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  • Copernicus GmbH  (19)
  • 1
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 11, No. 24 ( 2011-12-21), p. 13061-13143
    Abstract: 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.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2011
    detail.hit.zdb_id: 2092549-9
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  • 2
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 10, No. 16 ( 2010-08-25), p. 7907-7927
    Abstract: Abstract. We present comprehensive results on continuous atmospheric cluster and particle measurements in the size range ~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.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2010
    detail.hit.zdb_id: 2092549-9
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  • 3
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 14, No. 8 ( 2014-04-30), p. 4327-4348
    Abstract: 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.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2014
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  • 4
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 8, No. 3 ( 2015-03-12), p. 1207-1215
    Abstract: Abstract. In this work various microphysical properties including mass concentration, size distribution and morphology of aerosol particles generated by laser ablation of a high purity graphite sample were investigated in detail. Supplementary chemical analysis of the generated particles including microstructure investigation by high-resolution transmission electron microscopy (HRTEM) and Raman spectroscopy were also made. These measurements proved that the proposed method can be used to model the real atmospheric carbonaceous particulate under various climate relevant conditions regarding its specific properties investigated here. However, to introduce the presented methodology as a novel BC surrogate, further improvement and investigation including simplification in experimental setup, comprehensive analysis of thermochemical refractiveness and optical responses of the generated particles as well as comparative study with the presently available concurrent surrogates are required. The related results of these issues are planned to be demonstrated in other studies.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2015
    detail.hit.zdb_id: 2505596-3
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  • 5
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 11, No. 11 ( 2011-06-15), p. 5505-5538
    Abstract: Abstract. Two years of harmonized aerosol number size distribution data from 24 European field monitoring sites have been analysed. The results give a comprehensive overview of the European near surface aerosol particle number concentrations and number size distributions between 30 and 500 nm of dry particle diameter. Spatial and temporal distribution of aerosols in the particle sizes most important for climate applications are presented. We also analyse the annual, weekly and diurnal cycles of the aerosol number concentrations, provide log-normal fitting parameters for median number size distributions, and give guidance notes for data users. Emphasis is placed on the usability of results within the aerosol modelling community. We also show that the aerosol number concentrations of Aitken and accumulation mode particles (with 100 nm dry diameter as a cut-off between modes) are related, although there is significant variation in the ratios of the modal number concentrations. Different aerosol and station types are distinguished from this data and this methodology has potential for further categorization of stations aerosol number size distribution types. The European submicron aerosol was divided into characteristic types: Central European aerosol, characterized by single mode median size distributions, unimodal number concentration histograms and low variability in CCN-sized aerosol number concentrations; Nordic aerosol with low number concentrations, although showing pronounced seasonal variation of especially Aitken mode particles; Mountain sites (altitude over 1000 m a.s.l.) with a strong seasonal cycle in aerosol number concentrations, high variability, and very low median number concentrations. Southern and Western European regions had fewer stations, which decreases the regional coverage of these results. Aerosol number concentrations over the Britain and Ireland had very high variance and there are indications of mixed air masses from several source regions; the Mediterranean aerosol exhibit high seasonality, and a strong accumulation mode in the summer. The greatest concentrations were observed at the Ispra station in Northern Italy with high accumulation mode number concentrations in the winter. The aerosol number concentrations at the Arctic station Zeppelin in Ny-Å lesund in Svalbard have also a strong seasonal cycle, with greater concentrations of accumulation mode particles in winter, and dominating summer Aitken mode indicating more recently formed particles. Observed particles did not show any statistically significant regional work-week or weekday related variation in number concentrations studied. Analysis products are made for open-access to the research community, available in a freely accessible internet site. The results give to the modelling community a reliable, easy-to-use and freely available comparison dataset of aerosol size distributions.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2011
    detail.hit.zdb_id: 2092549-9
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  • 6
    Online Resource
    Online Resource
    Copernicus GmbH ; 2015
    In:  Proceedings of the International Association of Hydrological Sciences Vol. 370 ( 2015-06-11), p. 89-95
    In: Proceedings of the International Association of Hydrological Sciences, Copernicus GmbH, Vol. 370 ( 2015-06-11), p. 89-95
    Abstract: Abstract. The current work addresses one of the key building blocks towards an improved understanding of flood processes and associated changes in flood characteristics and regimes in Europe: the development of a comprehensive, extensive European flood database. The presented work results from ongoing cross-border research collaborations initiated with data collection and joint interpretation in mind. A detailed account of the current state, characteristics and spatial and temporal coverage of the European Flood Database, is presented. At this stage, the hydrological data collection is still growing and consists at this time of annual maximum and daily mean discharge series, from over 7000 hydrometric stations of various data series lengths. Moreover, the database currently comprises data from over 50 different data sources. The time series have been obtained from different national and regional data sources in a collaborative effort of a joint European flood research agreement based on the exchange of data, models and expertise, and from existing international data collections and open source websites. These ongoing efforts are contributing to advancing the understanding of regional flood processes beyond individual country boundaries and to a more coherent flood research in Europe.
    Type of Medium: Online Resource
    ISSN: 2199-899X
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2015
    detail.hit.zdb_id: 2827925-6
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  • 7
    Online Resource
    Online Resource
    Copernicus GmbH ; 2006
    In:  Atmospheric Chemistry and Physics Vol. 6, No. 11 ( 2006-08-30), p. 3563-3570
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 6, No. 11 ( 2006-08-30), p. 3563-3570
    Abstract: Abstract. We present here the optical properties of humic-like substances (HULIS) isolated from the fine fraction of biomass-burning aerosol collected in the Amazon basin during the LBA-SMOCC (Large scale Biosphere atmosphere experiment in Amazonia – SMOke aerosols, Clouds, rainfall and Climate) experiment in September 2002. From the isolated HULIS, aerosol particles were generated and their scattering and absorption coefficients measured. The size distribution and mass of the particles were also recorded. The value of the index of refraction was derived from "closure" calculations based on particle size, scattering and absorption measurements. On average, the complex index of refraction at 532 nm of HULIS collected during day and nighttime was 1.65–0.0019i and 1.69–0.0016i, respectively. In addition, the imaginary part of the complex index of refraction was calculated using the measured absorption coefficient of the bulk HULIS. The mass absorption coefficient of the HULIS at 532 nm was found to be quite low (0.031 and 0.029 m2 g−1 for the day and night samples, respectively). However, due to the high absorption Ångström exponent (6–7) of HULIS, the specific absorption increases substantially towards shorter wavelengths (~2–3 m2 g−1 at 300 nm), causing a relatively high (up to 50%) contribution to the light absorption of our Amazonian aerosol at 300 nm. For the relative contribution of HULIS to light absorption in the entire solar spectrum, lower values (6.4–8.6%) are obtained, but those are still not negligible.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2006
    detail.hit.zdb_id: 2092549-9
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  • 8
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 8, No. 1 ( 2015-01-09), p. 125-147
    Abstract: Abstract. The monosaccharide anhydrides (MAs) levoglucosan, galactosan and mannosan are products of incomplete combustion and pyrolysis of cellulose and hemicelluloses, and are found to be major constituents of biomass burning (BB) aerosol particles. Hence, ambient aerosol particle concentrations of levoglucosan are commonly used to study the influence of residential wood burning, agricultural waste burning and wildfire emissions on ambient air quality. A European-wide intercomparison on the analysis of the three monosaccharide anhydrides was conducted based on ambient aerosol quartz fiber filter samples collected at a Norwegian urban background site during winter. Thus, the samples' content of MAs is representative for BB particles originating from residential wood burning. The purpose of the intercomparison was to examine the comparability of the great diversity of analytical methods used for analysis of levoglucosan, mannosan and galactosan in ambient aerosol filter samples. Thirteen laboratories participated, of which three applied high-performance anion-exchange chromatography (HPAEC), four used high-performance liquid chromatography (HPLC) or ultra-performance liquid chromatography (UPLC) and six resorted to gas chromatography (GC). The analytical methods used were of such diversity that they should be considered as thirteen different analytical methods. All of the thirteen laboratories reported levels of levoglucosan, whereas nine reported data for mannosan and/or galactosan. Eight of the thirteen laboratories reported levels for all three isomers. The accuracy for levoglucosan, presented as the mean percentage error (PE) for each participating laboratory, varied from −63 to 20%; however, for 62% of the laboratories the mean PE was within ±10%, and for 85% the mean PE was within ±20%. For mannosan, the corresponding range was −60 to 69%, but as for levoglucosan, the range was substantially smaller for a subselection of the laboratories; i.e. for 33% of the laboratories the mean PE was within ±10%. For galactosan, the mean PE for the participating laboratories ranged from −84 to 593%, and as for mannosan 33% of the laboratories reported a mean PE within ±10%. The variability of the various analytical methods, as defined by their minimum and maximum PE value, was typically better for levoglucosan than for mannosan and galactosan, ranging from 3.2 to 41% for levoglucosan, from 10 to 67% for mannosan and from 6 to 364% for galactosan. For the levoglucosan to mannosan ratio, which may be used to assess the relative importance of softwood versus hardwood burning, the variability only ranged from 3.5 to 24 . To our knowledge, this is the first major intercomparison on analytical methods used to quantify monosaccharide anhydrides in ambient aerosol filter samples conducted and reported in the scientific literature. The results show that for levoglucosan the accuracy is only slightly lower than that reported for analysis of SO42- (sulfate) on filter samples, a constituent that has been analysed by numerous laboratories for several decades, typically by ion chromatography and which is considered a fairly easy constituent to measure. Hence, the results obtained for levoglucosan with respect to accuracy are encouraging and suggest that levels of levoglucosan, and to a lesser extent mannosan and galactosan, obtained by most of the analytical methods currently used to quantify monosaccharide anhydrides in ambient aerosol filter samples, are comparable. Finally, the various analytical methods used in the current study should be tested for other aerosol matrices and concentrations as well, the most obvious being summertime aerosol samples affected by wildfires and/or agricultural fires.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2015
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  • 9
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 10, No. 12 ( 2010-06-28), p. 5625-5639
    Abstract: Abstract. HUmic-LIke Substances (HULIS) have been identified as major contributors to the organic carbon in atmospheric aerosol. The term "HULIS" is used to describe the organic material found in aerosol particles that resembles the humic organic material in rivers and sea water and in soils. In this study, two sets of filter samples from atmospheric aerosols were collected at different sites. One set of samples was collected at the K-puszta rural site in Hungary, about 80 km SE of Budapest, and a second was collected at a site in Rondônia, Amazonia, Brazil, during the Large-Scale Biosphere-Atmosphere Experiment in Amazonia – Smoke Aerosols, Clouds, Rainfall and Climate (LBA-SMOCC) biomass burning season experiment. HULIS were extracted from the samples and their hygroscopic properties were studied using a Hygroscopicity Tandem Differential Mobility Analyzer (H-TDMA) at relative humidity (RH) 〈100%, and a cloud condensation nucleus counter (CCNC) at RH 〉100%. The H-TDMA measurements were carried out at a dry diameter of 100 nm and for RH ranging from 30 to 98%. At 90% RH the HULIS samples showed diameter growth factors between 1.04 and 1.07, reaching values of 1.4 at 98% RH. The cloud nucleating properties of the two sets of aerosol samples were analysed using two types of thermal static cloud condensation nucleus counters. Two different parameterization models were applied to investigate the potential effect of HULIS surface activity, both yielding similar results. For the K-puszta winter HULIS sample, the surface tension at the point of activation was estimated to be lowered by between 34% (47.7 mN/m) and 31% (50.3 mN/m) for dry sizes between 50 and 120 nm in comparison to pure water. A moderate lowering was also observed for the entire water soluble aerosol sample, including both organic and inorganic compounds, where the surface tension was decreased by between 2% (71.2 mN/m) and 13% (63.3 mN/m).
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2010
    detail.hit.zdb_id: 2092549-9
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  • 10
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 7, No. 9 ( 2007-05-10), p. 2371-2398
    Abstract: Abstract. In order to predict the physical properties of aerosol particles, it is necessary to adequately capture the behaviour of the ubiquitous complex organic components. One of the key properties which may affect this behaviour is the contribution of the organic components to the surface tension of aqueous particles in the moist atmosphere. Whilst the qualitative effect of organic compounds on solution surface tensions has been widely reported, our quantitative understanding on mixed organic and mixed inorganic/organic systems is limited. Furthermore, it is unclear whether models that exist in the literature can reproduce the surface tension variability for binary and higher order multi-component organic and mixed inorganic/organic systems of atmospheric significance. The current study aims to resolve both issues to some extent. Surface tensions of single and multiple solute aqueous solutions were measured and compared with predictions from a number of model treatments. On comparison with binary organic systems, two predictive models found in the literature provided a range of values resulting from sensitivity to calculations of pure component surface tensions. Results indicate that a fitted model can capture the variability of the measured data very well, producing the lowest average percentage deviation for all compounds studied. The performance of the other models varies with compound and choice of model parameters. The behaviour of ternary mixed inorganic/organic systems was unreliably captured by using a predictive scheme and this was dependent on the composition of the solutes present. For more atmospherically representative higher order systems, entirely predictive schemes performed poorly. It was found that use of the binary data in a relatively simple mixing rule, or modification of an existing thermodynamic model with parameters derived from binary data, was able to accurately capture the surface tension variation with concentration. Thus, it would appear that in order to model multi-component surface tensions involving compounds used in this study one requires the use of appropriate binary data. However, results indicate that the use of theoretical frameworks which contain parameters derived from binary data may predict unphysical behaviour when taken beyond the concentration ranges used to fit such parameters. The effect of deviations between predicted and measured surface tensions on predicted critical saturation ratios was quantified, by incorporating the surface tension models into an existing thermodynamic framework whilst firstly neglecting bulk to surface partitioning. Critical saturation ratios as a function of dry size for all of the multi-component systems were computed and it was found that deviations between predictions increased with decreasing particle dry size. As expected, use of the surface tension of pure water, rather than calculate the influence of the solutes explicitly, led to a consistently higher value of the critical saturation ratio indicating that neglect of the compositional effects will lead to significant differences in predicted activation behaviour even at large particle dry sizes. Following this two case studies were used to study the possible effect of bulk to surface partitioning on critical saturation ratios. By employing various assumptions it was possible to perform calculations not only for a binary system but also for a mixed organic system. In both cases this effect lead to a significant increase in the predicted critical supersaturation ratio compared to the above treatment. Further analysis of this effect will form the focus of future work.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2007
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