| 1. |
- Almeida, Joao, et al.
(författare)
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Molecular understanding of sulphuric acid-amine particle nucleation in the atmosphere
- 2013
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Ingår i: Nature. - : Springer Science and Business Media LLC. - 0028-0836 .- 1476-4687. ; 502:7471, s. 359-
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Tidskriftsartikel (refereegranskat)abstract
- Nucleation of aerosol particles from trace atmospheric vapours is thought to provide up to half of global cloud condensation nuclei(1). Aerosols can cause a net cooling of climate by scattering sunlight and by leading to smaller but more numerous cloud droplets, which makes clouds brighter and extends their lifetimes(2). Atmospheric aerosols derived from human activities are thought to have compensated for a large fraction of the warming caused by greenhouse gases(2). However, despite its importance for climate, atmospheric nucleation is poorly understood. Recently, it has been shown that sulphuric acid and ammonia cannot explain particle formation rates observed in the lower atmosphere(3). It is thought that amines may enhance nucleation(4-16), but until now there has been no direct evidence for amine ternary nucleation under atmospheric conditions. Here we use the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN and find that dimethylamine above three parts per trillion by volume can enhance particle formation rates more than 1,000-fold compared with ammonia, sufficient to account for the particle formation rates observed in the atmosphere. Molecular analysis of the clusters reveals that the faster nucleation is explained by a base-stabilization mechanism involving acid-amine pairs, which strongly decrease evaporation. The ion-induced contribution is generally small, reflecting the high stability of sulphuric acid-dimethylamine clusters and indicating that galactic cosmic rays exert only a small influence on their formation, except at low overall formation rates. Our experimental measurements are well reproduced by a dynamical model based on quantum chemical calculations of binding energies of molecular clusters, without any fitted parameters. These results show that, in regions of the atmosphere near amine sources, both amines and sulphur dioxide should be considered when assessing the impact of anthropogenic activities on particle formation.
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| 2. |
- Cai, Jing, et al.
(författare)
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Size-segregated particle number and mass concentrations from different emission sources in urban Beijing
- 2020
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:21, s. 12721-12740
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Tidskriftsartikel (refereegranskat)abstract
- Although secondary particulate matter is reported to be the main contributor of PM2.5 during haze in Chinese megacities, primary particle emissions also affect particle concentrations. In order to improve estimates of the contribution of primary sources to the particle number and mass concentrations, we performed source apportionment analyses using both chemical fingerprints and particle size distributions measured at the same site in urban Beijing from April to July 2018. Both methods resolved factors related to primary emissions, including vehicular emissions and cooking emissions, which together make up 76% and 24% of total particle number and organic aerosol (OA) mass, respectively. Similar source types, including particles related to vehicular emissions (1.6 +/- 1.1 mu gm(-3); 2.4 +/- 1.8 x 10(3) cm(-3) and 5.5 +/- 2.8 x 10(3) cm(-3) for two traffic-related components), cooking emissions (2.6 +/- 1.9 mu gm(-3) and 5.5 +/- 3.3 x 10(3) cm(-3)) and secondary aerosols (51 +/- 41 mu gm(-3) and 4.2 +/- 3.0 x 10(3) cm(-3)), were resolved by both methods. Converted mass concentrations from particle size distributions components were comparable with those from chemical fingerprints. Size distribution source apportionment separated vehicular emissions into a component with a mode diameter of 20 nm (traffic-ultrafine) and a component with a mode diameter of 100 nm (traffic-fine). Consistent with similar day- and nighttime diesel vehicle PM2.5 emissions estimated for the Beijing area, traffic-fine particles, hydrocarbon-like OA (HOA, traffic-related factor resulting from source apportionment using chemical fingerprints) and black carbon (BC) showed similar diurnal patterns, with higher concentrations during the night and morning than during the afternoon when the boundary layer is higher. Traffic-ultrafine particles showed the highest concentrations during the rush-hour period, suggesting a prominent role of local gasoline vehicle emissions. In the absence of new particle formation, our re-sults show that vehicular-related emissions (14% and 30% for ultrafine and fine particles, respectively) and cooking-activity-related emissions (32 %) dominate the particle number concentration, while secondary particulate matter (over 80 %) governs PM2.5 mass during the non-heating season in Beijing.
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| 3. |
- Hussein, Tareq, et al.
(författare)
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Modeling regional deposited dose of submicron aerosol particles
- 2013
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Ingår i: Science of the Total Environment. - : Elsevier BV. - 1879-1026 .- 0048-9697. ; 458, s. 140-149
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Tidskriftsartikel (refereegranskat)abstract
- We developed a simple model to calculate the regional deposited dose of submicron aerosol particles in the respiratory system. This model incorporates measured outdoor and modeled indoor particle number size distributions, detailed activity patterns of three age groups (teens, adults, and the elderly), semi-empirical estimation of the regional deposition fraction, hygroscopic properties of urban aerosols, and reported breathing minute volumes. We calculated the total and regional deposited dose based on three concentration metrics: particle number (PN), mass (PM), and surface area (PSA). The 24-h total deposited dose of fine particles in adult males was around 40 mu g (57 x 109 particles, 8 x 102 mm(2)) and 41 mu g (40 x 109 particles, 8 x 102 mm(2)) on workdays and weekends, respectively. The total and regional 24-h deposited dose based on any of the metrics was at most 1.5 times higher in males than in females. The deposited dose values in the other age groups were slightly different than in adults. Regardless of the particle size fraction or the deposited dose metric, the pulmonary/alveolar region received the largest fraction of the deposited dose. These values represent the lowest estimate of the deposited dose and they are expected to be higher in real-life conditions after considering indoor sources of aerosol particles and spatial variability of outdoor aerosols. This model can be extended to youngsters (<12 years old) after gaining accurate information about the deposition fraction inside their respiratory system and their breathing pattern. This investigation is foreseen to bridge the gap between exposure and response in epidemiological studies. (C) 2013 Elsevier B.V. All rights reserved.
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| 4. |
- Kulmala, Markku, et al.
(författare)
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CO2-induced terrestrial climate feedback mechanism : From carbon sink to aerosol source and back
- 2014
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Ingår i: Boreal environment research. - 1239-6095 .- 1797-2469. ; 19, s. 122-131
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Tidskriftsartikel (refereegranskat)abstract
- Feedbacks mechanisms are essential components of our climate system, as they either increase or decrease changes in climate-related quantities in the presence of external forcings. In this work, we provide the first quantitative estimate regarding the terrestrial climate feedback loop connecting the increasing atmospheric carbon dioxide concentration, changes in gross primary production (GPP) associated with the carbon uptake, organic aerosol formation in the atmosphere, and transfer of both diffuse and global radiation. Our approach was to combine process-level understanding with comprehensive, long-term field measurement data set collected from a boreal forest site in southern Finland. Our best estimate of the gain in GPP resulting from the feedback is 1.3 (range 1.02-1.5), which is larger than the gains of the few atmospheric chemistry-climate feedbacks estimated using large-scale models. Our analysis demonstrates the power of using comprehensive field measurements in investigating the complicated couplings between the biosphere and atmosphere on one hand, and the need for complementary approaches relying on the combination of field data, satellite observations model simulations on the other hand.
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| 5. |
- Kulmala, Markku, et al.
(författare)
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Measurement of the nucleation of atmospheric aerosol particles
- 2012
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Ingår i: Nature Protocols. - : Springer Science and Business Media LLC. - 1754-2189 .- 1750-2799. ; 7:9, s. 1651-1667
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Tidskriftsartikel (refereegranskat)abstract
- The formation of new atmospheric aerosol particles and their subsequent growth have been observed frequently at various locations all over the world. The atmospheric nucleation rate (or formation rate) and growth rate (GR) are key parameters to characterize the phenomenon. Recent progress in measurement techniques enables us to measure atmospheric nucleation at the size (mobility diameter) of 1.5 (+/- 0.4) nm. The detection limit has decreased from 3 to 1 nm within the past 10 years. In this protocol, we describe the procedures for identifying new-particle-formation (NPF) events, and for determining the nucleation, formation and growth rates during such events under atmospheric conditions. We describe the present instrumentation, best practices and other tools used to investigate atmospheric nucleation and NPF at a certain mobility diameter (1.5, 2.0 or 3.0 nm). The key instruments comprise devices capable of measuring the number concentration of the formed nanoparticles and their size, such as a suite of modern condensation particle counters (CPCs) and air ion spectrometers, and devices for characterizing the pre-existing particle number concentration distribution, such as a differential mobility particle sizer (DMPS). We also discuss the reliability of the methods used and requirements for proper measurements and data analysis. The time scale for realizing this procedure is 1 year.
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| 6. |
- Kyro, Ella-Maria, et al.
(författare)
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Long-term Aerosol and Trace Gas Measurements in Eastern Lapland, Finland : The Impact of Kola Air Pollution to New Particle Formation
- 2013
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Ingår i: NUCLEATION AND ATMOSPHERIC AEROSOLS. - : American Institute of Physics (AIP). - 9780735411524 ; , s. 409-412
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Konferensbidrag (refereegranskat)abstract
- Sulfur emissions from the Kola Peninsula smelter industry have been decreasing over the past two decades. We investigated the effect of this to new particle formation at SMEAR I station in Eastern Lapland, Finland, using long-term measurements of trace gases and aerosol size distributions. We show that the number of events per year has decreased and can be linked with the decreasing sulfur emissions from Kola.
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| 7. |
- Laj, Paolo, et al.
(författare)
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A global analysis of climate-relevant aerosol properties retrieved from the network of Global Atmosphere Watch (GAW) near-surface observatories
- 2020
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Ingår i: Atmospheric Measurement Techniques. - : Copernicus GmbH. - 1867-1381 .- 1867-8548. ; 13:8, s. 4353-4392
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Tidskriftsartikel (refereegranskat)abstract
- Aerosol particles are essential constituents of the Earth's atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence times, resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in situ near-surface segment of the atmospheric observation system. This paper will provide the widest effort so far to document variability of climate-relevant in situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High-quality data from almost 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single-scattering albedo, and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information, including data provision procedures, quality control and analysis, data policy, and usage of the ground-based aerosol measurement network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system.
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| 8. |
- Lappalainen, Hanna K., et al.
(författare)
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Pan-Eurasian Experiment (PEEX) : towards a holistic understanding of the feedbacks and interactions in the land-atmosphere-ocean-society continuum in the northern Eurasian region
- 2016
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:22, s. 14421-14461
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Tidskriftsartikel (refereegranskat)abstract
- The northern Eurasian regions and Arctic Ocean will very likely undergo substantial changes during the next decades. The Arctic-boreal natural environments play a crucial role in the global climate via albedo change, carbon sources and sinks as well as atmospheric aerosol production from biogenic volatile organic compounds. Furthermore, it is expected that global trade activities, demographic movement, and use of natural resources will be increasing in the Arctic regions. There is a need for a novel research approach, which not only identifies and tackles the relevant multi-disciplinary research questions, but also is able to make a holistic system analysis of the expected feedbacks. In this paper, we introduce the research agenda of the Pan-Eurasian Experiment (PEEX), a multi-scale, multi-disciplinary and international program started in 2012 (https://www.atm.helsinki.fi/peex/). PEEX sets a research approach by which large-scale research topics are investigated from a system perspective and which aims to fill the key gaps in our understanding of the feedbacks and interactions between the land-atmosphereaquatic-society continuum in the northern Eurasian region. We introduce here the state of the art for the key topics in the PEEX research agenda and present the future prospects of the research, which we see relevant in this context.
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| 9. |
- Lawler, Michael J., et al.
(författare)
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Unexpectedly acidic nanoparticles formed in dimethylamine-ammonia-sulfuric-acid nucleation experiments at CLOUD
- 2016
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:21, s. 13601-13618
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Tidskriftsartikel (refereegranskat)abstract
- New particle formation driven by acid-base chemistry was initiated in the CLOUD chamber at CERN by introducing atmospherically relevant levels of gas-phase sulfuric acid and dimethylamine (DMA). Ammonia was also present in the chamber as a gas-phase contaminant from earlier experiments. The composition of particles with volume median diameters (VMDs) as small as 10 nm was measured by the Thermal Desorption Chemical Ionization Mass Spectrometer (TDCIMS). Particulate ammonium-to-dimethylaminium ratios were higher than the gas-phase ammonia-to-DMA ratios, suggesting preferential uptake of ammonia over DMA for the collected 10-30 nm VMD particles. This behavior is not consistent with present nanoparticle physicochemical models, which predict a higher dimethylaminium fraction when NH3 and DMA are present at similar gas-phase concentrations. Despite the presence in the gas phase of at least 100 times higher base concentrations than sulfuric acid, the recently formed particles always had measured base : acid ratios lower than 1 : 1. The lowest base fractions were found in particles below 15 nm VMD, with a strong size-dependent composition gradient. The reasons for the very acidic composition remain uncertain, but a plausible explanation is that the particles did not reach thermodynamic equilibrium with respect to the bases due to rapid heterogeneous conversion of SO2 to sulfate. These results indicate that sulfuric acid does not require stabilization by ammonium or dimethylaminium as acid-base pairs in particles as small as 10 nm.
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| 10. |
- Lehtipalo, Katrianne, et al.
(författare)
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Multicomponent new particle formation from sulfuric acid, ammonia, and biogenic vapors
- 2018
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Ingår i: Science Advances. - : American Association for the Advancement of Science (AAAS). - 2375-2548. ; 4:12
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Tidskriftsartikel (refereegranskat)abstract
- A major fraction of atmospheric aerosol particles, which affect both air quality and climate, form from gaseous precursors in the atmosphere. Highly oxygenated organic molecules (HOMs), formed by oxidation of biogenic volatile organic compounds, are known to participate in particle formation and growth. However, it is not well understood how they interact with atmospheric pollutants, such as nitrogen oxides (NOx) and sulfur oxides (SOx) from fossil fuel combustion, as well as ammonia (NH3) from livestock and fertilizers. Here, we show how NOx suppresses particle formation, while HOMs, sulfuric acid, and NH3 have a synergistic enhancing effect on particle formation. We postulate a novel mechanism, involving HOMs, sulfuric acid, and ammonia, which is able to closely reproduce observations of particle formation and growth in daytime boreal forest and similar environments. The findings elucidate the complex interactions between biogenic and anthropogenic vapors in the atmospheric aerosol system.
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| 11. |
- Nieminen, Tuomo, et al.
(författare)
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Global analysis of continental boundary layer new particle formation based on long-term measurements
- 2018
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 18:19, s. 14737-14756
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Tidskriftsartikel (refereegranskat)abstract
- Atmospheric new particle formation (NPF) is an important phenomenon in terms of global particle number concentrations. Here we investigated the frequency of NPF, formation rates of 10 nm particles, and growth rates in the size range of 10-25 nm using at least 1 year of aerosol number size-distribution observations at 36 different locations around the world. The majority of these measurement sites are in the Northern Hemisphere. We found that the NPF frequency has a strong seasonal variability. At the measurement sites analyzed in this study, NPF occurs most frequently in March-May (on about 30 % of the days) and least frequently in December-February (about 10 % of the days). The median formation rate of 10 nm particles varies by about 3 orders of magnitude (0.01-10 cm(-3) s(-1)) and the growth rate by about an order of magnitude (1-10 nm h(-1)). The smallest values of both formation and growth rates were observed at polar sites and the largest ones in urban environments or anthropogenically influenced rural sites. The correlation between the NPF event frequency and the particle formation and growth rate was at best moderate among the different measurement sites, as well as among the sites belonging to a certain environmental regime. For a better understanding of atmospheric NPF and its regional importance, we would need more observational data from different urban areas in practically all parts of the world, from additional remote and rural locations in North America, Asia, and most of the Southern Hemisphere (especially Australia), from polar areas, and from at least a few locations over the oceans.
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| 12. |
- Paasonen, Pauli, et al.
(författare)
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Warming-induced increase in aerosol number concentration likely to moderate climate change
- 2013
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Ingår i: Nature Geoscience. - 1752-0908. ; 6:6, s. 438-442
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Tidskriftsartikel (refereegranskat)abstract
- Atmospheric aerosol particles influence the climate system directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei(1-4). Apart from black carbon aerosol, aerosols cause a negative radiative forcing at the top of the atmosphere and substantially mitigate the warming caused by greenhouse gases(1). In the future, tightening of controls on anthropogenic aerosol and precursor vapour emissions to achieve higher air quality may weaken this beneficial effect(5-)7. Natural aerosols, too, might affect future warming(2,3,8,9). Here we analyse long-term observations of concentrations and compositions of aerosol particles and their biogenic precursor vapours in continental mid-and high-latitude environments. We use measurements of particle number size distribution together with boundary layer heights derived from reanalysis data to show that the boundary layer burden of cloud condensation nuclei increases exponentially with temperature. Our results confirm a negative feedback mechanism between the continental biosphere, aerosols and climate: aerosol cooling effects are strengthened by rising biogenic organic vapour emissions in response to warming, which in turn enhance condensation on particles and their growth to the size of cloud condensation nuclei. This natural growth mechanism produces roughly 50% of particles at the size of cloud condensation nuclei across Europe. We conclude that biosphere-atmosphere interactions are crucial for aerosol climate effects and can significantly influence the effects of anthropogenic aerosol emission controls, both on climate and air quality.
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| 13. |
- Pajunoja, Aki, et al.
(författare)
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Adsorptive uptake of water by semisolid secondary organic aerosols
- 2015
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Ingår i: Geophysical Research Letters. - 0094-8276 .- 1944-8007. ; 42:8, s. 3063-3068
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Tidskriftsartikel (refereegranskat)abstract
- Aerosol climate effects are intimately tied to interactions with water. Here we combine hygroscopicity measurements with direct observations about the phase of secondary organic aerosol (SOA) particles to show that water uptake by slightly oxygenated SOA is an adsorption-dominated process under subsaturated conditions, where low solubility inhibits water uptake until the humidity is high enough for dissolution to occur. This reconciles reported discrepancies in previous hygroscopicity closure studies. We demonstrate that the difference in SOA hygroscopic behavior in subsaturated and supersaturated conditions can lead to an effect up to about 30% in the direct aerosol forcinghighlighting the need to implement correct descriptions of these processes in atmospheric models. Obtaining closure across the water saturation point is therefore a critical issue for accurate climate modeling.
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| 14. |
- Pandolfi, Marco, et al.
(författare)
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A European aerosol phenomenology-6 : scattering properties of atmospheric aerosol particles from 28 ACTRIS sites
- 2018
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 18:11, s. 7877-7911
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Tidskriftsartikel (refereegranskat)abstract
- This paper presents the light-scattering properties of atmospheric aerosol particles measured over the past decade at 28 ACTRIS observatories, which are located mainly in Europe. The data include particle light scattering (sigma(sp)) and hemispheric backscattering (sigma(bsp)) coefficients, scattering Angstrom exponent (SAE), backscatter fraction (BF) and asymmetry parameter (g). An increasing gradient of sigma(sp) is observed when moving from remote environments (arctic/mountain) to regional and to urban environments. At a regional level in Europe, sigma(sp) also increases when moving from Nordic and Baltic countries and from western Europe to central/eastern Europe, whereas no clear spatial gradient is observed for other station environments. The SAE does not show a clear gradient as a function of the placement of the station. However, a west-to-east-increasing gradient is observed for both regional and mountain placements, suggesting a lower fraction of fine-mode particle in western/south-western Europe compared to central and eastern Europe, where the fine-mode particles dominate the scattering. The g does not show any clear gradient by station placement or geographical location reflecting the complex relationship of this parameter with the physical properties of the aerosol particles. Both the station placement and the geographical location are important factors affecting the intraannual variability. At mountain sites, higher sigma(sp) and SAE values are measured in the summer due to the enhanced boundary layer influence and/or new particle-formation episodes. Conversely, the lower horizontal and vertical dispersion during winter leads to higher sigma(sp) values at all low-altitude sites in central and eastern Europe compared to summer. These sites also show SAE maxima in the summer (with corresponding g minima). At all sites, both SAE and g show a strong variation with aerosol particle loading. The lowest values of g are always observed together with low sigma(sp) values, indicating a larger contribution from particles in the smaller accumulation mode. During periods of high sigma(sp) values, the variation of g is less pronounced, whereas the SAE increases or decreases, suggesting changes mostly in the coarse aerosol particle mode rather than in the fine mode. Statistically significant decreasing trends of sigma(sp) are observed at 5 out of the 13 stations included in the trend analyses. The total reductions of sigma(sp) are consistent with those reported for PM2.5 and PM10 mass concentrations over similar periods across Europe.
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| 15. |
- Riipinen, Ilona, et al.
(författare)
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The contribution of organics to atmospheric nanoparticle growth
- 2012
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Ingår i: Nature Geoscience. - : Springer Science and Business Media LLC. - 1752-0894 .- 1752-0908. ; 5:7, s. 453-458
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Tidskriftsartikel (refereegranskat)abstract
- Aerosols have a strong, yet poorly quantified, effect on climate. The growth of the smallest atmospheric particles from diameters in the nanometre range to sizes at which they may act as seeds for cloud droplets is a key step linking aerosols to clouds and climate. In many environments, atmospheric nanoparticles grow by taking up organic compounds that are derived from biogenic hydrocarbon emissions. Several mechanisms may control this uptake. Condensation of low-volatility vapours and formation of organic salts probably dominate the very first steps of growth in particles close to 1 nm in diameter. As the particles grow further, formation of organic polymers and effects related to the phase of the particle probably become increasingly important. We suggest that dependence of particle growth mechanisms on particle size needs to be investigated more systematically.
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| 16. |
- Schobesberger, Siegfried, et al.
(författare)
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Airborne measurements over the boreal forest of southern Finland during new particle formation events in 2009 and 2010
- 2013
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Ingår i: Boreal environment research. - 1239-6095 .- 1797-2469. ; 18:2, s. 145-163
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Tidskriftsartikel (refereegranskat)abstract
- Schobesberger, S., Vaananen, R., Leino, K., Virkkula, A., Backman, J., Pohja, T., Siivola, E., Franchin, A., Mikkila, J., Paramonov, M., Aalto, P.P., Krejci, R., Petaja, T. & Kulmala, M. 2013: Airborne measurements over the boreal forest of southern Finland during new particle formation events in 2009 and 2010. Boreal Env. Res. 18: 145-163. We conducted airborne observations of aerosol physical properties over the southern Finland boreal forest environment. The aim was to investigate the lower tropospheric aerosol (up to 4-km altitude) over an area of 250 by 200 km, in particular during new particle formation (NPF) events, and to address the spatial variability of aerosol number concentration and number size distribution. The regional NPF events, detected both airborne and at the ground, with air masses originating from the Arctic or northern Atlantic Ocean were studied throughout the boundary layer and throughout the area covered. Three suitable case studies are presented in more detail. In two of these studies, the concentrations of nucleation mode particles (3-10 nm in diameter) were found considerably higher (up to a factor of 30) in the upper parts of the planetary boundary layer compared to ground-based measurements during the nucleation events. The observed vertical variation can be connected to boundary layer dynamics and interactions between the boundary layer and the lower free troposphere, likely yielding high concentrations of newly formed aerosol particles. Our results suggest that nucleation does not necessarily occur close to the surface. In one presented case we found evidence of NPF occurring in a limited area above cloud, in the complete absence of a regional NPF event.
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| 17. |
- Shrivastava, Manish, et al.
(författare)
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Recent advances in understanding secondary organic aerosol : Implications for global climate forcing
- 2017
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Ingår i: Reviews of Geophysics. - 8755-1209. ; 55:2, s. 509-559
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Tidskriftsartikel (refereegranskat)abstract
- Anthropogenic emissions and land use changes have modified atmospheric aerosol concentrations and size distributions over time. Understanding preindustrial conditions and changes in organic aerosol due to anthropogenic activities is important because these features (1) influence estimates of aerosol radiative forcing and (2) can confound estimates of the historical response of climate to increases in greenhouse gases. Secondary organic aerosol (SOA), formed in the atmosphere by oxidation of organic gases, represents a major fraction of global submicron-sized atmospheric organic aerosol. Over the past decade, significant advances in understanding SOA properties and formation mechanisms have occurred through measurements, yet current climate models typically do not comprehensively include all important processes. This review summarizes some of the important developments during the past decade in understanding SOA formation. We highlight the importance of some processes that influence the growth of SOA particles to sizes relevant for clouds and radiative forcing, including formation of extremely low volatility organics in the gas phase, acid-catalyzed multiphase chemistry of isoprene epoxydiols, particle-phase oligomerization, and physical properties such as volatility and viscosity. Several SOA processes highlighted in this review are complex and interdependent and have nonlinear effects on the properties, formation, and evolution of SOA. Current global models neglect this complexity and nonlinearity and thus are less likely to accurately predict the climate forcing of SOA and project future climate sensitivity to greenhouse gases. Efforts are also needed to rank the most influential processes and nonlinear process-related interactions, so that these processes can be accurately represented in atmospheric chemistry-climate models.
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| 18. |
- Sipila, Mikko, et al.
(författare)
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The Role of Sulfuric Acid in Atmospheric Nucleation
- 2010
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Ingår i: Science. - : American Association for the Advancement of Science (AAAS). - 0036-8075 .- 1095-9203. ; 327:5970, s. 1243-1246
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Tidskriftsartikel (refereegranskat)abstract
- Nucleation is a fundamental step in atmospheric new-particle formation. However, laboratory experiments on nucleation have systematically failed to demonstrate sulfuric acid particle formation rates as high as those necessary to account for ambient atmospheric concentrations, and the role of sulfuric acid in atmospheric nucleation has remained a mystery. Here, we report measurements of new particles ( with diameters of approximately 1.5 nanometers) observed immediately after their formation at atmospherically relevant sulfuric acid concentrations. Furthermore, we show that correlations between measured nucleation rates and sulfuric acid concentrations suggest that freshly formed particles contain one to two sulfuric acid molecules, a number consistent with assumptions that are based on atmospheric observations. Incorporation of these findings into global models should improve the understanding of the impact of secondary particle formation on climate.
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| 19. |
- Wang, Jian, et al.
(författare)
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Amazon boundary layer aerosol concentration sustained by vertical transport during rainfall
- 2016
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Ingår i: Nature. - : Springer Science and Business Media LLC. - 0028-0836 .- 1476-4687. ; 539:7629, s. 416-419
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Tidskriftsartikel (refereegranskat)abstract
- The nucleation of atmospheric vapours is an important source of new aerosol particles that can subsequently grow to form cloud condensation nuclei in the atmosphere(1). Most field studies of atmospheric aerosols over continents are influenced by atmospheric vapours of anthropogenic origin (for example, ref. 2) and, in consequence, aerosol processes in pristine, terrestrial environments remain poorly understood. The Amazon rainforest is one of the few continental regions where aerosol particles and their precursors can be studied under near-natural conditions(3-5), but the origin of small aerosol particles that grow into cloud condensation nuclei in the Amazon boundary layer remains unclear(6-8). Here we present aircraft- and ground-based measurements under clean conditions during the wet season in the central Amazon basin. We find that high concentrations of small aerosol particles (with diameters of less than 50 nanometres) in the lower free troposphere are transported from the free troposphere into the boundary layer during precipitation events by strong convective downdrafts and weaker downward motions in the trailing stratiform region. This rapid vertical transport can help to maintain the population of particles in the pristine Amazon boundary layer, and may therefore influence cloud properties and climate under natural conditions.
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| 20. |
- Wang, Mingyi, et al.
(författare)
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Rapid growth of new atmospheric particles by nitric acid and ammonia condensation
- 2020
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Ingår i: Nature. - : Springer Science and Business Media LLC. - 0028-0836 .- 1476-4687. ; 581:7807, s. 184-
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Tidskriftsartikel (refereegranskat)abstract
- A list of authors and their affiliations appears at the end of the paper New-particle formation is a major contributor to urban smog(1,2), but how it occurs in cities is often puzzling(3). If the growth rates of urban particles are similar to those found in cleaner environments (1-10 nanometres per hour), then existing understanding suggests that new urban particles should be rapidly scavenged by the high concentration of pre-existing particles. Here we show, through experiments performed under atmospheric conditions in the CLOUD chamber at CERN, that below about +5 degrees Celsius, nitric acid and ammonia vapours can condense onto freshly nucleated particles as small as a few nanometres in diameter. Moreover, when it is cold enough (below -15 degrees Celsius), nitric acid and ammonia can nucleate directly through an acid-base stabilization mechanism to form ammonium nitrate particles. Given that these vapours are often one thousand times more abundant than sulfuric acid, the resulting particle growth rates can be extremely high, reaching well above 100 nanometres per hour. However, these high growth rates require the gas-particle ammonium nitrate system to be out of equilibrium in order to sustain gas-phase supersaturations. In view of the strong temperature dependence that we measure for the gas-phase supersaturations, we expect such transient conditions to occur in inhomogeneous urban settings, especially in wintertime, driven by vertical mixing and by strong local sources such as traffic. Even though rapid growth from nitric acid and ammonia condensation may last for only a few minutes, it is nonetheless fast enough to shepherd freshly nucleated particles through the smallest size range where they are most vulnerable to scavenging loss, thus greatly increasing their survival probability. We also expect nitric acid and ammonia nucleation and rapid growth to be important in the relatively clean and cold upper free troposphere, where ammonia can be convected from the continental boundary layer and nitric acid is abundant from electrical storms(4,5).
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| 21. |
- Yli-Juuti, Taina, et al.
(författare)
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Effect Of Salt Formation On Condensation Of Organic Compounds On Atmospheric Nanoparticles
- 2013
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Ingår i: NUCLEATION AND ATMOSPHERIC AEROSOLS. - : AIP. - 9780735411524 ; , s. 445-448
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Konferensbidrag (refereegranskat)abstract
- Freshly formed atmospheric nanoparticles have been observed to contain also such organic compounds which have too high saturation vapor pressure to condense on nanoparticles reversibly. The condensation of these compounds on the particles may be facilitated by particle phase processes that transform the compounds into less-volatile form. Here we use particle growth model MABNAG to study the effect of particle phase acid-base chemistry on the condensation of organic acids and bases.
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