| 1. |
- Beddows, D. C. S., et al.
(author)
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Variations in tropospheric submicron particle size distributions across the European continent 2008-2009
- 2014
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In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 14:8, s. 4327-4348
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Journal article (peer-reviewed)abstract
- Cluster analysis of particle number size distributions from background sites across Europe is presented. This generated a total of nine clusters of particle size distributions which could be further combined into two main groups, namely: a south-to-north category (four clusters) and a west-to-east category (five clusters). The first group was identified as most frequently being detected inside and around northern Germany and neighbouring countries, showing clear evidence of local afternoon nucleation and growth events that could be linked to movement of air masses from south to north arriving ultimately at the Arctic contributing to Arctic haze. The second group of particle size spectra proved to have narrower size distributions and collectively showed a dependence of modal diameter upon the longitude of the site (west to east) at which they were most frequently detected. These clusters indicated regional nucleation (at the coastal sites) growing to larger modes further inland. The apparent growth rate of the modal diameter was around 0.6-0.9 nm h(-1). Four specific air mass back-trajectories were successively taken as case studies to examine in real time the evolution of aerosol size distributions across Europe. While aerosol growth processes can be observed as aerosol traverses Europe, the processes are often obscured by the addition of aerosol by emissions en route. This study revealed that some of the 24 stations exhibit more complex behaviour than others, especially when impacted by local sources or a variety of different air masses. Overall, the aerosol size distribution clustering analysis greatly simplifies the complex data set and allows a description of aerosol aging processes, which reflects the longer-term average development of particle number size distributions as air masses advect across Europe.
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| 2. |
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| 3. |
- Kecorius, Simonas, et al.
(author)
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Significant increase of aerosol number concentrations in air masses crossing a densely trafficked sea area
- 2016
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In: Oceanologia. - : Elsevier BV. - 0078-3234. ; 58:1, s. 1-12
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Journal article (peer-reviewed)abstract
- In this study, we evaluated 10 months data (September 2009 to June 2010) of atmospheric aerosol particle number size distribution at three atmospheric observation stations along the Baltic Sea coast: Vavihill (upwind, Sweden), Uto (upwind, Finland), and Preila (downwind, Lithuania). Differences in aerosol particle number size distributions between the upwind and downwind stations during situations of connected atmospheric flow, when the air passed each station, were used to assess the contribution of ship emissions to the aerosol number concentration (diameter interval 50-400 nm) in the Lithuanian background coastal environment. A clear increase in particle number concentration could be noticed, by a factor of 1.9 from Uto to Preila (the average total number concentration at Uto was 791 cm(-3)), and by a factor of 1.6 from Vavihill to Preila (the average total number concentration at Vavihill was 998 cm(-3)). The simultaneous measurements of absorption Angstrom exponents close to unity at Preila supported our conclusion that ship emissions in the Baltic Sea contributed to the increase in particle number concentration at Preila. (C) 2015 Institute of Oceanology of the Polish Academy of Sciences.
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| 4. |
- Kivekäs, Niku, et al.
(author)
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Contribution of ship traffic to aerosol particle concentrations downwind of a major shipping lane
- 2014
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In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 14:16, s. 8255-8267
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Journal article (peer-reviewed)abstract
- Particles in the atmosphere are of concern due to their toxic properties and effects on climate. In coastal areas, ship emissions can be a significant anthropogenic source. In this study we investigated the contribution from ship emissions to the total particle number and mass concentrations at a remote location. We studied the particle number concentration (12 to 490 nm in diameter), the mass concentration (12 to 150 nm in diameter) and number and volume size distribution of aerosol particles in ship plumes for a period of 4.5 months at Hovsore, a coastal site on the western coast of Jutland in Denmark. During episodes of western winds, the site is about 50 km downwind of a major shipping lane and the plumes are approximately 1 hour old when they arrive at the site. We have used a sliding percentile-based method for separating the plumes from the measured background values and to calculate the ship plume contribution to the total particle number and PM0.15 mass concentration (mass of particles below 150 nm in diameter, converted from volume assuming sphericity) at the site. The method is not limited to particle number or volume concentration, but can also be used for different chemical species in both particle and gas phase. The total number of analyzed ship plumes was 726, covering on average 19% of the time when air masses were arriving at the site over the shipping lane. During the periods when plumes were present, the particle concentration exceeded the background values on average by 790 cm(-3) by number and 0.10 gm(-3) by mass. The corresponding daily average values were 170 cm-3 and 0.023 gm-3, respectively. This means that the ship plumes contributed between 11 and 19% to the particle number concentration and between 9 and 18% to PM0.15 during days when air was arriving over the shipping lane. The estimated annual contribution from ship plumes, where all wind directions were included, was in the range of 5-8% in particle number concentration and 4-8% in PM0.15.
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| 5. |
- Kivekäs, Niku, et al.
(author)
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Coupling an aerosol box model with one-dimensional flow : A tool for understanding observations of new particle formation events
- 2016
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In: Tellus. Series B: Chemical and Physical Meteorology. - : Stockholm University Press. - 1600-0889 .- 0280-6509. ; 68:1
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Journal article (peer-reviewed)abstract
- Field observations of new particle formation and the subsequent particle growth are typically only possible at a fixed measurement location, and hence do not follow the temporal evolution of an air parcel in a Lagrangian sense. Standard analysis for determining formation and growth rates requires that the time-dependent formation rate and growth rate of the particles are spatially invariant; air parcel advection means that the observed temporal evolution of the particle size distribution at a fixed measurement location may not represent the true evolution if there are spatial variations in the formation and growth rates. Here we present a zerodimensional aerosol box model coupled with one-dimensional atmospheric flow to describe the impact of advection on the evolution of simulated new particle formation events. Wind speed, particle formation rates and growth rates are input parameters that can vary as a function of time and location, using wind speed to connect location to time. The output simulates measurements at a fixed location; formation and growth rates of the particle mode can then be calculated from the simulated observations at a stationary point for different scenarios and be compared with the 'true' input parameters. Hence, we can investigate how spatial variations in the formation and growth rates of new particles would appear in observations of particle number size distributions at a fixed measurement site. We show that the particle size distribution and growth rate at a fixed location is dependent on the formation and growth parameters upwind, even if local conditions do not vary. We also show that different input parameters used may result in very similar simulated measurements. Erroneous interpretation of observations in terms of particle formation and growth rates, and the time span and areal extent of new particle formation, is possible if the spatial effects are not accounted for.
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| 6. |
- Kristensson, Adam, et al.
(author)
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NanoMap: Geographical mapping of atmospheric new-particle formation through analysis of particle number size distribution and trajectory data
- 2014
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In: Boreal Environment Research: An International Interdisciplinary Journal. - 1239-6095. ; 19, s. 329-342
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Journal article (peer-reviewed)abstract
- Particle number size distributions at various field sites are used to identify atmospheric new-particle formation (NPF) event days. However, the spatial distribution of regionally extensive events is unknown. To remedy this situation, the NanoMap method has been developed to enable the estimation of where NPF occurs within 500 km from any field station using as input size distribution and meteorological trajectories only. Also, the horizontal extension of NPF can be determined. An open-source program to run NanoMap is available on the internet. NanoMap has been developed using as an example the Finnish field site at Hyytiala. It shows that there are frequent NPF events over the Baltic Sea, but not as frequent as over Finland for certain wind directions; hence NanoMap is able to pinpoint areas with a low or high occurrence of NPF events. The method should be applicable to almost any field site.
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| 7. |
- Leinonen, Ville, et al.
(author)
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Comparison of particle number size distribution trends in ground measurements and climate models
- 2022
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In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 22:19, s. 12873-12905
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Journal article (peer-reviewed)abstract
- Despite a large number of studies, out of all drivers of radiative forcing, the effect of aerosols has the largest uncertainty in global climate model radiative forcing estimates. There have been studies of aerosol optical properties in climate models, but the effects of particle number size distribution need a more thorough inspection. We investigated the trends and seasonality of particle number concentrations in nucleation, Aitken, and accumulation modes at 21 measurement sites in Europe and the Arctic. For 13 of those sites, with longer measurement time series, we compared the field observations with the results from five climate models, namely EC-Earth3, ECHAM-M7, ECHAM-SALSA, NorESM1.2, and UKESM1. This is the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five earth system models (ESMs). We found that the trends of particle number concentrations were mostly consistent and decreasing in both measurements and models. However, for many sites, climate models showed weaker decreasing trends than the measurements. Seasonal variability in measured number concentrations, quantified by the ratio between maximum and minimum monthly number concentration, was typically stronger at northern measurement sites compared to other locations. Models had large differences in their seasonal representation, and they can be roughly divided into two categories: for EC-Earth and NorESM, the seasonal cycle was relatively similar for all sites, and for other models the pattern of seasonality varied between northern and southern sites. In addition, the variability in concentrations across sites varied between models, some having relatively similar concentrations for all sites, whereas others showed clear differences in concentrations between remote and urban sites. To conclude, although all of the model simulations had identical input data to describe anthropogenic mass emissions, trends in differently sized particles vary among the models due to assumptions in emission sizes and differences in how models treat size-dependent aerosol processes. The inter-model variability was largest in the accumulation mode, i.e. sizes which have implications for aerosol–cloud interactions. Our analysis also indicates that between models there is a large variation in efficiency of long-range transportation of aerosols to remote locations. The differences in model results are most likely due to the more complex effect of different processes instead of one specific feature (e.g. the representation of aerosol or emission size distributions). Hence, a more detailed characterization of microphysical processes and deposition processes affecting the long-range transport is needed to understand the model variability.
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| 8. |
- Nieminen, Tuomo, et al.
(author)
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Global analysis of continental boundary layer new particle formation based on long-term measurements
- 2018
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In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 18:19, s. 14737-14756
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Journal article (peer-reviewed)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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| 9. |
- Rosenfeld, Daniel, et al.
(author)
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Global observations of aerosol-cloud-precipitation-climate interactions
- 2014
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In: Reviews of Geophysics. - 8755-1209. ; 52:4, s. 750-808
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Research review (peer-reviewed)abstract
- Cloud drop condensation nuclei (CCN) and ice nuclei (IN) particles determine to a large extent cloud microstructure and, consequently, cloud albedo and the dynamic response of clouds to aerosol-induced changes to precipitation. This can modify the reflected solar radiation and the thermal radiation emitted to space. Measurements of tropospheric CCN and IN over large areas have not been possible and can be only roughly approximated from satellite-sensor-based estimates of optical properties of aerosols. Our lack of ability to measure both CCN and cloud updrafts precludes disentangling the effects of meteorology from those of aerosols and represents the largest component in our uncertainty in anthropogenic climate forcing. Ways to improve the retrieval accuracy include multiangle and multipolarimetric passive measurements of the optical signal and multispectral lidar polarimetric measurements. Indirect methods include proxies of trace gases, as retrieved by hyperspectral sensors. Perhaps the most promising emerging direction is retrieving the CCN properties by simultaneously retrieving convective cloud drop number concentrations and updraft speeds, which amounts to using clouds as natural CCN chambers. These satellite observations have to be constrained by in situ observations of aerosol-cloud-precipitation-climate (ACPC) interactions, which in turn constrain a hierarchy of model simulations of ACPC. Since the essence of a general circulation model is an accurate quantification of the energy and mass fluxes in all forms between the surface, atmosphere and outer space, a route to progress is proposed here in the form of a series of box flux closure experiments in the various climate regimes. A roadmap is provided for quantifying the ACPC interactions and thereby reducing the uncertainty in anthropogenic climate forcing.
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| 10. |
- Shen, Xiaojing, et al.
(author)
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Spatial distribution and occurrence probability of regional new particle formation events in eastern China
- 2018
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In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 18:2, s. 587-599
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Journal article (peer-reviewed)abstract
- In this work, the spatial extent of new particle formation (NPF) events and the relative probability of observing particles originating from different spatial origins around three rural sites in eastern China were investigated using the NanoMap method, using particle number size distribution (PNSD) data and air mass back trajectories. The length of the datasets used were 7, 1.5, and 3 years at rural sites Shangdianzi (SDZ) in the North China Plain (NCP), Mt. Tai (TS) in central eastern China, and Lin'an (LAN) in the Yangtze River Delta region in eastern China, respectively. Regional NPF events were observed to occur with the horizontal extent larger than 500 km at SDZ and TS, favoured by the fast transport of northwesterly air masses. At LAN, however, the spatial footprint of NPF events was mostly observed around the site within 100-200 km. Difference in the horizontal spatial distribution of new particle source areas at different sites was connected to typical meteorological conditions at the sites. Consecutive large-scale regional NPF events were observed at SDZ and TS simultaneously and were associated with a high surface pressure system dominating over this area. Simultaneous NPF events at SDZ and LAN were seldom observed. At SDZ the polluted air masses arriving over the NCP were associated with higher particle growth rate (GR) and new particle formation rate (J ) than air masses from Inner Mongolia (IM). At TS the same phenomenon was observed for J , but GR was somewhat lower in air masses arriving over the NCP compared to those arriving from IM. The capability of NanoMap to capture the NPF occurrence probability depends on the length of the dataset of PNSD measurement but also on topography around the measurement site and typical air mass advection speed during NPF events. Thus the long-term measurements of PNSD in the planetary boundary layer are necessary in the further study of spatial extent and the probability of NPF events. The spatial extent, relative probability of occurrence, and typical evolution of PNSD during NPF events presented in this study provide valuable information to further understand the climate and air quality effects of new particle formation.
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| 11. |
- Svensson, Jonas, et al.
(author)
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Light-absorption of dust and elemental carbon in snow in the Indian Himalayas and the Finnish Arctic
- 2018
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In: Atmospheric Measurement Techniques. - : Copernicus GmbH. - 1867-1381 .- 1867-8548. ; 11:3, s. 1403-1416
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Journal article (peer-reviewed)abstract
- Light-absorbing impurities (LAIs) deposited in snow have the potential to substantially affect the snow radiation budget, with subsequent implications for snow melt. To more accurately quantify the snow albedo, the contribution from different LAIs needs to be assessed. Here we estimate the main LAI components, elemental carbon (EC) (as a proxy for black carbon) and mineral dust in snow from the Indian Himalayas and paired the results with snow samples from Arctic Finland. The impurities are collected onto quartz filters and are analyzed thermal-optically for EC, as well as with an additional optical measurement to estimate the light-absorption of dust separately on the filters. Laboratory tests were conducted using substrates containing soot and mineral particles, especially prepared to test the experimental setup. Analyzed ambient snow samples show EC concentrations that are in the same range as presented by previous research, for each respective region. In terms of the mass absorption cross section (MAC) our ambient EC surprisingly had about half of the MAC value compared to our laboratory standard EC (chimney soot), suggesting a less light absorptive EC in the snow, which has consequences for the snow albedo reduction caused by EC. In the Himalayan samples, larger contributions by dust (in the range of 50% or greater for the light absorption caused by the LAI) highlighted the importance of dust acting as a light absorber in the snow. Moreover, EC concentrations in the Indian samples, acquired from a 120 cm deep snow pit (possibly covering the last five years of snow fall), suggest an increase in both EC and dust deposition. This work emphasizes the complexity in determining the snow albedo, showing that LAI concentrations alone might not be sufficient, but additional transient effects on the light-absorbing properties of the EC need to be considered and studied in the snow. Equally as imperative is the confirmation of the spatial and temporal representativeness of these data by comparing data from several and deeper pits explored at the same time.
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| 12. |
- Svensson, Jonas, et al.
(author)
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Soot-doped natural snow and its albedo - Results from field experiments
- 2016
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In: Boreal Environment Research. - 1239-6095. ; 21, s. 481-503
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Journal article (peer-reviewed)abstract
- Soot has a pronounced effect on the cryosphere and experiments are still needed to reduce the associated uncertainties. This work presents a series of experiments to address this issue, with soot being deposited onto a natural snow surface after which the albedo changes were monitored. The albedo reduction was the most pronounced for the snow with higher soot content, and it was observed immediately following soot deposition. Compared with a previous laboratory study the effects of soot on the snow were not as prominent in outdoor conditions. During snowmelt, about 50% of the originally deposited soot particles were observed to remain at the snow surface. More detailed experiments are however needed to better explain soot’s effect on snow and to better quantify this effect. Our albedo versus soot parameterization agreed relatively well with previously published relationships.
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| 13. |
- Vaananen, R., et al.
(author)
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Analysis of particle size distribution changes between three measurement sites in northern Scandinavia
- 2013
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In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7324. ; 13:23, s. 11887-11903
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Journal article (peer-reviewed)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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| 14. |
- Väänänen, Riikka, et al.
(author)
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Analysis of particle size distribution changes between three measurement sites in Northern Scandinavia
- 2013
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In: Nucleation and Atmospheric Aerosols - 19th International Conference. - : AIP. - 1551-7616 .- 0094-243X. - 9780735411524 ; 1527, s. 531-534
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Conference paper (peer-reviewed)abstract
- Measured aerosol size distributions from three measurement stations and modeled air mass trajectory data were combined to study aerosol dynamics in the boreal forest zone in Northern Scandinavia. Three approaches were used: investigation of new particle formation events, analysis of air masses arriving from ocean to continent, and study of changes in the aerosol size distributions when air masses travel from one measurement site to another. The statistical analysis of air masses travelling either from the Atlantic Ocean to measurement sites or from one site to another showed that on average the condensational growth was present during the summer season, and it was not restricted only to the days when evident new particle formation was observed. The rate of this average apparent growth of particle diameter was 3-7 times smaller than the growth rate of nucleation mode particles during the new particle formation events.
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| 15. |
- Öström, Emilie, et al.
(author)
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Biogenic SOA formation through gas-phase oxidation and gas-to-particle partitioning-a comparison between process models of varying complexity
- 2014
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In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7324. ; 14:21, s. 11853-11869
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Journal article (peer-reviewed)abstract
- Biogenic volatile organic compounds (BVOCs) emitted by vegetation play an important role for aerosol mass loadings since the oxidation products of these compounds can take part in the formation and growth of secondary organic aerosols (SOA). The concentrations and properties of BVOCs and their oxidation products in the atmosphere are poorly characterized, which leads to high uncertainties in modeled SOA mass and properties. In this study, the formation of SOA has been modeled along an air-mass trajectory over northern European boreal forest using two aerosol dynamics box models where the prediction of the condensable organics from the gas-phase oxidation of BVOC is handled with schemes of varying complexity. The use of box model simulations along an air-mass trajectory allows us to compare, under atmospheric relevant conditions, different model parameterizations and their effect on SOA formation. The result of the study shows that the modeled mass concentration of SOA is highly dependent on the organic oxidation scheme used to predict oxidation products. A near-explicit treatment of organic gas-phase oxidation (Master Chemical Mechanism version 3.2) was compared to oxidation schemes that use the volatility basis set (VBS) approach. The resulting SOA mass modeled with different VBS schemes varies by a factor of about 7 depending on how the first-generation oxidation products are parameterized and how they subsequently age (e.g., how fast the gas-phase oxidation products react with the OH radical, how they respond to temperature changes, and if they are allowed to fragment during the aging process). Since the VBS approach is frequently used in regional and global climate models due to its relatively simple treatment of the oxidation products compared to near-explicit oxidation schemes, a better understanding of the above-mentioned processes is needed. Based on the results of this study, fragmentation should be included in order to obtain a realistic SOA formation. Furthermore, compared to the most commonly used VBS schemes, the near-explicit method produces less-but more oxidized-SOA.
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| 16. |
- Öström, Emilie, et al.
(author)
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Modeling the role of highly oxidized multifunctional organic molecules for the growth of new particles over the boreal forest region
- 2017
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In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 17:14, s. 8887-8901
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Journal article (peer-reviewed)abstract
- In this study, the processes behind observed new particle formation (NPF) events and subsequent organic-dominated particle growth at the Pallas Atmosphere-Ecosystem Supersite in Northern Finland are explored with the one-dimensional column trajectory model ADCHEM. The modeled sub-micron particle mass is up to ∼75 % composed of SOA formed from highly oxidized multifunctional organic molecules (HOMs) with low or extremely low volatility. In the model the newly formed particles with an initial diameter of 1.5 nm reach a diameter of 7 nm about 2 h earlier than what is typically observed at the station. This is an indication that the model tends to overestimate the initial particle growth. In contrast, the modeled particle growth to CCN size ranges (> 50 nm in diameter) seems to be underestimated because the increase in the concentration of particles above 50 nm in diameter typically occurs several hours later compared to the observations. Due to the high fraction of HOMs in the modeled particles, the oxygen-to-carbon (O : C) atomic ratio of the SOA is nearly 1. This unusually high O : C and the discrepancy between the modeled and observed particle growth might be explained by the fact that the model does not consider any particle-phase reactions involving semi-volatile organic compounds with relatively low O : C. In the model simulations where condensation of low-volatility and extremely low-volatility HOMs explain most of the SOA formation, the phase state of the SOA (assumed either liquid or amorphous solid) has an insignificant impact on the evolution of the particle number size distributions. However, the modeled particle growth rates are sensitive to the method used to estimate the vapor pressures of the HOMs. Future studies should evaluate how heterogeneous reactions involving semi-volatility HOMs and other less-oxidized organic compounds can influence the SOA composition- and size-dependent particle growth.
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