trends are consistent with the combination of a 20% decrease in the anthropogenic CO emissions seen in Europe and North America during the 1996-2006 period and a 20% increase in the anthropogenic CO emissions in East Asia, during the same time period. The possible impacts of CH(4) and biogenic volatile organic compounds (BVOCs) are also considered. The European and global-scale EMEP models have been evaluated against the measured CO and C(2)H(6) partial columns from Jungfraujoch, Zugspitze, Bremen, Harestua, Kiruna and Ny-Alesund. The European model reproduces, on average the measurements at the different sites fairly well and within 10-22% deviation for CO and 14-31% deviation for C(2)H(6). Their seasonal amplitude is captured within 6-35% and 9-124% for CO and C(2)H(6), respectively. However, 61-98% of the CO and C(2)H(6) partial columns in the European model are shown to arise from the boundary conditions, making the global-scale model a more suitable alternative when modeling these two species. In the evaluation of the global model the average partial columns for 2006 are shown to be within 1-9% and 37-50% of the measurements for CO and C(2)H(6), respectively. The global model sensitivity for assumptions made in this paper is also analyzed.
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| 4. |
- Angot, H., et al.
(författare)
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Chemical cycling and deposition of atmospheric mercury in polar regions: review of recent measurements and comparison with models
- 2016
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:16, s. 10735-10763
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Tidskriftsartikel (refereegranskat)abstract
- Mercury (Hg) is a worldwide contaminant that can cause adverse health effects to wildlife and humans. While atmospheric modeling traces the link from emissions to deposition of Hg onto environmental surfaces, large uncertainties arise from our incomplete understanding of atmospheric processes (oxidation pathways, deposition, and re-emission). Atmospheric Hg reactivity is exacerbated in high latitudes and there is still much to be learned from polar regions in terms of atmospheric processes. This paper provides a synthesis of the atmospheric Hg monitoring data available in recent years (2011-2015) in the Arctic and in Antarctica along with a comparison of these observations with numerical simulations using four cutting-edge global models. The cycle of atmospheric Hg in the Arctic and in Antarctica presents both similarities and differences. Coastal sites in the two regions are both influenced by springtime atmospheric Hg depletion events and by summertime snowpack re-emission and oceanic evasion of Hg. The cycle of atmospheric Hg differs between the two regions primarily because of their different geography. While Arctic sites are significantly influenced by northern hemispheric Hg emissions especially in winter, coastal Antarctic sites are significantly influenced by the reactivity observed on the East Antarctic ice sheet due to katabatic winds. Based on the comparison of multi-model simulations with observations, this paper discusses whether the processes that affect atmospheric Hg seasonality and inter-annual variability are appropriately represented in the models and identifies research gaps in our understanding of the atmospheric Hg cycling in high latitudes.
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| 5. |
- Barlakas, Vasileios, 1986, et al.
(författare)
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The sub-adiabatic model as a concept for evaluating the representation and radiative effects of low-level clouds in a high-resolution atmospheric model
- 2020
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:1, s. 303-322
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Tidskriftsartikel (refereegranskat)abstract
- The realistic representation of low-level clouds, including their radiative effects, in atmospheric models remains challenging. A sensitivity study is presented to establish a conceptual approach for the evaluation of low-level clouds and their radiative impact in a highly resolved atmospheric model. Considering simulations for six case days, the analysis supports the notion that the properties of clouds more closely match the assumptions of the sub-adiabatic rather than the vertically homogeneous cloud model, suggesting its use as the basis for evaluation. For the considered cases, 95.7% of the variance in cloud optical thickness is explained by the variance in the liquid water path, while the droplet number concentration and the sub-adiabatic fraction contribute only 3.5% and 0.2% to the total variance, respectively. A mean sub-adiabatic fraction of 0.45 is found, which exhibits strong inter-day variability. Applying a principal component analysis and subsequent varimax rotation to the considered set of nine properties, four dominating modes of variability are identified, which explain 97.7% of the total variance. The first and second components correspond to the cloud base and top height, and to liquid water path, optical thickness, and cloud geometrical extent, respectively, while the cloud droplet number concentration and the sub-adiabatic fraction are the strongest contributors to the third and fourth components. Using idealized offline radiative transfer calculations, it is confirmed that the shortwave and longwave cloud radiative effects exhibit little sensitivity to the vertical structure of clouds. This reconfirms, based on an unprecedented large set of highly resolved vertical cloud profiles, that the cloud optical thickness and the cloud top and bottom heights are the main factors dominating the shortwave and longwave radiative effect of clouds and should be evaluated together with radiative fluxes using observations to attribute model deficiencies in the radiative fluxes to deficiencies in the representation of clouds. Considering the different representations of cloud microphysical processes in atmospheric models, the analysis has been further extended and the deviations between the radiative impact of the single- and double-moment schemes are assessed. Contrasting the shortwave cloud radiative effect obtained from the double-moment scheme to that of a single-moment scheme, differences of about similar to 40 Wm(-2) and significant scatter are observed. The differences are attributable to a higher cloud albedo resulting from the high values of droplet number concentration in particular in the boundary layer predicted by the double-moment scheme, which reach median values of around similar to 600 cm(-3).
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| 6. |
- Baron, P., et al.
(författare)
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Observation of horizontal winds in the middle-atmosphere between 30 degrees S and 55 degrees N during the northern winter 2009-2010
- 2013
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 13:12, s. 6049-6064
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Tidskriftsartikel (refereegranskat)abstract
- Although the links between stratospheric dynamics, climate and weather have been demonstrated, direct observations of stratospheric winds are lacking, in particular at altitudes above 30 km. We report observations of winds between 8 and 0.01 hPa (similar to 35-80 km) from October 2009 to April 2010 by the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES) on the International Space Station. The altitude range covers the region between 35-60 km where previous space-borne wind instruments show a lack of sensitivity. Both zonal and meridional wind components were obtained, though not simultaneously, in the latitude range from 30 degrees S to 55 degrees N and with a single profile precision of 7-9 ms(-1) between 8 and 0.6 hPa and better than 20 ms(-1) at altitudes above. The vertical resolution is 5-7 km except in the upper part of the retrieval range (10 km at 0.01 hPa). In the region between 1-0.05 hPa, an absolute value of the mean difference 5 ms(-1)). In the mesosphere, SMILES and ECMWF zonal winds exhibit large differences (>20 ms(-1)), especially in the tropics. We illustrate our results by showing daily and monthly zonal wind variations, namely the semi-annual oscillation in the tropics and reversals of the flow direction between 50-55 degrees N during sudden stratospheric warmings. The daily comparison with ECMWF winds reveals that in the beginning of February, a significantly stronger zonal westward flow is measured in the tropics at 2 hPa compared to the flow computed in the analysis (difference of similar to 20 ms(-1)). The results show that the comparison between SMILES and ECMWF winds is not only relevant for the quality assessment of the new SMILES winds, but it also provides insights on the quality of the ECMWF winds themselves. Although the instrument was not specifically designed for measuring winds, the results demonstrate that space-borne sub-mm wave radiometers have the potential to provide good quality data for improving the stratospheric winds in atmospheric models.
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| 7. |
- Beecken, Jörg, 1982, et al.
(författare)
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Emission factors of SO2, NOx and particles from ships in Neva Bay from ground-based and helicopter-borne measurements and AIS-based modeling
- 2015
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 15:9, s. 5229-5241
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Tidskriftsartikel (refereegranskat)abstract
- Emission factors of SO2, NOx and size-distributed particle numbers were measured for approximately 300 different ships in the Gulf of Finland and Neva Bay area during two campaigns in August/September 2011 and June/July 2012. The measurements were carried out from a harbor vessel and from an Mi-8 helicopter downwind of passing ships. Other measurements were carried out from shore sites near the island of Kronstadt and along the Neva River in the urban area of Saint Petersburg. Most ships were running at reduced speed (10 kn), i.e., not at their optimal load. Vessels for domestic and international shipping were monitored. It was seen that the distribution of the SO2 emission factors is bi-modal, with averages of 4.6 and 18.2 gSO(2) kg(fuel)(-1) for the lower and the higher mode, respectively. The emission factors show compliance with the 1% fuel sulfur content Sulfur Emission Control Areas (SECA) limit for 90% of the vessels in 2011 and 97% in 2012. The distribution of the NOx emission factor is mono-modal, with an average of 58 gNO(x) kg(fuel)(-1). The corresponding emission related to the generated power yields an average of 12.1 gNO(x) kWh(-1). The distribution of the emission factors for particulate number shows that nearly 90% of all particles in the 5.6 nm to 10 mu m size range were below 70 nm in diameter. The distribution of the corresponding emission factors for the mass indicates two separated main modes, one for particles between 30 and 300 nm and the other for above 2 mu m. The average particle emission factors were found to be in the range from 0.7 to 2.7 x 10(16) particles kg(fuel)(-1) and 0.2 to 3.4 gPM kg(fuel)(-1), respectively. The NOx and particulate emissions are comparable with other studies. The measured emission factors were compared, for individual ships, to modeled ones using the Ship Traffic Emission Assessment Model (STEAM) of the Finnish Meteorological Institute. A reasonably good agreement for gaseous sulfur and nitrogen emissions can be seen for ships in international traffic, but significant deviations are found for inland vessels. Regarding particulate mass, the values of the modeled data are about 2-3 times higher than the measured results, which probably reflects the assumptions made in the modeled fuel sulfur content. The sulfur contents in the fuel retrieved from the measurements were lower than the previously used assumptions by the City of Saint Petersburg when carrying out atmospheric modeling, and using these measurements it was possible to better assess the impact of shipping on air quality.
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| 8. |
- Bergström, Robert, et al.
(författare)
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Biotic stress: a significant contributor to organic aerosol in Europe?
- 2014
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus Publications. - 1680-7316 .- 1680-7324. ; 14:24, s. 13643-13660
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Tidskriftsartikel (refereegranskat)abstract
- We have investigated the potential impact on organic aerosol formation from biotic stress-induced emissions (SIE) of organic molecules from forests in Europe (north of lat. 45° N). Emission estimates for sesquiterpenes (SQT), methyl salicylate (MeSA) and unsaturated C17 compounds, due to different stressors, are based on experiments in the Jülich Plant Atmosphere Chamber (JPAC), combined with estimates of the fraction of stressed trees in Europe based on reported observed tree damage. SIE were introduced in the EMEP MSC-W chemical transport model and secondary organic aerosol (SOA) yields from the SIE were taken from the JPAC experiments. Based on estimates of current levels of infestation and the JPAC aerosol yields, the model results suggest that the contribution to SOA in large parts of Europe may be substantial. It is possible that SIE contributes as much, or more, to organic aerosol than the constitutive biogenic VOC emissions, at least during some periods. Based on the assumptions in this study, SIE-SOA are estimated to constitute between 50 and 70 % of the total biogenic SOA (BSOA) in a current-situation scenario where the biotic stress in northern and central European forests causes large SIE of MeSA and SQT. An alternative current-situation scenario with lower SIE, consisting solely of SQT, leads to lower SIE-SOA, between 20 and 40 % of the total BSOA. Hypothetical future scenarios with increased SIE, due to higher degrees of biotic stress, show that SOA formation due to SIE can become even larger. Unsaturated C17 BVOC (biogenic volatile organic compounds) emitted by spruce infested by the forest-honey generating bark louse, Cinara pilicornis, have a high SOA-forming potential. A model scenario investigating the effect of a regional, episodic infestation of Cinara pilicornis in Baden-Württemberg, corresponding to a year with high production of forest honey, shows that these types of events could lead to very large organic aerosol formation in the infested region. We have used the best available laboratory data on biotic SIE applicable to northern and central European forests. Using these data and associated assumptions, we have shown that SIE are potentially important for SOA formation but the magnitude of the impact is uncertain and needs to be constrained by further laboratory, field and modelling studies. As an example, the MeSA, which is released as a consequence of various types of biotic stress, is found to have a potentially large impact on SIE-SOA in Europe, but different assumptions regarding the nighttime chemistry of MeSA can change its SOA potential substantially. Thus, further investigations of the atmospheric chemistry of MeSA and observational field studies are needed to clarify the role of this compound in the atmosphere.
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| 9. |
- Bergström, Robert, et al.
(författare)
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Modelling of organic aerosols over Europe (2002-2007) using a volatility basis set (VBS) framework: application of different assumptions regarding the formation of secondary organic aerosol
- 2012
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:18, s. 8499-8527
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Tidskriftsartikel (refereegranskat)abstract
- A new organic aerosol module has been implemented into the EMEP chemical transport model. Four different volatility basis set (VBS) schemes have been tested in long-term simulations for Europe, covering the six years 2002-2007. Different assumptions regarding partitioning of primary organic aerosol and aging of primary semi-volatile and intermediate volatility organic carbon (S/IVOC) species and secondary organic aerosol (SOA) have been explored. Model results are compared to filter measurements, aerosol mass spectrometry (AMS) data and source apportionment studies, as well as to other model studies. The present study indicates that many different sources contribute significantly to organic aerosol in Europe. Biogenic and anthropogenic SOA, residential wood combustion and vegetation fire emissions may all contribute more than 10% each over substantial parts of Europe. This study shows smaller contributions from biogenic SOA to organic aerosol in Europe than earlier work, but relatively greater anthropogenic SOA. Simple VBS based organic aerosol models can give reasonably good results for summer conditions but more observational studies are needed to constrain the VBS parameterisations and to help improve emission inventories. The volatility distribution of primary emissions is one important issue for further work. Emissions of volatile organic compounds from biogenic sources are also highly uncertain and need further validation. We can not reproduce winter levels of organic aerosol in Europe, and there are many indications that the present emission inventories substantially underestimate emissions from residential wood combustion in large parts of Europe.
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| 10. |
- Boman, Johan, 1955, et al.
(författare)
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Elemental content of PM2.5 aerosol particles collected in Göteborg during the Göte-2005 campaign in February 2005
- 2009
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 9, s. 2597-2606
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Tidskriftsartikel (refereegranskat)abstract
- The Göte-2005 measurement campaign aimed at studying the influence of the winter thermal inversions on urban air pollution. Elemental speciation of PM2.5 aerosol particles, collected on Teflon filters at three urban sites and one rural site in the Göteborg region, was a major part of the study. Trace element analysis was done by Energy Dispersive X-Ray Fluorescence (EDXRF) spectrometry and the concentrations of S, Cl, K, Ca, Ti, V, Mn, Fe, Ni, Cu, Zn, Br and Pb were determined. The elemental content of the particles, local wind speed and direction, and backward trajectories were used to investigate possible sources for the pollutants. We concluded that S, V, Ni, Br, and Pb had their main sources outside the central Göteborg area, since elevated concentrations of these elements were not observed during an inversion episode. Sea traffic and harbour activities were identified, primarily by the S and V content of the particles. This study showed that the elemental analysis by EDXRF presents valuable information for tracing the origin of air masses arriving at a measurement site.
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