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Sökning: WFRF:(Kulmala P)

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1.
  • Kulmala, M., et al. (författare)
  • General overview: European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) - integrating aerosol research from nano to global scales
  • 2011
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:24, s. 13061-13143
  • Tidskriftsartikel (refereegranskat)abstract
    • In this paper we describe and summarize the main achievements of the European Aerosol Cloud Climate and Air Quality Interactions project (EUCAARI). EUCAARI started on 1 January 2007 and ended on 31 December 2010 leaving a rich legacy including: (a) a comprehensive database with a year of observations of the physical, chemical and optical properties of aerosol particles over Europe, (b) comprehensive aerosol measurements in four developing countries, (c) a database of airborne measurements of aerosols and clouds over Europe during May 2008, (d) comprehensive modeling tools to study aerosol processes fron nano to global scale and their effects on climate and air quality. In addition a new Pan-European aerosol emissions inventory was developed and evaluated, a new cluster spectrometer was built and tested in the field and several new aerosol parameterizations and computations modules for chemical transport and global climate models were developed and evaluated. These achievements and related studies have substantially improved our understanding and reduced the uncertainties of aerosol radiative forcing and air quality-climate interactions. The EUCAARI results can be utilized in European and global environmental policy to assess the aerosol impacts and the corresponding abatement strategies.
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2.
  • Brasseur, Z., et al. (författare)
  • Measurement report: Introduction to the HyICE-2018 campaign for measurements of ice-nucleating particles and instrument inter-comparison in the Hyytiala boreal forest
  • 2022
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 22:8, s. 5117-5145
  • Tidskriftsartikel (refereegranskat)abstract
    • The formation of ice particles in Earth's atmosphere strongly influences the dynamics and optical properties of clouds and their impacts on the climate system. Ice formation in clouds is often triggered heterogeneously by ice-nucleating particles (INPs) that represent a very low number of particles in the atmosphere. To date, many sources of INPs, such as mineral and soil dust, have been investigated and identified in the low and mid latitudes. Although less is known about the sources of ice nucleation at high latitudes, efforts have been made to identify the sources of INPs in the Arctic and boreal environments. In this study, we investigate the INP emission potential from high-latitude boreal forests in the mixed-phase cloud regime. We introduce the HyICE-2018 measurement campaign conducted in the boreal forest of Hyytiala, Finland, between February and June 2018. The campaign utilized the infrastructure of the Station for Measuring Ecosystem-Atmosphere Relations (SMEAR) II, with additional INP instruments, including the Portable Ice Nucleation Chamber I and II (PINC and PINCii), the SPectrometer for Ice Nuclei (SPIN), the Portable Ice Nucleation Experiment (PINE), the Ice Nucleation SpEctrometer of the Karlsruhe Institute of Technology (INSEKT) and the Microlitre Nucleation by Immersed Particle Instrument (mu L-NIPI), used to quantify the INP concentrations and sources in the boreal environment. In this contribution, we describe the measurement infrastructure and operating procedures during HyICE-2018, and we report results from specific time periods where INP instruments were run in parallel for inter-comparison purposes. Our results show that the suite of instruments deployed during HyICE-2018 reports consistent results and therefore lays the foundation for forthcoming results to be considered holistically. In addition, we compare measured INP concentrations to INP parameterizations, and we observe good agreement with the Tobo et al. (2013) parameterization developed from measurements conducted in a ponderosa pine forest ecosystem in Colorado, USA.
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3.
  • Yan, C., et al. (författare)
  • Size-dependent influence of NOx on the growth rates of organic aerosol particles
  • 2020
  • Ingår i: Science Advances. - : American Association for the Advancement of Science (AAAS). - 2375-2548. ; 6:22
  • Tidskriftsartikel (refereegranskat)abstract
    • Atmospheric new-particle formation (NPF) affects climate by contributing to a large fraction of the cloud condensation nuclei (CCN). Highly oxygenated organic molecules (HOMs) drive the early particle growth and therefore substantially influence the survival of newly formed particles to CCN. Nitrogen oxide (NOx) is known to suppress the NPF driven by HOMs, but the underlying mechanism remains largely unclear. Here, we examine the response of particle growth to the changes of HOM formation caused by NOx. We show that NOx suppresses particle growth in general, but the suppression is rather nonuniform and size dependent, which can be quantitatively explained by the shifted HOM volatility after adding NOx. By illustrating how NOx affects the early growth of new particles, a critical step of CCN formation, our results help provide a refined assessment of the potential climatic effects caused by the diverse changes of NOx level in forest regions around the globe.
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4.
  • Asmi, A., et al. (författare)
  • Aerosol decadal trends - Part 2: In-situ aerosol particle number concentrations at GAW and ACTRIS stations
  • 2013
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7324. ; 13:2, s. 895-916
  • Tidskriftsartikel (refereegranskat)abstract
    • We have analysed the trends of total aerosol particle number concentrations (N) measured at long-term measurement stations involved either in the Global Atmosphere Watch (GAW) and/or EU infrastructure project ACTRIS. The sites are located in Europe, North America, Antarctica, and on Pacific Ocean islands. The majority of the sites showed clear decreasing trends both in the full-length time series, and in the intra-site comparison period of 2001-2010, especially during the winter months. Several potential driving processes for the observed trends were studied, and even though there are some similarities between N trends and air temperature changes, the most likely cause of many northern hemisphere trends was found to be decreases in the anthropogenic emissions of primary particles, SO2 or some co-emitted species. We could not find a consistent agreement between the trends of N and particle optical properties in the few stations with long time series of all of these properties. The trends of N and the proxies for cloud condensation nuclei (CCN) were generally consistent in the few European stations where the measurements were available. This work provides a useful comparison analysis for modelling studies of trends in aerosol number concentrations.
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5.
  • Asmi, A., et al. (författare)
  • Number size distributions and seasonality of submicron particles in = rope 2008-2009
  • 2011
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:11, s. 5505-5538
  • Tidskriftsartikel (refereegranskat)abstract
    • Two years of harmonized aerosol number size distribution data from 24 = ropean field monitoring sites have been analysed. The results give a = mprehensive overview of the European near surface aerosol particle = mber concentrations and number size distributions between 30 and 500 = of dry particle diameter. Spatial and temporal distribution of = rosols in the particle sizes most important for climate applications = e presented. We also analyse the annual, weekly and diurnal cycles of = e aerosol number concentrations, provide log-normal fitting parameters = r median number size distributions, and give guidance notes for data = ers. Emphasis is placed on the usability of results within the aerosol = delling community.
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6.
  • Beddows, D. C. S., et al. (författare)
  • Variations in tropospheric submicron particle size distributions across the European continent 2008-2009
  • 2014
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 14:8, s. 4327-4348
  • Tidskriftsartikel (refereegranskat)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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7.
  • Jimenez, J. L., et al. (författare)
  • Evolution of Organic Aerosols in the Atmosphere
  • 2009
  • Ingår i: Science. - : American Association for the Advancement of Science (AAAS). - 0036-8075 .- 1095-9203. ; 326:5959, s. 1525-1529
  • Tidskriftsartikel (refereegranskat)abstract
    • Organic aerosol (OA) particles affect climate forcing and human health, but their sources and evolution remain poorly characterized. We present a unifying model framework describing the atmospheric evolution of OA that is constrained by high-time-resolution measurements of its composition, volatility, and oxidation state. OA and OA precursor gases evolve by becoming increasingly oxidized, less volatile, and more hygroscopic, leading to the formation of oxygenated organic aerosol (OOA), with concentrations comparable to those of sulfate aerosol throughout the Northern Hemisphere. Our model framework captures the dynamic aging behavior observed in both the atmosphere and laboratory: It can serve as a basis for improving parameterizations in regional and global models.
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8.
  • Kim, J., et al. (författare)
  • Hygroscopicity of nanoparticles produced from homogeneous nucleation in the CLOUD experiments
  • 2016
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:1, s. 293-304
  • Tidskriftsartikel (refereegranskat)abstract
    • Sulfuric acid, amines and oxidized organics have been found to be important compounds in the nucleation and initial growth of atmospheric particles. Because of the challenges involved in determining the chemical composition of objects with very small mass, however, the properties of the freshly nucleated particles and the detailed pathways of their formation processes are still not clear. In this study,we focus on a challenging size range, i.e., particles that have grown to diameters of 10 and 15 nm following nucleation, and measure their water uptake. Water uptake is useful information for indirectly obtaining chemical composition of aerosol particles. We use a nanometer-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) at sub-saturated conditions (ca. 90% relative humidity at 293 K) to measure the hygroscopicity of particles during the seventh Cosmics Leaving OUtdoor Droplets (CLOUD7) campaign performed at CERN in 2012. In CLOUD7, the hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from alpha-pinene oxidation. The hygroscopicity parameter kappa decreased with increasing particle size, indicating decreasing acidity of particles. No clear effect of the sulfuric acid concentration on the hygroscopicity of 10 nm particles produced from sulfuric acid and dimethylamine was observed, whereas the hygroscopicity of 15 nm particles sharply decreased with decreasing sulfuric acid concentrations. In particular, when the concentration of sulfuric acid was 5.1 x 10(6) molecules cm(-3) in the gas phase, and the dimethylamine mixing ratio was 11.8 ppt, the measured kappa of 15 nm particles was 0.31 +/- 0.01: close to the value reported for dimethylaminium sulfate (DMAS) (kappa(DMAS) similar to 0.28). Furthermore, the difference in kappa between sulfuric acid and sulfuric acid-dimethylamine experiments increased with increasing particle size. The kappa values of particles in the presence of sulfuric acid and organics were much smaller than those of particles in the presence of sulfuric acid and dimethylamine. This suggests that the organics produced from alpha-pinene ozonolysis play a significant role in particle growth even at 10 nm sizes.
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9.
  • Kyro, E. -M, et al. (författare)
  • Trends in new particle formation in eastern Lapland, Finland : effect of decreasing sulfur emissions from Kola Peninsula
  • 2014
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 14:9, s. 4383-4396
  • Tidskriftsartikel (refereegranskat)abstract
    • The smelter industry in Kola Peninsula is the largest source of anthropogenic SO2 in the Arctic part of Europe and one of the largest within the Arctic domain. Due to socio-economic changes in Russia, the emissions have been decreasing especially since the late 1990s resulting in decreased SO2 concentrations close to Kola in eastern Lapland, Finland. At the same time, the frequency of new particle formation days has been decreasing distinctively at SMEAR I station in eastern Lapland, especially during spring and autumn. We show that sulfur species, namely sulfur dioxide and sulfuric acid, have an important role in both new particle formation and subsequent growth and that the decrease in new particle formation days is a result of the reduction of sulfur emissions originating from Kola Peninsula. In addition to sulfur species, there are many other quantities, such as formation rate of aerosol particles, condensation sink and nucleation mode particle number concentration, which are related to the number of observed new particle formation (NPF) days and need to be addressed when linking sulfur emissions and NPF. We show that while most of these quantities exhibit statistically significant trends, the reduction in Kola sulfur emissions is the most obvious reason for the rapid decline in NPF days. Sulfuric acid explains approximately 20-50% of the aerosol condensational growth observed at SMEAR I, and there is a large seasonal variation with highest values obtained during spring and autumn. We found that (i) particles form earlier after sunrise during late winter and early spring due to high concentrations of SO2 and H2SO4; (ii) several events occurred during the absence of light, and they were connected to higher than average concentrations of SO2; and (iii) high SO2 concentrations could advance the onset of nucleation by several hours. Moreover, air masses coming over Kola Peninsula seemed to favour new particle formation.
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10.
  • Monks, P. S., et al. (författare)
  • Atmospheric composition change : global and regional air quality
  • 2009
  • Ingår i: Atmospheric Environment. - : Elsevier BV. - 1352-2310 .- 1873-2844. ; 43:33, s. 5268-5350
  • Forskningsöversikt (refereegranskat)abstract
    • Air quality transcends all scales with in the atmosphere from the local to the global with handovers and feedbacks at each scale interaction. Air quality has manifold effects on health, ecosystems heritage and, climate. In this review the state of scientific understanding in relation to global and regional air quality is outlined. The review discusses air quality, in terms of emissions, processing and transport of trace gases and aerosols. New insights into the characterization of both natural and anthropogenic emissions are reviewed looking at both natural (e.g. dust and lightning) as well as plant emissions. Trends in anthropogenic emissions both by region and globally are discussed as well as biomass burning emissions. In terms of chemical processing the major air quality elements of ozone, non-methane hydrocarbons, nitrogen oxides and aerosols are covered. A number of topics are presented as a way of integrating the process view into the atmospheric context; these include the atmospheric oxidation efficiency, halogen and HOx chemistry, nighttime chemistry, tropical chemistry, heat waves, megacities, biomass burning and the regional hot spot of the Mediterranean. New findings with respect to the transport of pollutants across the scales are discussed, in particular the move to quantify the impact of long-range transport on regional air quality. Gaps and research questions that remain intractable are identified. The review concludes with a focus of research and policy questions for the coming decade. In particular, the policy challenges for concerted air quality and climate change policy (co-benefit) are discussed.
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11.
  • Reddington, C. L., et al. (författare)
  • Primary versus secondary contributions to particle number concentrations in the European boundary layer
  • 2011
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:23, s. 12007-12036
  • Tidskriftsartikel (refereegranskat)abstract
    • It is important to understand the relative contribution of primary and secondary particles to regional and global aerosol so that models can attribute aerosol radiative forcing to different sources. In large-scale models, there is considerable uncertainty associated with treatments of particle formation (nucleation) in the boundary layer (BL) and in the size distribution of emitted primary particles, leading to uncertainties in predicted cloud condensation nuclei (CCN) concentrations. Here we quantify how primary particle emissions and secondary particle formation influence size-resolved particle number concentrations in the BL using a global aerosol microphysics model and aircraft and ground site observations made during the May 2008 campaign of the European Integrated Project on Aerosol Cloud Climate Air Quality Interactions (EUCAARI). We tested four different parameterisations for BL nucleation and two assumptions for the emission size distribution of anthropogenic and wildfire carbonaceous particles. When we emit carbonaceous particles at small sizes (as recommended by the Aerosol Inter-comparison project, AEROCOM), the spatial distributions of campaign-mean number concentrations of particles with diameter >50 nm (N(50)) and >100 nm (N(100)) were well captured by the model (R(2)>= 0.8) and the normalised mean bias (NMB) was also small (-18% for N(50) and -1% for N(100)). Emission of carbonaceous particles at larger sizes, which we consider to be more realistic for low spatial resolution global models, results in equally good correlation but larger bias (R(2)>= 0.8, NMB = -52% and -29%), which could be partly but not entirely compensated by BL nucleation. Within the uncertainty of the observations and accounting for the uncertainty in the size of emitted primary particles, BL nucleation makes a statistically significant contribution to CCN-sized particles at less than a quarter of the ground sites. Our results show that a major source of uncertainty in CCN-sized particles in polluted European air is the emitted size of primary carbonaceous particles. New information is required not just from direct observations, but also to determine the effective emission size and composition of primary particles appropriate for different resolution models.
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12.
  • Bianchi, F., et al. (författare)
  • The SALTENA Experiment : Comprehensive Observations of Aerosol Sources, Formation, and Processes in the South American Andes
  • 2022
  • Ingår i: Bulletin of The American Meteorological Society - (BAMS). - 0003-0007 .- 1520-0477. ; 103:2, s. E212-E229
  • Tidskriftsartikel (refereegranskat)abstract
    • This paper presents an introduction to the Southern Hemisphere High Altitude Experiment on Particle Nucleation and Growth (SALTENA). This field campaign took place between December 2017 and June 2018 (wet to dry season) at Chacaltaya (CHC), a GAW (Global Atmosphere Watch) station located at 5,240 m MSL in the Bolivian Andes. Concurrent measurements were conducted at two additional sites in El Alto (4,000 m MSL) and La Paz (3,600 m MSL). The overall goal of the campaign was to identify the sources, understand the formation mechanisms and transport, and characterize the properties of aerosol at these stations. State-of-the-art instruments were brought to the station complementing the ongoing permanent GAW measurements, to allow a comprehensive description of the chemical species of anthropogenic and biogenic origin impacting the station and contributing to new particle formation. In this overview we first provide an assessment of the complex meteorology, airmass origin, and boundary layer-free troposphere interactions during the campaign using a 6-month high-resolution Weather Research and Forecasting (WRF) simulation coupled with Flexible Particle dispersion model (FLEXPART). We then show some of the research highlights from the campaign, including (i) chemical transformation processes of anthropogenic pollution while the air masses are transported to the CHC station from the metropolitan area of La Paz-El Alto, (ii) volcanic emissions as an important source of atmospheric sulfur compounds in the region, (iii) the characterization of the compounds involved in new particle formation, and (iv) the identification of long-range-transported compounds from the Pacific or the Amazon basin. We conclude the article with a presentation of future research foci. The SALTENA dataset highlights the importance of comprehensive observations in strategic high-altitude locations, especially the undersampled Southern Hemisphere.
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16.
  • Lappalainen, H. K., et al. (författare)
  • Overview: Recent advances in the understanding of the northern Eurasian environments and of the urban air quality in China - a Pan-Eurasian Experiment (PEEX) programme perspective
  • 2022
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 22:7, s. 4413-4469
  • Tidskriftsartikel (refereegranskat)abstract
    • The Pan-Eurasian Experiment (PEEX) Science Plan, released in 2015, addressed a need for a holistic system understanding and outlined the most urgent research needs for the rapidly changing Arctic-boreal region. Air quality in China, together with the long-range transport of atmospheric pollutants, was also indicated as one of the most crucial topics of the research agenda. These two geographical regions, the northern Eurasian Arctic-boreal region and China, especially the megacities in China, were identified as a "PEEX region". It is also important to recognize that the PEEX geographical region is an area where science-based policy actions would have significant impacts on the global climate. This paper summarizes results obtained during the last 5 years in the northern Eurasian region, together with recent observations of the air quality in the urban environments in China, in the context of the PEEX programme. The main regions of interest are the Russian Arctic, northern Eurasian boreal forests (Siberia) and peatlands, and the megacities in China. We frame our analysis against research themes introduced in the PEEX Science Plan in 2015. We summarize recent progress towards an enhanced holistic understanding of the land-atmosphere-ocean systems feedbacks. We conclude that although the scientific knowledge in these regions has increased, the new results are in many cases insufficient, and there are still gaps in our understanding of large-scale climate-Earth surface interactions and feedbacks. This arises from limitations in research infrastructures, especially the lack of coordinated, continuous and comprehensive in situ observations of the study region as well as integrative data analyses, hindering a comprehensive system analysis. The fast-changing environment and ecosystem changes driven by climate change, socio-economic activities like the China Silk Road Initiative, and the global trends like urbanization further complicate such analyses. We recognize new topics with an increasing importance in the near future, especially "the enhancing biological sequestration capacity of greenhouse gases into forests and soils to mitigate climate change" and the "socio-economic development to tackle air quality issues".
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17.
  • Mann, G. W., et al. (författare)
  • Intercomparison and evaluation of global aerosol microphysical properties among AeroCom models of a range of complexity
  • 2014
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 14:9, s. 4679-4713
  • 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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18.
  • Ruuskanen, T. M., et al. (författare)
  • Concentrations and fluxes of aerosol particles during the LAPBIAT measurement campaign at Varrio field station
  • 2007
  • Ingår i: Atmospheric Chemistry And Physics. - 1680-7316 .- 1680-7324. ; 7:14, s. 3683-3700
  • Tidskriftsartikel (refereegranskat)abstract
    • The LAPBIAT measurement campaign took place in the Varrio SMEAR I measurement station located in Eastern Lapland in the spring of 2003 between 26 April and 11 May. In this paper we describe the measurement campaign, concentrations and fluxes of aerosol particles, air ions and trace gases, paying special attention to an aerosol particle formation event broken by a air mass change from a clean Arctic air mass with new particle formation to polluted one approaching from industrial areas of Kola Peninsula, Russia, lacking new particle formation. Aerosol particle number flux measurements show strong downward fluxes during that time. Concentrations of coarse aerosol particles were high for 1-2 days before the nucleation event (i.e. 28-29 April), very low immediately before and during the observed aerosol particle formation event (30 April) and increased moderately from the moment of sudden break of the event. In general particle deposition measurements based on snow samples show the same changes. Measurements of the mobility distribution of air ions showed elevated concentrations of intermediate air ions during the particle formation event. We estimated the growth rates in the nucleation mode size range. For particles <10 nm, the growth rate increases with size on 30 April. Dispersion modelling made with model SILAM support the conclusion that the nucleation event was interrupted by an outbreak of sulphate-rich air mass in the evening of 30 April that originated from the industry at Kola Peninsula, Russia. The results of this campaign highlight the need for detailed research in atmospheric transport of air constituents for understanding the aerosol dynamics.
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20.
  • Schneider, J., et al. (författare)
  • The seasonal cycle of ice-nucleating particles linked to the abundance of biogenic aerosol in boreal forests
  • 2021
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:5, s. 3899-3918
  • Tidskriftsartikel (refereegranskat)abstract
    • Ice-nucleating particles (INPs) trigger the formation of cloud ice crystals in the atmosphere. Therefore, they strongly influence cloud microphysical and optical properties and precipitation and the life cycle of clouds. Improving weather forecasting and climate projection requires an appropriate formulation of atmospheric INP concentrations. This remains challenging as the global INP distribution and variability depend on a variety of aerosol types and sources, and neither their short-term variability nor their long-term seasonal cycles are well covered by continuous measurements. Here, we provide the first year-long set of observations with a pronounced INP seasonal cycle in a boreal forest environment. Besides the observed seasonal cycle in INP concentrations with a minimum in wintertime and maxima in early and late summer, we also provide indications for a seasonal variation in the prevalent INP type. We show that the seasonal dependency of INP concentrations and prevalent INP types is most likely driven by the abundance of biogenic aerosol. As current parameterizations do not reproduce this variability, we suggest a new mechanistic description for boreal forest environments which considers the seasonal variation in INP concentrations. For this, we use the ambient air temperature measured close to the ground at 4.2 m height as a proxy for the season, which appears to affect the source strength of biogenic emissions and, thus, the INP abundance over the boreal forest. Furthermore, we provide new INP parameterizations based on the Ice Nucleation Active Surface Site (INAS) approach, which specifically describes the ice nucleation activity of boreal aerosols particles prevalent in different seasons. Our results characterize the boreal forest as an important but variable INP source and provide new perspectives to describe these new findings in atmospheric models.
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21.
  • Scholz, W., et al. (författare)
  • Measurement report: Long-range transport and the fate of dimethyl sulfide oxidation products in the free troposphere derived from observations at the high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes
  • 2023
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 23:2, s. 895-920
  • Tidskriftsartikel (refereegranskat)abstract
    • Dimethyl sulfide (DMS) is the primary natural contributor to the atmospheric sulfur burden. Observations concerning the fate of DMS oxidation products after long-range transport in the remote free troposphere are, however, sparse. Here we present quantitative chemical ionization mass spectrometric measurements of DMS and its oxidation products sulfuric acid (H2SO4), methanesulfonic acid (MSA), dimethylsulfoxide (DMSO), dimethylsulfone (DMSO2), methanesulfinic acid (MSIA), methyl thioformate (MTF), methanesulfenic acid (MSEA, CH3SOH), and a compound of the likely structure CH3S(O)(2)OOH in the gas phase, as well as measurements of the sulfate and methanesulfonate aerosol mass fractions. The measurements were performed at the Global Atmosphere Watch (GAW) station Chacaltaya in the Bolivian Andes located at 5240 m above sea level (a.s.l.). DMS and DMS oxidation products are brought to the Andean high-altitude station by Pacific air masses during the dry season after convective lifting over the remote Pacific ocean to 6000-8000 m a.s.l. and subsequent longrange transport in the free troposphere (FT). Most of the DMS reaching the station is already converted to the rather unreactive sulfur reservoirs DMSO2 in the gas phase and methanesulfonate (MS-) in the particle phase, which carried nearly equal amounts of sulfur to the station. The particulate sulfate at Chacaltaya is however dominated by regional volcanic emissions during the time of the measurement and not significantly affected by the marine air masses. In one of the FT events, even some DMS was observed next to reactive intermediates such as methyl thioformate, dimethylsulfoxide, and methanesulfinic acid. Also for this event, back trajectory calculations show that the air masses came from above the ocean (distance > 330 km) with no local surface contacts. This study demonstrates the potential impact of marine DMS emissions on the availability of sulfur containing vapors in the remote free troposphere far away from the ocean.
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22.
  • Scott, C. E., et al. (författare)
  • Impact on short-lived climate forcers increases projected warming due to deforestation
  • 2018
  • Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 9:1
  • Tidskriftsartikel (refereegranskat)abstract
    • The climate impact of deforestation depends on the relative strength of several biogeochemical and biogeophysical effects. In addition to affecting the exchange of carbon dioxide (CO2) and moisture with the atmosphere and surface albedo, vegetation emits biogenic volatile organic compounds (BVOCs) that alter the formation of short-lived climate forcers (SLCFs), which include aerosol, ozone and methane. Here we show that a scenario of complete global deforestation results in a net positive radiative forcing (RF; 0.12 W m-2) from SLCFs, with the negative RF from decreases in ozone and methane concentrations partially offsetting the positive aerosol RF. Combining RFs due to CO2, surface albedo and SLCFs suggests that global deforestation could cause 0.8 K warming after 100 years, with SLCFs contributing 8% of the effect. However, deforestation as projected by the RCP8.5 scenario leads to zero net RF from SLCF, primarily due to nonlinearities in the aerosol indirect effect.
  •  
23.
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24.
  • Arneth, Almut, et al. (författare)
  • Terrestrial biogeochemical feedbacks in the climate system
  • 2010
  • Ingår i: Nature Geoscience. - : Springer Science and Business Media LLC. - 1752-0908 .- 1752-0894. ; 3:8, s. 525-532
  • Forskningsöversikt (refereegranskat)abstract
    • The terrestrial biosphere is a key regulator of atmospheric chemistry and climate. During past periods of climate change, vegetation cover and interactions between the terrestrial biosphere and atmosphere changed within decades. Modern observations show a similar responsiveness of terrestrial biogeochemistry to anthropogenically forced climate change and air pollution. Although interactions between the carbon cycle and climate have been a central focus, other biogeochemical feedbacks could be as important in modulating future climate change. Total positive radiative forcings resulting from feedbacks between the terrestrial biosphere and the atmosphere are estimated to reach up to 0.9 or 1.5 W m(-2) K-1 towards the end of the twenty-first century, depending on the extent to which interactions with the nitrogen cycle stimulate or limit carbon sequestration. This substantially reduces and potentially even eliminates the cooling effect owing to carbon dioxide fertilization of the terrestrial biota. The overall magnitude of the biogeochemical feedbacks could potentially be similar to that of feedbacks in the physical climate system, but there are large uncertainties in the magnitude of individual estimates and in accounting for synergies between these effects.
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25.
  • Bilde, M., et al. (författare)
  • Saturation Vapor Pressures and Transition Enthalpies of Low-Volatility Organic Molecules of Atmospheric Relevance: From Dicarboxylic Acids to Complex Mixtures
  • 2015
  • Ingår i: Chemical Reviews. - : American Chemical Society (ACS). - 0009-2665 .- 1520-6890. ; 115:10, s. 4115-4156
  • Forskningsöversikt (refereegranskat)abstract
    • There are a number of techniques that can be used that differ in terms of whether they fundamentally probe the equilibrium and the temperature range over which they can be applied. The series of homologous, straight-chain dicarboxylic acids have received much attention over the past decade given their atmospheric relevance, commercial availability, and low saturation vapor pressures, thus making them ideal test compounds. Uncertainties in the solid-state saturation vapor pressures obtained from individual methodologies are typically on the order of 50-100%, but the differences between saturation vapor pressures obtained with different methods are approximately 1-4 orders of magnitude, with the spread tending to increase as the saturation vapor pressure decreases. Some of the dicarboxylic acids can exist with multiple solid-state structures that have distinct saturation vapor pressures. Furthermore, the samples on which measurements are performed may actually exist as amorphous subcooled liquids rather than solid crystalline compounds, again with consequences for the measured saturation vapor pressures, since the subcooled liquid phase will have a higher saturation vapor pressure than the crystalline solid phase. Compounds with equilibrium vapor pressures in this range will exhibit the greatest sensitivities in terms of their gas to particle partitioning to uncertainties in their saturation vapor pressures, with consequent impacts on the ability of explicit and semiexplicit chemical models to simulate secondary organic aerosol formation.
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26.
  • Bower, K. N., et al. (författare)
  • ACE-2 HILLCLOUD. An overview of the ACE-2 ground-based cloud experiment
  • 2000
  • Ingår i: Tellus. Series B: Chemical and Physical Meteorology. - : Stockholm University Press. - 0280-6509. ; 52:2, s. 750-778
  • Tidskriftsartikel (refereegranskat)abstract
    • The ACE-2 HILLCLOUD experiment was carried out on the island of Tenerife in June-July 1997 to investigate the interaction of the boundary layer aerosol with a hill cap cloud forming over a ridge to the north-east of the island. The cloud was used as a natural flow through reactor to investigate the dependence of the cloud microphysics and chemistry on the characteristics of the aerosols and trace gases entering cloud, and to simultaneously study the influence of the physical and chemical processes occurring within the cloud on the size distribution, chemical and hygroscopic properties of the aerosol exiting cloud. 5 major ground base sites were used, measuring trace gases and aerosols upwind and downwind of the cloud, and cloud microphysics and chemistry and interstitial aerosol and gases within the cloud on the hill. 8 intensive measurement periods or runs were undertaken during cloud events, (nocturnally for seven of the eight runs) and were carried out in a wide range of airmass conditions from clean maritime to polluted continental. Polluted air was characterised by higher than average concentrations of ozone (> 50 ppbv), fine and accumulation mode aerosols (> 3000 and > 1500 cm -3 , respectively) and higher aerosol mass loadings. Cloud droplet number concentrations N, increased from 50 cm -3 in background maritime air to > 2500 cm -3 in aged polluted continental air, a concentration much higher than had previously been detected. Surprisingly, N was seen to vary almost linearly with aerosol number across this range. The droplet aerosol analyser (DAA) measured higher droplet numbers than the corrected forward scattering spectrometer probe (FSSP) in the most polluted air, but at other times there was good agreement (FSSP = 0.95 DAA with an r 2 = 0.89 for N < 1200 cm -3 ). Background ammonia gas concentrations were around 0.3 ppbv even in air originating over the ocean, another unexpected but important result for the region. NO 2 was present in background concentrations of typically 15 pptv to 100 pptv and NO 3 . (the nitrate radical) was observed at night throughout. Calculations suggest NO 3 . losses were mainly by reaction with DMS to produce nitric acid. Low concentrations of SO 2 (~30 pptv), HNO 3 and HCl were always present. HNO 3 concentrations were higher in polluted episodes and calculations implied that these exceeded those which could be accounted for by NO 2 oxidation. It is presumed that nitric and hydrochloric acids were present as a result of outgassing from aerosol, the HNO 3 from nitrate rich aerosol transported into the region from upwind of Tenerife, and HCl from sea salt aerosol newly formed at the sea surface. The oxidants hydrogen peroxide and ozone were abundant (i.e., were well in excess over SO 2 throughout the experiment). Occasions of significant aerosol growth following cloud processing were observed, particularly in cleaner cases. Observations and modelling suggested this was due mainly to the take up of nitric acid, hydrochloric acid and ammonia by the smallest activated aerosol particles. On a few occasions a small contribution was made by the in-cloud oxidation of S(IV). The implications of these results from HILLCLOUD for the climatologically more important stratocumulus Marine Boundary Layer (MBL) clouds are considered.
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27.
  • Crippa, M., et al. (författare)
  • Organic aerosol components derived from 25 AMS data sets across Europe using a consistent ME-2 based source apportionment approach
  • 2014
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7324. ; 14:12, s. 6159-6176
  • Tidskriftsartikel (refereegranskat)abstract
    • Organic aerosols (OA) represent one of the major constituents of submicron particulate matter (PM1) and comprise a huge variety of compounds emitted by different sources. Three intensive measurement field campaigns to investigate the aerosol chemical composition all over Europe were carried out within the framework of the European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) and the intensive campaigns of European Monitoring and Evaluation Programme (EMEP) during 2008 (May-June and September-October) and 2009 (February-March). In this paper we focus on the identification of the main organic aerosol sources and we define a standardized methodology to perform source apportionment using positive matrix factorization (PMF) with the multilinear engine (ME-2) on Aerodyne aerosol mass spectrometer (AMS) data. Our source apportionment procedure is tested and applied on 25 data sets accounting for two urban, several rural and remote and two high altitude sites; therefore it is likely suitable for the treatment of AMS-related ambient data sets. For most of the sites, four organic components are retrieved, improving significantly previous source apportionment results where only a separation in primary and secondary OA sources was possible. Generally, our solutions include two primary OA sources, i.e. hydrocarbon-like OA (HOA) and biomass burning OA (BBOA) and two secondary OA components, i.e. semi-volatile oxygenated OA (SV-OOA) and low-volatility oxygenated OA (LV-OOA). For specific sites cooking-related (COA) and marine-related sources (MSA) are also separated. Finally, our work provides a large overview of organic aerosol sources in Europe and an interesting set of highly time resolved data for modeling purposes.
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28.
  • Dall'Osto, M., et al. (författare)
  • Novel insights on new particle formation derived from a pan-european observing system
  • 2018
  • Ingår i: Scientific Reports. - : Springer Science and Business Media LLC. - 2045-2322. ; 8
  • Tidskriftsartikel (refereegranskat)abstract
    • The formation of new atmospheric particles involves an initial step forming stable clusters less than a nanometre in size (similar to 10 nm). Although at times, the same species can be responsible for both processes, it is thought that more generally each step comprises differing chemical contributors. Here, we present a novel analysis of measurements from a unique multi-station ground-based observing system which reveals new insights into continental-scale patterns associated with new particle formation. Statistical cluster analysis of this unique 2-year multi-station dataset comprising size distribution and chemical composition reveals that across Europe, there are different major seasonal trends depending on geographical location, concomitant with diversity in nucleating species while it seems that the growth phase is dominated by organic aerosol formation. The diversity and seasonality of these events requires an advanced observing system to elucidate the key processes and species driving particle formation, along with detecting continental scale changes in aerosol formation into the future.
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29.
  • Hussein, T., et al. (författare)
  • Time span and spatial scale of regional new particle formation events over Finland and Southern Sweden
  • 2009
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 9:14, s. 4699-4716
  • Tidskriftsartikel (refereegranskat)abstract
    • We investigated the time span and spatial scale of regional new particle formation (NPF) events in Finland and Southern Sweden using measured particle number size distributions at five background stations. We define the time span of a NPF event as the time period from the first moment when the newly formed mode of aerosol particles is observable below 25 nm until the newly formed mode is not any more distinguishable from other background modes of aerosol particles after growing to bigger sizes. We identify the spatial scale of regional NPF events based on two independent approaches. The first approach is based on the observation within a network of stationary measurement stations and the second approach is based on the time span and the history of air masses back-trajectories. According to the second approach, about 60% and 28% of the events can be traced to distances longer than 220 km upwind from where the events were observed in Southern Finland (Hyytiälä) and Northern Finland (Värriö), respectively. The analysis also showed that the observed regional NPF events started over the continents but not over the Atlantic Ocean. The first approach showed that although large spatial scale NPF events are frequently observed at several locations simultaneously, they are rarely identical (similar characteristics and temporal variations) due to differences in the initial meteorological and geographical conditions between the stations. The growth of the newly formed particles during large spatial scale events can be followed for more than 30 h where the newly formed aerosol particles end up in the Aitken mode (diameter 25–100 nm) and accumulation mode size ranges (diameter 0.1–1 μm). This study showed clear evidence that regional NPF events can pose a significant source for accumulation mode particles over the Scandinavian continent provided that these findings can be generalized to many of the air masses traveling over the European continent.
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30.
  • Jaars, Kerneels, et al. (författare)
  • Measurements of biogenic volatile organic compounds at a grazed savannah grassland agricultural landscape in South Africa
  • 2016
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:24, s. 15665-15688
  • Tidskriftsartikel (refereegranskat)abstract
    • Biogenic volatile organic compounds (BVOCs) play an important role in the chemistry of the troposphere, especially in the formation of tropospheric ozone (O3) and secondary organic aerosols (SOA). Ecosystems produce and emit a large number of BVOCs. It is estimated on a global scale that approximately 90% of annual BVOC emissions are from terrestrial sources. In this study, measurements of BVOCs were conducted at the Welgegund measurement station (South Africa), which is considered to be a regionally representative background site situated in savannah grasslands. Very few BVOC measurements exist for savannah grasslands and results presented in this study are the most extensive for this type of landscape. Samples were collected twice a week for 2h during the daytime and 2h during the night-time through two long-term sampling campaigns from February 2011 to February 2012 and from December 2013 to February 2015, respectively. Individual BVOCs were identified and quantified using a thermal desorption instrument, which was connected to a gas chromatograph and a mass selective detector. The annual median concentrations of isoprene, 2-methyl-3-butene-2-ol (MBO), monoterpene and sesquiterpene (SQT) during the first campaign were 14, 7, 120 and 8pptv, respectively, and 14, 4, 83 and 4pptv, respectively, during the second campaign. The sum of the concentrations of the monoterpenes were at least an order of magnitude higher than the concentrations of other BVOC species during both sampling campaigns, with α-pinene being the most abundant species. The highest BVOC concentrations were observed during the wet season and elevated soil moisture was associated with increased BVOC concentrations. However, comparisons with measurements conducted at other landscapes in southern Africa and the rest of the world that have more woody vegetation indicated that BVOC concentrations were, in general, significantly lower for savannah grasslands. Furthermore, BVOC concentrations were an order of magnitude lower compared to total aromatic concentrations measured at Welgegund. An analysis of concentrations by wind direction indicated that isoprene concentrations were higher from the western sector that is considered to be a relatively clean regional background region with no large anthropogenic point sources, while wind direction did not indicate any significant differences in the concentrations of the other BVOC species. Statistical analysis indicated that soil moisture had the most significant impact on atmospheric levels of MBO, monoterpene and SQT concentrations, whereas temperature had the greatest influence on isoprene levels. The combined O3 formation potentials of all the BVOCs measured calculated with maximum incremental reactivity (MIR) coefficients during the first and second campaign were 1162 and 1022pptv, respectively. α-Pinene and limonene had the highest reaction rates with O3, whereas isoprene exhibited relatively small contributions to O3 depletion. Limonene, α-pinene and terpinolene had the largest contributions to the OH reactivity of BVOCs measured at Welgegund for all of the months during both sampling campaigns.
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31.
  • Keskinen, H., et al. (författare)
  • Evolution of Nanoparticle Composition in CLOUD in Presence of Sulphuric Acid, Ammonia and Organics
  • 2013
  • Ingår i: NUCLEATION AND ATMOSPHERIC AEROSOLS. - : American Institute of Physics (AIP). - 9780735411524 ; , s. 291-294
  • 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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32.
  • Kirkby, Jasper, et al. (författare)
  • Ion-induced nucleation of pure biogenic particles
  • 2016
  • Ingår i: Nature. - : Springer Science and Business Media LLC. - 0028-0836 .- 1476-4687. ; 533:7604, s. 521-526
  • Tidskriftsartikel (refereegranskat)abstract
    • Atmospheric aerosols and their effect on clouds are thought to be important for anthropogenic radiative forcing of the climate, yet remain poorly understood(1). Globally, around half of cloud condensation nuclei originate from nucleation of atmospheric vapours(2). It is thought that sulfuric acid is essential to initiate most particle formation in the atmosphere(3,4), and that ions have a relatively minor role(5). Some laboratory studies, however, have reported organic particle formation without the intentional addition of sulfuric acid, although contamination could not be excluded(6,7). Here we present evidence for the formation of aerosol particles from highly oxidized biogenic vapours in the absence of sulfuric acid in a large chamber under atmospheric conditions. The highly oxygenated molecules (HOMs) are produced by ozonolysis of a-pinene. We find that ions from Galactic cosmic rays increase the nucleation rate by one to two orders of magnitude compared with neutral nucleation. Our experimental findings are supported by quantum chemical calculations of the cluster binding energies of representative HOMs. Ion-induced nucleation of pure organic particles constitutes a potentially widespread source of aerosol particles in terrestrial environments with low sulfuric acid pollution.
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33.
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34.
  • Kulmala, Satu-Maria A., et al. (författare)
  • Type-specific persistence of high-risk human papillomavirus infections in the New Independent States of the former Soviet Union Cohort Study
  • 2007
  • Ingår i: Cancer Epidemiology, Biomarkers and Prevention. - 1055-9965 .- 1538-7755. ; 16:1, s. 17-22
  • Tidskriftsartikel (refereegranskat)abstract
    • Background: Prospective follow-up studies have recently suggested that persistent high-risk human papillomavirus (HPV) infections play a key role in the progression of CIN lesions and in the development of cervical cancer. However, data on type-specific persistence, viral integration, and the role of multiple infections are scanty. Materials and Methods: A cross-sectional/cohort study was conducted between 1998 and 2002 in three New Independent States of the former Soviet Union comprising a cohort of 3,187 women, of whom 854 women were followed up for a mean of 17 months (SD, 11.6). HPV genotyping was done with real-time PCR, detecting HPV types 16, 18/45, 31, 33/52/58, 35, and 39. The integration status of HPV16 was examined by using a novel Taqman-based PCR method. Results: The mean clearance time for the individual high– risk–type infection was 16.5 months (range = 0.9-34.9 months). HPV16 and HPV31 were the most persistent infections (clearance times = 18.1 and 16.2 months, respectively), whereas HPV39 infections cleared most rapidly. The mean copies per cell in HPV18/45, HPV31, HPV33/52/58, and HPV39 infections were higher in persisting HPV infections than in HPV infections that cleared, but the difference was not significant. Integration of HPV16 was not found to correlate with HPV persistence. Conclusions: A large proportion of women remained high-risk HPV positive after 18 months. Coinfection with multiple HPV types, viral load, or integration status did not correlate with persistence of high-risk HPV infections.
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35.
  • Laaksonen, A., et al. (författare)
  • The role of VOC oxidation products in continental new particle formation
  • 2008
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 8:10, s. 2657-2665
  • 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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36.
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37.
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38.
  • Manninen, H. E., et al. (författare)
  • EUCAARI ion spectrometer measurements at 12 European sites - analysis of new particle formation events
  • 2010
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 10:16, s. 7907-7927
  • Tidskriftsartikel (refereegranskat)abstract
    • We present comprehensive results on continuous atmospheric cluster and particle measurements in the size range similar to 1-42 nm within the European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) project. We focused on characterizing the spatial and temporal variation of new particle formation events and relevant particle formation parameters across Europe. Different types of air ion and cluster mobility spectrometers were deployed at 12 field sites across Europe from March 2008 to May 2009. The measurements were conducted in a wide variety of environments, including coastal and continental locations as well as sites at different altitudes (both in the boundary layer and the free troposphere). New particle formation events were detected at all of the 12 field sites during the year-long measurement period. From the data, nucleation and growth rates of newly formed particles were determined for each environment. In a case of parallel ion and neutral cluster measurements, we could also estimate the relative contribution of ion-induced and neutral nucleation to the total particle formation. The formation rates of charged particles at 2 nm accounted for 1-30% of the corresponding total particle formation rates. As a significant new result, we found out that the total particle formation rate varied much more between the different sites than the formation rate of charged particles. This work presents, so far, the most comprehensive effort to experimentally characterize nucleation and growth of atmospheric molecular clusters and nanoparticles at ground-based observation sites on a continental scale.
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39.
  • Nieminen, T., et al. (författare)
  • Parameterization of ion-induced nucleation rates based on ambient = servations
  • 2011
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:7, s. 3393-3402
  • Tidskriftsartikel (refereegranskat)abstract
    • Atmospheric ions participate in the formation of new atmospheric aerosol particles, yet their exact role in this process has remained unclear. Here we derive a new simple parameterization for ion-induced nucleation or, more precisely, for the formation rate of charged 2-nm particles. The parameterization is semi-empirical in the sense that it is based on comprehensive results of one-year-long atmospheric cluster and particle measurements in the size range similar to 1-42 nm within the EUCAARI (European Integrated project on Aerosol Cloud Climate and Air Quality interactions) project. Data from 12 field sites across Europe measured with different types of air ion and cluster mobility spectrometers were used in our analysis, with more in-depth analysis made using data from four stations with concomitant sulphuric acid measurements. The parameterization is given in two slightly different forms: a more accurate one that requires information on sulfuric acid and nucleating organic vapor concentrations, and a simpler one in which this information is replaced with the global radiation intensity. These new parameterizations are applicable to all large-scale atmospheric models containing size-resolved aerosol microphysics, and a scheme to calculate concentrations of sulphuric acid, condensing organic vapours and cluster ions.
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40.
  • Nordin, E. Z., et al. (författare)
  • Secondary organic aerosol formation from idling gasoline passenger vehicle emissions investigated in a smog chamber
  • 2013
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 13:12, s. 6101-6116
  • Tidskriftsartikel (refereegranskat)abstract
    • Gasoline vehicles have recently been pointed out as potentially the main source of anthropogenic secondary organic aerosol (SOA) in megacities. However, there is a lack of laboratory studies to systematically investigate SOA formation in real-world exhaust. In this study, SOA formation from pure aromatic precursors, idling and cold start gasoline exhaust from three passenger vehicles (EURO2-EURO4) were investigated with photo-oxidation experiments in a 6 m(3) smog chamber. The experiments were carried out down to atmospherically relevant organic aerosol mass concentrations. The characterization instruments included a high-resolution aerosol mass spectrometer and a proton transfer mass spectrometer. It was found that gasoline exhaust readily forms SOA with a signature aerosol mass spectrum similar to the oxidized organic aerosol that commonly dominates the organic aerosol mass spectra downwind of urban areas. After a cumulative OH exposure of similar to 5 x 10(6) cm(-3) h, the formed SOA was 1-2 orders of magnitude higher than the primary OA emissions. The SOA mass spectrum from a relevant mixture of traditional light aromatic precursors gave f(43) (mass fraction at m/z = 43), approximately two times higher than to the gasoline SOA. However O:C and H:C ratios were similar for the two cases. Classical C-6-C-9 light aromatic precursors were responsible for up to 60% of the formed SOA, which is significantly higher than for diesel exhaust. Important candidates for additional precursors are higher-order aromatic compounds such as C-10 and C-11 light aromatics, naphthalene and methyl-naphthalenes. We conclude that approaches using only light aromatic precursors give an incomplete picture of the magnitude of SOA formation and the SOA composition from gasoline exhaust.
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41.
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42.
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43.
  • Paramonov, M., et al. (författare)
  • A synthesis of cloud condensation nuclei counter (CCNC) measurements within the EUCAARI network
  • 2015
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7324. ; 15:21, s. 12211-12229
  • Tidskriftsartikel (refereegranskat)abstract
    • Cloud condensation nuclei counter (CCNC) measurements performed at 14 locations around the world within the European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) framework have been analysed and discussed with respect to the cloud condensation nuclei (CCN) activation and hygroscopic properties of the atmospheric aerosol. The annual mean ratio of activated cloud condensation nuclei (N-CCN) to the total number concentration of particles (N-CN), known as the activated fraction A, shows a similar functional dependence on supersaturation S at many locations - exceptions to this being certain marine locations, a free troposphere site and background sites in south-west Germany and northern Finland. The use of total number concentration of particles above 50 and 100 nm diameter when calculating the activated fractions (A(50) and A(100), respectively) renders a much more stable dependence of A on S; A(50) and A(100) also reveal the effect of the size distribution on CCN activation. With respect to chemical composition, it was found that the hygroscopicity of aerosol particles as a function of size differs among locations. The hygroscopicity parameter kappa decreased with an increasing size at a continental site in south-west Germany and fluctuated without any particular size dependence across the observed size range in the remote tropical North Atlantic and rural central Hungary. At all other locations kappa increased with size. In fact, in Hyytiala, Vavihill, Jungfraujoch and Pallas the difference in hygroscopicity between Aitken and accumulation mode aerosol was statistically significant at the 5% significance level. In a boreal environment the assumption of a size-independent kappa can lead to a potentially substantial overestimation of N-CCN at S levels above 0.6 %. The same is true for other locations where kappa was found to increase with size. While detailed information about aerosol hygroscopicity can significantly improve the prediction of N-CCN, total aerosol number concentration and aerosol size distribution remain more important parameters. The seasonal and diurnal patterns of CCN activation and hygroscopic properties vary among three long-term locations, highlighting the spatial and temporal variability of potential aerosol-cloud interactions in various environments.
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44.
  • Petaja, T., et al. (författare)
  • Sub-micron atmospheric aerosols in the surroundings of Marseille and Athens : physical characterization and new particle formation
  • 2007
  • Ingår i: Atmospheric Chemistry And Physics. - 1680-7316 .- 1680-7324. ; 7:10, s. 2705-2720
  • Tidskriftsartikel (refereegranskat)abstract
    • The properties of atmospheric aerosol particles in Marseille and Athens were investigated. The studies were performed in Marseille, France, during July 2002 and in Athens, Greece, during June 2003. The aerosol size distribution and the formation and growth rates of newly formed particles were characterized using Differential Mobility Particle Sizers. Hygroscopic properties were observed using a Hygroscopic Tandem Differential Mobility Analyzer setup. During both campaigns, the observations were performed at suburban, almost rural sites, and the sites can be considered to show general regional background behavior depending on the wind direction. At both sites there were clear pattern for both aerosol number concentration and hygroscopic properties. Nucleation mode number concentration increased during the morning hours indicating new particle formation, which was observed during more than 30% of the days. The observed formation rate was typically more than 1 cm(-3) s(-1), and the growth rate was between 1.2 - 9.9 nm h(-1). Based on hygroscopicity measurements in Athens, the nucleation mode size increase was due to condensation of both water insoluble and water soluble material. However, during a period of less anthropogenic influence, the growth was to a larger extent due to water insoluble components. When urban pollution was more pronounced, growth due to condensation of water soluble material dominated.
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45.
  • Scott, C. E., et al. (författare)
  • Impact of gas-to-particle partitioning approaches on the simulated radiative effects of biogenic secondary organic aerosol
  • 2015
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7324 .- 1680-7316. ; 15:22, s. 12989-13001
  • Tidskriftsartikel (refereegranskat)abstract
    • The oxidation of biogenic volatile organic compounds (BVOCs) gives a range of products, from semi-volatile to extremely low-volatility compounds. To treat the interaction of these secondary organic vapours with the particle phase, global aerosol microphysics models generally use either a thermodynamic partitioning approach (assuming instant equilibrium between semi-volatile oxidation products and the particle phase) or a kinetic approach (accounting for the size dependence of condensation). We show that model treatment of the partitioning of biogenic organic vapours into the particle phase, and consequent distribution of material across the size distribution, controls the magnitude of the first aerosol indirect effect (AIE) due to biogenic secondary organic aerosol (SOA). With a kinetic partitioning approach, SOA is distributed according to the existing condensation sink, enhancing the growth of the smallest particles, i.e. those in the nucleation mode. This process tends to increase cloud droplet number concentrations in the presence of biogenic SOA. By contrast, an approach that distributes SOA according to pre-existing organic mass restricts the growth of the smallest particles, limiting the number that are able to form cloud droplets. With an organically mediated new particle formation mechanism, applying a mass-based rather than a kinetic approach to partitioning reduces our calculated global mean AIE due to biogenic SOA by 24 %. Our results suggest that the mechanisms driving organic partitioning need to be fully understood in order to accurately describe the climatic effects of SOA.
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46.
  • Solomon, A, et al. (författare)
  • Multidomain interventions: state-of-the-art and future directions for protocols to implement precision dementia risk reduction. A user manual for Brain Health Services-part 4 of 6
  • 2021
  • Ingår i: Alzheimer's research & therapy. - : Springer Science and Business Media LLC. - 1758-9193. ; 13:1, s. 171-
  • Tidskriftsartikel (refereegranskat)abstract
    • Although prevention of dementia and late-life cognitive decline is a major public health priority, there are currently no generally established prevention strategies or operational models for implementing such strategies into practice. This article is a narrative review of available evidence from multidomain dementia prevention trials targeting several risk factors and disease mechanisms simultaneously, in individuals without dementia at baseline. Based on the findings, we formulate recommendations for implementing precision risk reduction strategies into new services called Brain Health Services. A literature search was conducted using medical databases (MEDLINE via PubMed and SCOPUS) to select relevant studies: non-pharmacological multidomain interventions (i.e., combining two or more intervention domains), target population including individuals without dementia, and primary outcomes including cognitive/functional performance changes and/or incident cognitive impairment or dementia. Further literature searches covered the following topics: sub-group analyses assessing potential modifiers for the intervention effect on cognition in the multidomain prevention trials, dementia risk scores used as surrogate outcomes in multidomain prevention trials, dementia risk scores in relation to brain pathology markers, and cardiovascular risk scores in relation to dementia. Multidomain intervention studies conducted so far appear to have mixed results and substantial variability in target populations, format and intensity of interventions, choice of control conditions, and outcome measures. Most trials were conducted in high-income countries. The differences in design between the larger, longer-term trials that met vs. did not meet their primary outcomes suggest that multidomain intervention effectiveness may be dependent on a precision prevention approach, i.e., successfully identifying the at-risk groups who are most likely to benefit. One such successful trial has already developed an operational model for implementing the intervention into practice. Evidence on the efficacy of risk reduction interventions is promising, but not yet conclusive. More long-term multidomain randomized controlled trials are needed to fill the current evidence gaps, especially concerning low- and middle-income countries and integration of dementia prevention with existing cerebrovascular prevention programs. A precision risk reduction approach may be most effective for dementia prevention. Such an approach could be implemented in Brain Health Services.
  •  
47.
  • Suni, T., et al. (författare)
  • The significance of land-atmosphere interactions in the Earth system-iLEAPS achievements and perspectives
  • 2015
  • Ingår i: Anthropocene. - : Elsevier BV. - 2213-3054. ; 12, s. 69-84
  • Tidskriftsartikel (refereegranskat)abstract
    • The integrated land ecosystem-atmosphere processes study (iLEAPS) is an international research project focussing on the fundamental processes that link land-atmosphere exchange, climate, the water cycle, and tropospheric chemistry. The project, iLEAPS, was established 2004 within the International Geosphere-Biosphere Programme (IGBP). During its first decade, iLEAPS has proven to be a vital project, well equipped to build a community to address the challenges involved in understanding the complex Earth system: multidisciplinary, integrative approaches for both observations and modeling. The iLEAPS community has made major advances in process understanding, land-surface modeling, and observation techniques and networks. The modes of iLEAPS operation include elucidating specific iLEAPS scientific questions through networks of process studies, field campaigns, modeling, long-term integrated field studies, international interdisciplinary mega-campaigns, synthesis studies, databases, as well as conferences on specific scientific questions and synthesis meetings. Another essential component of iLEAPS is knowledge transfer and it also encourages community-and policy-related outreach activities associated with the regional integrative projects. As a result of its first decade of work, iLEAPS is now setting the agenda for its next phase (2014-2024) under the new international initiative, future Earth. Human influence has always been an important part of land-atmosphere science but in order to respond to the new challenges of global sustainability, closer ties with social science and economics groups will be necessary to produce realistic estimates of land use and anthropogenic emissions by analysing future population increase, migration patterns, food production allocation, land management practices, energy production, industrial development, and urbanization.
  •  
48.
  • Tunved, P, et al. (författare)
  • One year boundary layer aerosol size distribution data from five nordic background stations
  • 2003
  • Ingår i: Atmospheric Chemistry and Physics. - 1680-7324. ; 3, s. 2183-2205
  • 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.
  •  
49.
  • Vaananen, R., et al. (författare)
  • Analysis of particle size distribution changes between three measurement sites in northern Scandinavia
  • 2013
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7324. ; 13:23, s. 11887-11903
  • 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.
  •  
50.
  • Yli-Juuti, T., et al. (författare)
  • Growth rates of nucleation mode particles in Hyytiala during 2003-2009 : variation with particle size, season, data analysis method and ambient conditions
  • 2011
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:24, s. 12865-12886
  • Tidskriftsartikel (refereegranskat)abstract
    • The condensational growth rate of aerosol particles formed in atmospheric new particle formation events is one of the most important factors influencing the lifetime of these particles and their ability to become climatically relevant. Diameter growth rates (GR) of nucleation mode particles were studied based on almost 7 yr of data measured during the years 2003-2009 at a boreal forest measurement station SMEAR II in Hyytiala, Finland. The particle growth rates were estimated using particle size distributions measured with a Differential Mobility Particle Sizer (DMPS), a Balanced Scanning Mobility Analyzer (BSMA) and an Air Ion Spectrometer (AIS). Two GR analysis methods were tested. The particle growth rates were also compared to an extensive set of ambient meteorological parameters and trace gas concentrations to investigate the processes/constituents limiting the aerosol growth. The median growth rates of particles in the nucleation mode size ranges with diameters of 1.5-3 nm, 3-7 nm and 7-20 nm were 1.9 nm h(-1), 3.8 nm h(-1), and 4.3 nm h(-1), respectively. The median relative uncertainties in the growth rates due to the size distribution instrumentation in these size ranges were 25 %, 19 %, and 8 %, respectively. For the smallest particles (1.5-3 nm) the AIS data yielded on average higher growth rate values than the BSMA data, and higher growth rates were obtained from positively charged size distributions as compared with negatively charged particles. For particles larger than 3 nm in diameter no such systematic differences were found. For these particles the uncertainty in the growth rate related to the analysis method, with relative uncertainty of 16 %, was similar to that related to the instruments. The growth rates of 7-20 nm particles showed positive correlation with monoterpene concentrations and their oxidation rate by ozone. The oxidation rate by OH did not show a connection with GR. Our results indicate that the growth of nucleation mode particles in Hyytiala is mainly limited by the concentrations of organic precursors.
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