| 11. |
- Kiendler-Scharr, A., et al.
(författare)
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Ubiquity of organic nitrates from nighttime chemistry in the European submicron aerosol
- 2016
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Ingår i: Geophysical Research Letters. - 0094-8276. ; 43:14, s. 7735-7744
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Tidskriftsartikel (refereegranskat)abstract
- In the atmosphere nighttime removal of volatile organic compounds is initiated to a large extent by reaction with the nitrate radical (NO3) forming organic nitrates which partition between gas and particulate phase. Here we show based on particle phase measurements performed at a suburban site in the Netherlands that organic nitrates contribute substantially to particulate nitrate and organic mass. Comparisons with a chemistry transport model indicate that most of the measured particulate organic nitrates are formed by NO3 oxidation. Using aerosol composition data from three intensive observation periods at numerous measurement sites across Europe, we conclude that organic nitrates are a considerable fraction of fine particulate matter (PM1) at the continental scale. Organic nitrates represent 34% to 44% of measured submicron aerosol nitrate and are found at all urban and rural sites, implying a substantial potential of PM reduction by NOx emission control.
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| 12. |
- Knote, C., et al.
(författare)
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Towards an online-coupled chemistry-climate model: evaluation of trace gases and aerosols in COSMO-ART
- 2011
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Ingår i: Geoscientific Model Development. - : Copernicus GmbH. - 1991-959X .- 1991-9603. ; 4:4, s. 1077-1102
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Tidskriftsartikel (refereegranskat)abstract
- The online-coupled, regional chemistry transport model COSMO-ART is evaluated for periods in all seasons against several measurement datasets to assess its ability to represent gaseous pollutants and ambient aerosol characteristics over the European domain. Measurements used in the comparison include long-term station observations, satellite and ground-based remote sensing products, and complex datasets of aerosol chemical composition and number size distribution from recent field campaigns. This is the first time these comprehensive measurements of aerosol characteristics in Europe are used to evaluate a regional chemistry transport model. We show a detailed analysis of the simulated size-resolved chemical composition under different meteorological conditions. Mean, variability and spatial distribution of the concentrations of O-3 and NOx are well reproduced. SO2 is found to be overestimated, simulated PM2.5 and PM10 levels are on average underestimated, as is AOD. We find indications of an overestimation of shipping emissions. Time evolution of aerosol chemical composition is captured, although some biases are found in relative composition. Nitrate aerosol components are on average overestimated, and sulfates underestimated. The accuracy of simulated organics depends strongly on season and location. While strongly underestimated during summer, organic mass is comparable in spring and autumn. We see indications for an overestimated fractional contribution of primary organic matter in urban areas and an underestimation of SOA at many locations. Aerosol number concentrations compare well with measurements for larger size ranges, but overestimations of particle number concentration with factors of 2-5 are found for particles smaller than 50 nm. Size distribution characteristics are often close to measurements, but show discrepancies at polluted sites. Suggestions for further improvement of the modeling system consist of the inclusion of a revised secondary organic aerosols scheme, aqueous-phase chemistry and improved aerosol boundary conditions. Our work sets the basis for subsequent studies of aerosol characteristics and climate impacts with COSMO-ART, and highlights areas where improvements are necessary for current regional modeling systems in general.
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| 13. |
- Kulmala, M., et al.
(författare)
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General overview: European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) - integrating aerosol research from nano to global scales
- 2011
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:24, s. 13061-13143
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Tidskriftsartikel (refereegranskat)abstract
- In this paper we describe and summarize the main achievements of the European Aerosol Cloud Climate and Air Quality Interactions project (EUCAARI). EUCAARI started on 1 January 2007 and ended on 31 December 2010 leaving a rich legacy including: (a) a comprehensive database with a year of observations of the physical, chemical and optical properties of aerosol particles over Europe, (b) comprehensive aerosol measurements in four developing countries, (c) a database of airborne measurements of aerosols and clouds over Europe during May 2008, (d) comprehensive modeling tools to study aerosol processes fron nano to global scale and their effects on climate and air quality. In addition a new Pan-European aerosol emissions inventory was developed and evaluated, a new cluster spectrometer was built and tested in the field and several new aerosol parameterizations and computations modules for chemical transport and global climate models were developed and evaluated. These achievements and related studies have substantially improved our understanding and reduced the uncertainties of aerosol radiative forcing and air quality-climate interactions. The EUCAARI results can be utilized in European and global environmental policy to assess the aerosol impacts and the corresponding abatement strategies.
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| 14. |
- Li, J. J., et al.
(författare)
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Characterization of Aerosol Aging Potentials at Suburban Sites in Northern and Southern China Utilizing a Potential Aerosol Mass (Go:PAM) Reactor and an Aerosol Mass Spectrometer
- 2019
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Ingår i: Journal of Geophysical Research-Atmospheres. - : American Geophysical Union (AGU). - 2169-897X .- 2169-8996. ; 124:10, s. 5629-5649
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Tidskriftsartikel (refereegranskat)abstract
- Aerosol mass spectrometry was used to characterize submicron aerosols before and after aging in a Gothenburg Potential Aerosol Mass (Go:PAM) reactor at two suburban sites in China, one in northern China at Changping (CP), Beijing, and a second in southern China at Hong Kong (HK). Organic aerosol (OA) dominated in the ambient nonrefractory particulate matter <1m (NR-PM1) for both CP (42-71%) and HK (43-61%), with a large contribution from secondary OA factors that were semivolatile oxygenated (SVOOA) and low-volatility oxygenated (LVOOA). Under constant OH exposure, OA enhancement (78-98%) dominated the NR-PM1 mass increment at both sites, while nitrate was enhanced the most among the inorganic species (7-9%). Overall, the CP site exhibited higher OA oxidation potential and more enhancement of SVOOA than LVOOA (7.5 vs. 2.7g/m(3)), but the reverse was observed in HK (0.8 vs. 2.6g/m(3)). In CP, more enhancement of the less oxygenated SVOOA suggests that aerosol aging was more sensitive to the abundant locally emitted primary OA and volatile organic compound precursors. On the contrary, the more formation of the highly oxidized LVOOA in HK indicates that aerosol aging mainly escalated the degree of oxygenation of OA as ambient aerosol was already quite aged and there was a lack of volatile organic compound precursors. The comparative measurements using the same oxidation system reveal distinct key factors and mechanisms that influence secondary aerosol formation in two suburban locations in China, providing scientific insights to assist formulation of location-specific mitigation measures of secondary pollution. Plain Language Summary Atmospheric submicron particles have significant impacts on the climate and human health. A large part of these particles are formed secondarily through successive aging of primary emissions. To study such aging processes, we used a reactor that can provide highly oxidizing conditions to simulate the oxidation of ambient aerosols at accelerated rates. An online mass spectrometer was connected after the reactor to measure changes in aerosol mass concentration and chemical composition between the ambient samples and the oxidized ones. We presented the first comparative measurements of the aging potentials of ambient aerosols in two suburban sites in northern and southern China (Changping District in Beijing, and Hong Kong). Results showed that generally aerosols at the Changping site had higher aging potentials after passing through the oxidation reactor, probably due to more local emissions of precursors, while air masses in Hong Kong were already in a higher oxidation state with lower aging potentials, mainly because of strong impacts from long-range transported pollution sources. Distinct aerosol aging pathways related to different ambient precursors were observed at the two sites. Understanding of the different characteristics of aerosol aging processes can lead to advances in air quality modeling and pollution management.
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| 15. |
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| 16. |
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| 17. |
- Liu, L., et al.
(författare)
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Photochemical modelling in the Po basin with focus on formaldehyde and ozone
- 2007
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 7, s. 121-137
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Tidskriftsartikel (refereegranskat)abstract
- As part of the EU project FORMAT ( Formaldehyde as a Tracer of Oxidation in the Troposphere), a field campaign was carried out in the vicinity of Milan during the summer of 2002. Results from a 3-D regional chemical transport model (NILU RCTM) were used to interpret the observations focusing primarily on HCHO and ozone. The performance of the model was assessed by comparing model results with ground based and aircraft measurements. The model results show good agreement with surface measurements, and the model is able to reproduce the photochemical episodes during fair weather days. The comparison indicates that the model can represent well the HCHO concentrations as well as their temporal and spatial variability. The relationship between HCHO and (O-3 x H2O) was used to validate the model ability to predict the HCHO concentrations. Further analysis revealed the importance of the representativeness of different instruments: in-situ concentrations might be locally enhanced by emissions, while long path measurements over a forest can be influenced by rapid formation of HCHO from isoprene. The model is able to capture the plume from the city of Milan and the modelled levels agree generally well with the aircraft measurements, although the wind fields used in the model can lead to a displacement of the ozone plume. During the campaign period, O3 levels were seldom higher than 80 ppb, the peak surface ozone maxima reached 90 ppb. Those relatively low values can be explained by low emissions during the August vacation and unstable weather conditions in this period. The modelled Delta O-3/Delta NOz slope at Alzate of 5.1 agrees well with the measured slope of 4.9.
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| 18. |
- Meyer, N. K., et al.
(författare)
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Analysis of the hygroscopic and volatile properties of ammonium sulphate seeded and unseeded SOA particles
- 2009
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Ingår i: Atmos. Chem. Phys.. ; 9, s. 721-732
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Tidskriftsartikel (refereegranskat)abstract
- The volatile and hygroscopic properties of ammonium sulphate seeded and unseeded secondary organic aerosol (SOA) derived from the photo-oxidation of atmospherically relevant concentrations of α-pinene were studied. The seed particles were electrospray generated ammonium sulphate ((NH4)2SO4) having diameters of approximately 33 nm with a quasi-mono-disperse size distribution (geometric standard deviation σg=1.3). The volatile and hygroscopic properties of both seeded and unseeded SOA were simultaneously measured with a VH-TDMA (volatility – hygroscopicity tandem differential mobility analyzer). VH-TDMA measurements of unseeded SOA show a decrease in the hygroscopic growth (HGF) factor for increased volatilisation temperatures such that the more volatile compounds appear to be more hygroscopic. This is opposite to the expected preferential evaporation of more volatile but less hygroscopic material, but could also be due to enhanced oligomerisation occurring at the higher temperature in the thermodenuder. In addition, HGF measurements of seeded SOA were measured as a function of time at two relative humidities, below (RH 75%) and above (RH 85%) the deliquescence relative humidity (DRH) of the pure ammonium sulphate seeds. As these measurements were conducted during the onset phase of photo-oxidation, during particle growth, they enabled us to find the dependence of the HGF as a function of the volume fraction of the SOA coating. HGF's measured at RH of 85% showed a continuous decrease as the SOA coating thickness increased. The measured growth factors show good agreements with ZSR predictions indicating that, at these RH values, there are only minor solute-solute interactions. At 75% RH, as the SOA fraction increased, a rapid increase in the HGF was observed indicating that an increasing fraction of the (NH4)2SO4 is subject to a phase transition, going into solution, with an increasing volume fraction of SOA. To our knowledge this is the first time that SOA derived from photo-oxidised α-pinene has been shown to affect the equilibrium water content of inorganic aerosols below their DRH. For SOA volume fractions above ~0.3 the measured growth factor followed roughly parallel to the ZSR prediction based on fully dissolved (NH4)2SO4 although with a small difference that was just larger than the error estimate. Both incomplete dissolution and negative solute-solute interactions could be responsible for the lower HGF observed compared to the ZSR predictions.
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| 19. |
- Monks, P. S., et al.
(författare)
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Atmospheric composition change : global and regional air quality
- 2009
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Ingår i: Atmospheric Environment. - : Elsevier BV. - 1352-2310 .- 1873-2844. ; 43:33, s. 5268-5350
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Forskningsöversikt (refereegranskat)abstract
- Air quality transcends all scales with in the atmosphere from the local to the global with handovers and feedbacks at each scale interaction. Air quality has manifold effects on health, ecosystems heritage and, climate. In this review the state of scientific understanding in relation to global and regional air quality is outlined. The review discusses air quality, in terms of emissions, processing and transport of trace gases and aerosols. New insights into the characterization of both natural and anthropogenic emissions are reviewed looking at both natural (e.g. dust and lightning) as well as plant emissions. Trends in anthropogenic emissions both by region and globally are discussed as well as biomass burning emissions. In terms of chemical processing the major air quality elements of ozone, non-methane hydrocarbons, nitrogen oxides and aerosols are covered. A number of topics are presented as a way of integrating the process view into the atmospheric context; these include the atmospheric oxidation efficiency, halogen and HOx chemistry, nighttime chemistry, tropical chemistry, heat waves, megacities, biomass burning and the regional hot spot of the Mediterranean. New findings with respect to the transport of pollutants across the scales are discussed, in particular the move to quantify the impact of long-range transport on regional air quality. Gaps and research questions that remain intractable are identified. The review concludes with a focus of research and policy questions for the coming decade. In particular, the policy challenges for concerted air quality and climate change policy (co-benefit) are discussed.
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| 20. |
- Nøjgaard, J. K., et al.
(författare)
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A local marine source of atmospheric particles in the High Arctic
- 2022
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Ingår i: Atmospheric Environment. - : Elsevier BV. - 1352-2310. ; 285
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Tidskriftsartikel (refereegranskat)abstract
- The chemical composition of non-refractory submicron aerosol (NR-PM1) was characterized at the Villum Research Station (Villum) at Station Nord in North Greenland during spring-summer 2016 using a Time of Flight Aerosol Chemical Speciation Monitor (ToF-ACSM). The composition is dominated by sulfate (48%) and organic species (40%). Positive Matrix Factorization (PMF) identified three key factors corresponding to a primary hydrocarbon-like organic aerosol (HOA), and two types of secondary organic aerosol: oxygenated organic aerosol (OOA) and a marine organic aerosol (MOA). The HOA factor accounts for 5% of the organic aerosol mass, which is consistent with previous findings at Villum. The OOA factor accounts for 77% of the organic aerosol mass and correlates with accumulation mode particles, which supports previous findings indicating that oxidized organic aerosols are predominantly from long-range transport during winter and spring at Villum. The MOA factor was characterized by mass spectral fragments of methane sulfonic acid (MSA) from atmospheric oxidation of dimethyl sulfide, for which reason the MOA factor is considered to be of biogenic origin. MOA accounts for 18% of the organic aerosol mass and correlates with locally produced Aitken mode particles. This indicates that biogenic processes are not only a significant source of aerosols at Villum, but MOA also appears to be formed in the vicinity of the measurement site. This local geographical origin was confirmed through air mass back trajectory modelling and source-receptor analysis. During May, air masses frequently arrived from the east, with source regions for the MOA factor and therewith MSA located in the Barents Sea and Lincoln Sea with lesser contributions from the Greenland Sea. During June, air mass origin shifted to the west, with source regions for the MOA factor and MSA shifting correspondingly to Baffin Bay and the Canadian Arctic Archipelago. While shifting transport patterns between May and June lead to shifting source regions, sea ice likely played a role as well. During May, marginal ice zones were present in the Barents Sea between Svalbard and Franz Josef Land, while during June, sea ice in the northern part of Baffin Bay retreated and sea ice in the Canadian Arctic Archipelago decreased. Although May and June experienced different transport patterns and sea ice conditions, levels of the MOA factor and MSA were similar between the months. This is likely due to similarities between marine biological activities in the Barents Sea and Baffin Bay. This research highlights the complex relationship between transport patterns, sea ice conditions, and atmospheric particle concentrations. Multiyear aerosol chemical composition from several High Arctic sites is encouraged to determine the full effects of ocean-atmosphere interactions and transport patterns on atmospheric aerosol concentrations.
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