| 1. |
- Keskinen, H., et al.
(författare)
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Evolution of Nanoparticle Composition in CLOUD in Presence of Sulphuric Acid, Ammonia and Organics
- 2013
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Ingår i: NUCLEATION AND ATMOSPHERIC AEROSOLS. - : American Institute of Physics (AIP). - 9780735411524 ; , s. 291-294
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Konferensbidrag (refereegranskat)abstract
- In this study, we investigate the composition of nucleated nanoparticles formed from sulphuric acid, ammonia, amines, and oxidised organics in the CLOUD chamber experiments at CERN. The investigation is carried out via analysis of the particle hygroscopicity (size range of 15-63 nm), ethanol affinity (15-50nm), oxidation state (<50 nm), and ion composition (few nanometers). The organic volume fraction of particles increased with an increase in particle diameter in presence of the sulphuric acid, ammonia and organics. Vice versa, the sulphuric acid volume fraction decreased when the particle diameter increased. The results provide information on the size-dependent composition of nucleated aerosol particles.
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| 2. |
- Laaksonen, A., et al.
(författare)
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The role of VOC oxidation products in continental new particle formation
- 2008
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 8:10, s. 2657-2665
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Tidskriftsartikel (refereegranskat)abstract
- Aerosol physical and chemical properties and trace gas concentrations were measured during the QUEST field campaign in March-April 2003, in Hyytiala, Finland. Our aim was to understand the role of oxidation products of VOC's such as mono- and sesquiterpenes in atmospheric nucleation events. Particle chemical compositions were measured using the Aerodyne Aerosol Mass Spectrometer, and chemical compositions of aerosol samples collected with low-pressure impactors and a high volume sampler were analysed using a number of techniques. The results indicate that during and after new particle formation, all particles larger than 50 nm in diameter contained similar organic substances that are likely to be mono- and sesquiterpene oxidation products. The oxidation products identified in the high volume samples were shown to be mostly aldehydes. In order to study the composition of particles in the 10-50 nm range, we made use of Tandem Differential Mobility Analyzer results. We found that during nucleation events, both 10 and 50 nm particle growth factors due to uptake of ethanol vapour correlate strongly with gas-phase monoterpene oxidation product (MTOP) concentrations, indicating that the organic constituents of particles smaller than 50 nm in diameter are at least partly similar to those of larger particles. We furthermore showed that particle growth rates during the nucleation events are correlated with the gas-phase MTOP concentrations. This indicates that VOC oxidation products may have a key role in determining the spatial and temporal features of the nucleation events. This conclusion was supported by our aircraft measurements of new 3-10 nm particle concentrations, which showed that the nucleation event on 28 March 2003, started at the ground layer, i.e. near the VOC source, and evolved together with the mixed layer. Furthermore, no new particle formation was detected upwind away from the forest, above the frozen Gulf of Bothnia.
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| 3. |
- Mann, G. W., et al.
(författare)
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Intercomparison and evaluation of global aerosol microphysical properties among AeroCom models of a range of complexity
- 2014
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 14:9, s. 4679-4713
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Tidskriftsartikel (refereegranskat)abstract
- Many of the next generation of global climate models will include aerosol schemes which explicitly simulate the microphysical processes that determine the particle size distribution. These models enable aerosol optical properties and cloud condensation nuclei (CCN) concentrations to be determined by fundamental aerosol processes, which should lead to a more physically based simulation of aerosol direct and indirect radiative forcings. This study examines the global variation in particle size distribution simulated by 12 global aerosol microphysics models to quantify model diversity and to identify any common biases against observations. Evaluation against size distribution measurements from a new European network of aerosol supersites shows that the mean model agrees quite well with the observations at many sites on the annual mean, but there are some seasonal biases common to many sites. In particular, at many of these European sites, the accumulation mode number concentration is biased low during winter and Aitken mode concentrations tend to be overestimated in winter and underestimated in summer. At high northern latitudes, the models strongly underpredict Aitken and accumulation particle concentrations compared to the measurements, consistent with previous studies that have highlighted the poor performance of global aerosol models in the Arctic. In the marine boundary layer, the models capture the observed meridional variation in the size distribution, which is dominated by the Aitken mode at high latitudes, with an increasing concentration of accumulation particles with decreasing latitude. Considering vertical profiles, the models reproduce the observed peak in total particle concentrations in the upper troposphere due to new particle formation, although modelled peak concentrations tend to be biased high over Europe. Overall, the multimodel-mean data set simulates the global variation of the particle size distribution with a good degree of skill, suggesting that most of the individual global aerosol microphysics models are performing well, although the large model diversity indicates that some models are in poor agreement with the observations. Further work is required to better constrain size-resolved primary and secondary particle number sources, and an improved understanding of nucleation and growth (e. g. the role of nitrate and secondary organics) will improve the fidelity of simulated particle size distributions.
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| 4. |
- Keskinen, H., et al.
(författare)
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Evolution of particle composition in CLOUD nucleation experiments
- 2013
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 13:11, s. 5587-5600
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Tidskriftsartikel (refereegranskat)abstract
- Sulphuric acid, ammonia, amines, and oxidised organics play a crucial role in nanoparticle formation in the atmosphere. In this study, we investigate the composition of nucleated nanoparticles formed from these compounds in the CLOUD (Cosmics Leaving Outdoor Droplets) chamber experiments at CERN (Centre europeen pour la recherche nucleaire). The investigation was carried out via analysis of the particle hygroscopicity, ethanol affinity, oxidation state, and ion composition. Hygroscopicity was studied by a hygroscopic tandem differential mobility analyser and a cloud condensation nuclei counter, ethanol affinity by an organic differential mobility analyser and particle oxidation level by a high-resolution time-of-flight aerosol mass spectrometer. The ion composition was studied by an atmospheric pressure interface time-of-flight mass spectrometer. The volume fraction of the organics in the particles during their growth from sizes of a few nanometers to tens of nanometers was derived from measured hygroscopicity assuming the Zdanovskii-Stokes-Robinson relationship, and compared to values gained from the spectrometers. The ZSR-relationship was also applied to obtain the measured ethanol affinities during the particle growth, which were used to derive the volume fractions of sulphuric acid and the other inorganics (e. g. ammonium salts). In the presence of sulphuric acid and ammonia, particles with a mobility diameter of 150 nm were chemically neutralised to ammonium sulphate. In the presence of oxidation products of pinanediol, the organic volume fraction of freshly nucleated particles increased from 0.4 to similar to 0.9, with an increase in diameter from 2 to 63 nm. Conversely, the sulphuric acid volume fraction decreased from 0.6 to 0.1 when the particle diameter increased from 2 to 50 nm. The results provide information on the composition of nucleated aerosol particles during their growth in the presence of various combinations of sulphuric acid, ammonia, dimethylamine and organic oxidation products.
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| 5. |
- Kulmala, M., et al.
(författare)
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Introduction : The Pan-Eurasian Experiment (PEEX) - multidisciplinary, multiscale and multicomponent research and capacity-building initiative
- 2015
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 15:22, s. 13085-13096
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Tidskriftsartikel (refereegranskat)abstract
- The Pan-Eurasian Experiment (PEEX) is a multidisciplinary, multiscale and multicomponent research, research infrastructure and capacity-building program. PEEX has originated from a bottom-up approach by the science communities and is aiming at resolving the major uncertainties in Earth system science and global sustainability issues concerning the Arctic and boreal pan-Eurasian regions, as well as China. The vision of PEEX is to solve interlinked, global grand challenges influencing human well-being and societies in northern Eurasia and China. Such challenges include climate change; air quality; biodiversity loss; urbanization; chemicalization; food and freshwater availability; energy production; and use of natural resources by mining, industry, energy production and transport sectors. Our approach is integrative and supra-disciplinary, recognizing the important role of the Arctic and boreal ecosystems in the Earth system. The PEEX vision includes establishing and maintaining long-term, coherent and coordinated research activities as well as continuous, comprehensive research and educational infrastructure and related capacity-building across the PEEX domain. In this paper we present the PEEX structure and summarize its motivation, objectives and future outlook.
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| 6. |
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| 7. |
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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. |
- Tunved, P, et al.
(författare)
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One year boundary layer aerosol size distribution data from five nordic background stations
- 2003
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Ingår i: Atmospheric Chemistry and Physics. - 1680-7324. ; 3, s. 2183-2205
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Tidskriftsartikel (refereegranskat)abstract
- Size distribution measurements performed at five different stations have been investigated during a one-year period between 01 June 2000 and 31 May 2001 with focus on diurnal, seasonal and geographical differences of size distribution properties. The stations involved cover a large geographical area ranging from the Finnish Lapland (67degrees N) down to southern Sweden (56degrees N) in the order Varrio, Pallas, Hyytiala, Aspvreten and Vavihill. The shape of the size distribution is typically bimodal during winter with a larger fraction of accumulation mode particles compared to the other seasons. Highest Aitken mode concentration is found during summer and spring during the year of study. The maximum of nucleation events occur during the spring months at all stations. Nucleation events occur during other months as well, although not as frequently. Large differences were found between different categories of stations. Northerly located stations such as Pallas and Varrio presented well-separated Aitken and accumulation modes, while the two modes often overlap significantly at the two southernmost stations Vavihill and Aspvreten. A method to cluster trajectories was used to analyse the impact of long-range transport on the observed aerosol properties. Clusters of trajectories arriving from the continent were clearly associated with size distributions shifted towards the accumulation mode. This feature was more pronounced the further south the station was located. Marine- or Arctic-type clusters were associated with large variability in the nuclei size ranges. A quasi-lagrangian approach was used to investigate transport related changes in the aerosol properties. Typically, an increase in especially Aitken mode concentrations was observed when advection from the north occurs, i.e. allowing more continental influence on the aerosol when comparing the different measurement sites. When trajectory clusters arrive to the stations from SW, a gradual decrease in number concentration is experienced in all modes as latitude of measurement site increases.
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| 10. |
- Vaananen, R., et al.
(författare)
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Analysis of particle size distribution changes between three measurement sites in northern Scandinavia
- 2013
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7324. ; 13:23, s. 11887-11903
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Tidskriftsartikel (refereegranskat)abstract
- We investigated atmospheric aerosol particle dynamics in a boreal forest zone in northern Scandinavia. We used aerosol number size distribution data measured with either a differential mobility particle sizer (DMPS) or scanning mobility particle sizer (SMPS) at three stations (Varrio, Pallas and Abisko), and combined these data with the HYSPLIT (Hybrid Single Particle Lagrangian Integrated Trajectory) air mass trajectory analysis. We compared three approaches analysis of new particle formation events, investigation of aerosol particle number size distributions during the air mass transport from the ocean to individual stations with different overland transport times, and analysis of changes in aerosol particle number size distributions during the air mass transport from one measurement station to another. Aitken-mode particles were found to have apparent average growth rates of 0.6-0.7 nm h(-1) when the air masses traveled over land. Particle growth rates during the new particle formation (NPF) events were 3-6 times higher than the apparent particle growth during the summer period. When comparing aerosol dynamics for different overland transport times between the different stations, no major differences were found, except that in Abisko the NPF events were observed to take place in air masses with shorter overland times than at the other stations. We speculate that this is related to the meteorological differences along the paths of air masses caused by the land surface topology. When comparing air masses traveling in an east-to-west direction with those traveling in a west-to-east direction, clear differences in the aerosol dynamics were seen. Our results suggest that the condensation growth has an important role in aerosol dynamics even when NPF is not evident.
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