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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.
  • Mueller, T., et al. (författare)
  • Characterization and intercomparison of aerosol absorption photometers : result of two intercomparison workshops
  • 2011
  • Ingår i: Atmospheric Measurement Techniques. - : Copernicus GmbH. - 1867-1381 .- 1867-8548. ; 4:2, s. 245-268
  • Tidskriftsartikel (refereegranskat)abstract
    • Absorption photometers for real time application have been available since the 1980s, but the use of filter-based instruments to derive information on aerosol properties (absorption coefficient and black carbon, BC) is still a matter of debate. Several workshops have been conducted to investigate the performance of individual instruments over the intervening years. Two workshops with large sets of aerosol absorption photometers were conducted in 2005 and 2007. The data from these instruments were corrected using existing methods before further analysis. The inter-comparison shows a large variation between the responses to absorbing aerosol particles for different types of instruments. The unit to unit variability between instruments can be up to 30% for Particle Soot Absorption Photometers (PSAPs) and Aethalometers. Multi Angle Absorption Photometers (MAAPs) showed a variability of less than 5%. Reasons for the high variability were identified to be variations in sample flow and spot size. It was observed that different flow rates influence system performance with respect to response to absorption and instrumental noise. Measurements with non absorbing particles showed that the current corrections of a cross sensitivity to particle scattering are not sufficient. Remaining cross sensitivities were found to be a function of the total particle load on the filter. The large variation between the response to absorbing aerosol particles for different types of instruments indicates that current correction functions for absorption photometers are not adequate.
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3.
  • 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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4.
  • Laj, P., et al. (författare)
  • Measuring Atmospheric Composition Change
  • 2009
  • Ingår i: Atmospheric Environment. - : Elsevier BV. - 1873-2844 .- 1352-2310. ; 43:33, s. 5351-5414
  • Tidskriftsartikel (refereegranskat)abstract
    • Scientific findings from the last decades have clearly highlighted the need for a more comprehensive approach to atmospheric change processes. In fact, observation of atmospheric composition variables has been an important activity of atmospheric research that has developed instrumental tools (advanced analytical techniques) and platforms (instrumented passenger aircrafts, ground-based in-situ and remote sensing stations, earth observation satellite instruments) providing essential information on the composition of the atmosphere. The variability of the atmospheric system and the extreme complexity of the atmospheric cycles for short-lived gaseous and aerosol species have led to the development of complex models to interpret observations, test our theoretical understanding of atmospheric chemistry and predict future atmospheric composition. The validation of numerical models requires accurate information concerning the variability of atmospheric composition for targeted species via comparison with observations and measurements. In this paper, we provide an overview of recent advances in instrumentation and methodologies for measuring atmospheric composition changes from space, aircraft and the surface as well as recent improvements in laboratory techniques that permitted scientific advance in the field of atmospheric chemistry. Emphasis is given to the most promising and innovative technologies that will become operational in the near future to improve knowledge of atmospheric composition. Our current observation capacity, however, is not satisfactory to understand and predict future atmospheric composition changes, in relation to predicted climate warming. Based on the limitation of the current European observing system, we address the major gaps in a second part of the paper to explain why further developments in current observation strategies are still needed to strengthen and optimise an observing system not only capable of responding to the requirements of atmospheric services but also to newly open scientific questions.
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5.
  • 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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6.
  • Putaud, J. -P, et al. (författare)
  • A European aerosol phenomenology-3 : Physical and chemical characteristics of particulate matter from 60 rural, urban, and kerbside sites across Europe
  • 2010
  • Ingår i: Atmospheric Environment. - : Elsevier BV. - 1352-2310 .- 1873-2844. ; 44:10, s. 1308-1320
  • Tidskriftsartikel (refereegranskat)abstract
    • This paper synthesizes data on aerosol (particulate matter, PM) physical and chemical characteristics, which were obtained over the past decade in aerosol research and monitoring activities at more than 60 natural background, rural, near-city, urban, and kerbside sites across Europe. The data include simultaneously measured PM10 and/or PM2.5 mass on the one hand, and aerosol particle number concentrations or PM chemistry on the other hand. The aerosol data presented in our previous works (Van Dingenen et al., 2004; Putaud et al., 2004) were updated and merged to those collected in the framework of the EU supported European Cooperation in the field of Scientific and Technical action COST633 (Particulate matter: Properties related to health effects). A number of conclusions from our previous studies were confirmed. There is no single ratio between PM2.5 and PM10 mass concentrations valid for all sites, although fairly constant ratios ranging from 0.5 to 0.9 are observed at most individual sites. There is no general correlation between PM mass and particle number concentrations, although particle number concentrations increase with PM2.5 levels at most sites. The main constituents of both PM10 and PM2.5 are generally organic matter, sulfate and nitrate. Mineral dust can also be a major constituent of PM10 at kerbside sites and in Southern Europe. There is a clear decreasing gradient in SO42- and NO3- contribution to PM10 when moving from rural to urban to kerbside sites. In contrast, the total carbon/PM10 ratio increases from rural to kerbside sites. Some new conclusions were also drawn from this work: the ratio between ultrafine particle and total particle number concentration decreases with PM2.5 concentration at all sites but one, and significant gradients in PM chemistry are observed when moving from Northwestern, to Southern to Central Europe. Compiling an even larger number of data sets would have further increased the significance of our conclusions, but collecting all the aerosol data sets obtained also through research projects remains a tedious task.
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7.
  • 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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8.
  • Choularton, T. W., et al. (författare)
  • The Great Dun Fell Cloud Experiment 1993 : An overview
  • 1997
  • Ingår i: Atmospheric Environment. - 1352-2310. ; 31:16, s. 2393-2405
  • Tidskriftsartikel (refereegranskat)abstract
    • The 1993 Ground-based Cloud Experiment on Great Dun Fell used a wide range of measurements of trace gases, aerosol particles and cloud droplets at five sites to study their sources and sinks especially those in cloud. These measurements have been interpreted using a variety of models. The conclusions add to our knowledge of air pollution, acidification of the atmosphere and the ground, eutrophication and climate change. The experiment is designed to use the hill cap cloud as a flow-through reactor, and was conducted in varying levels of pollution typical of much of the rural temperate continental northern hemisphere in spring-time.
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9.
  • Fuzzi, S., et al. (författare)
  • The Po Valley Fog Experiment 1989
  • 1992
  • Ingår i: Tellus. Series B: Chemical and Physical Meteorology. - : Stockholm University Press. - 0280-6509. ; 44:5, s. 448-468
  • Tidskriftsartikel (refereegranskat)abstract
    • An outline is presented here of the Po Valley Fog Experiment 1989, carried out within the EUROTRAC‐GCE project. This experiment is a joint effort by several European research groups from 5 countries. The physical and chemical behaviour of the fog multiphase system was studied experimentally following the temporal evolution of the relevant chemical species in the different phases (gas, droplet, interstitial aerosol) and the evolution of micrometeorological and microphysical conditions, from the pre‐fog situation through the whole fog evolution, to the post‐fog period. Some general results, useful for describing the general features of the fog system, are presented here, while specific scientific questions on the different processes taking place within the system itself will be addressed in other companion papers of this same issue.
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10.
  • Wiedensohler, A., et al. (författare)
  • Mobility particle size spectrometers: harmonization of technical standards and data structure to facilitate high quality long-term observations of atmospheric particle number size distributions
  • 2012
  • Ingår i: Atmospheric Measurement Techniques. - : Copernicus GmbH. - 1867-1381 .- 1867-8548. ; 5:3, s. 657-685
  • Tidskriftsartikel (refereegranskat)abstract
    • Mobility particle size spectrometers often referred to as DMPS (Differential Mobility Particle Sizers) or SMPS (Scanning Mobility Particle Sizers) have found a wide range of applications in atmospheric aerosol research. However, comparability of measurements conducted world-wide is hampered by lack of generally accepted technical standards and guidelines with respect to the instrumental set-up, measurement mode, data evaluation as well as quality control. Technical standards were developed for a minimum requirement of mobility size spectrometry to perform long-term atmospheric aerosol measurements. Technical recommendations include continuous monitoring of flow rates, temperature, pressure, and relative humidity for the sheath and sample air in the differential mobility analyzer. We compared commercial and custom-made inversion routines to calculate the particle number size distributions from the measured electrical mobility distribution. All inversion routines are comparable within few per cent uncertainty for a given set of raw data. Furthermore, this work summarizes the results from several instrument intercomparison workshops conducted within the European infrastructure project EUSAAR (European Supersites for Atmospheric Aerosol Research) and ACTRIS (Aerosols, Clouds, and Trace gases Research InfraStructure Network) to determine present uncertainties especially of custom-built mobility particle size spectrometers. Under controlled laboratory conditions, the particle number size distributions from 20 to 200 nm determined by mobility particle size spectrometers of different design are within an uncertainty range of around +/- 10% after correcting internal particle losses, while below and above this size range the discrepancies increased. For particles larger than 200 nm, the uncertainty range increased to 30%, which could not be explained. The network reference mobility spectrometers with identical design agreed within +/- 4% in the peak particle number concentration when all settings were done carefully. The consistency of these reference instruments to the total particle number concentration was demonstrated to be less than 5%. Additionally, a new data structure for particle number size distributions was introduced to store and disseminate the data at EMEP (European Monitoring and Evaluation Program). This structure contains three levels: raw data, processed data, and final particle size distributions. Importantly, we recommend reporting raw measurements including all relevant instrument parameters as well as a complete documentation on all data transformation and correction steps. These technical and data structure standards aim to enhance the quality of long-term size distribution measurements, their comparability between different networks and sites, and their transparency and traceability back to raw data.
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11.
  • 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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12.
  • Bower, K. N., et al. (författare)
  • The Great Dun Fell experiment 1995 : An overview
  • 1999
  • Ingår i: Atmospheric Research. - 0169-8095. ; 50:3-4, s. 151-184
  • Tidskriftsartikel (refereegranskat)abstract
    • During March and April of 1995 a major international field project was conducted at the UMIST field station site on Great Dun Fell in Cumbria, Northern England. The hill cap cloud which frequently envelopes this site was used as a natural flow through reactor to examine the sensitivity of the cloud microphysics to the aerosol entering the cloud and also to investigate the effects of the cloud in changing the aerosol size distribution, chemical composition and associated optical properties. To investigate these processes, detailed measurements of the cloud water chemistry (including the chemistry of sulphur compounds, organic and inorganic oxidised nitrogen and ammonia), cloud microphysics and properties of the aerosol and trace gas concentrations upwind and downwind of the cap cloud were undertaken. It was found that the cloud droplet number was generally strongly correlated to aerosol number concentration, with up to 2000 activated droplets cm-3 being observed in the most polluted conditions. In such conditions it was inferred that hygroscopic organic compounds were important in the activation process. Often, the size distribution of the aerosol was substantially modified by the cloud processing, largely due to the aqueous phase oxidation of S(IV) to sulphate by hydrogen peroxide, but also through the uptake and fixing of gas phase nitric acid as nitrate, increasing the calculated optical scattering of the aerosol substantially (by up to 24%). New particle formation was also observed in the ultrafine aerosol mode (at about 5 nm) downwind of the cap cloud, particularly in conditions of low total aerosol surface area and in the presence of ammonia and HCl gases. This was seen to occur at night as well as during the day via a mechanism which is not yet understood. The implications of these results for parameterising aerosol growth in Global Climate Models are explored.
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13.
  • Brenninkmeijer, C. A. M., et al. (författare)
  • Civil Aircraft for the regular investigation of the atmosphere based on an instrumented container: The new CARIBIC system
  • 2007
  • Ingår i: Atmospheric Chemistry and Physics. - 1680-7324. ; 7:18, s. 4953-4976
  • Tidskriftsartikel (refereegranskat)abstract
    • An airfreight container with automated instruments for measurement of atmospheric gases and trace compounds was operated on a monthly basis onboard a Boeing 767-300 ER of LTU International Airways during long-distance flights from 1997 to 2002 (CARIBIC, Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container, http://www.caribic-atmospheric.com). Subsequently a more advanced system has been developed, using a larger capacity container with additional equipment and an improved inlet system. CARIBIC phase #2 was implemented on a new long-range aircraft type Airbus A340-600 of the Lufthansa German Airlines (Star Alliance) in December 2004, creating a powerful flying observatory. The instrument package comprises detectors for the measurement of O-3, total and gaseous H2O, NO and NOy, CO, CO2, O-2, Hg, and number concentrations of sub-micrometer particles (>4 nm, >12 nm, and >18 nm diameter). Furthermore, an optical particle counter (OPC) and a proton transfer mass spectrometer (PTR-MS) are incorporated. Aerosol samples are collected for analysis of elemental composition and particle morphology after flight. Air samples are taken in glass containers for laboratory analyses of hydrocarbons, halocarbons and greenhouse gases (including isotopic composition of CO2) in several laboratories. Absorption tubes collect oxygenated volatile organic compounds. Three differential optical absorption spectrometers (DOAS) with their telescopes mounted in the inlet system measure atmospheric trace gases such as BrO, HONO, and NO2. A video camera mounted in the inlet provides information about clouds along the flight track. The flying observatory, its equipment and examples of measurement results are reported.
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14.
  • 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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15.
  • Spracklen, D. V., et al. (författare)
  • Explaining global surface aerosol number concentrations in terms of primary emissions and particle formation
  • 2010
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 10:10, s. 4775-4793
  • Tidskriftsartikel (refereegranskat)abstract
    • We synthesised observations of total particle number (CN) concentration from 36 sites around the world. We found that annual mean CN concentrations are typically 300-2000 cm(-3) in the marine boundary layer and free troposphere (FT) and 1000-10 000 cm(-3) in the continental boundary layer (BL). Many sites exhibit pronounced seasonality with summer time concentrations a factor of 2-10 greater than wintertime concentrations. We used these CN observations to evaluate primary and secondary sources of particle number in a global aerosol microphysics model. We found that emissions of primary particles can reasonably reproduce the spatial pattern of observed CN concentration (R-2=0.46) but fail to explain the observed seasonal cycle (R-2=0.1). The modeled CN concentration in the FT was biased low (normalised mean bias, NMB=-88%) unless a secondary source of particles was included, for example from binary homogeneous nucleation of sulfuric acid and water (NMB=-25%). Simulated CN concentrations in the continental BL were also biased low (NMB=-74%) unless the number emission of anthropogenic primary particles was increased or a mechanism that results in particle formation in the BL was included. We ran a number of simulations where we included an empirical BL nucleation mechanism either using the activation-type mechanism (nucleation rate, J, proportional to gas-phase sulfuric acid concentration to the power one) or kinetic-type mechanism (J proportional to sulfuric acid to the power two) with a range of nucleation coefficients. We found that the seasonal CN cycle observed at continental BL sites was better simulated by BL particle formation (R-2=0.3) than by increasing the number emission from primary anthropogenic sources (R-2=0.18). The nucleation constants that resulted in best overall match between model and observed CN concentrations were consistent with values derived in previous studies from detailed case studies at individual sites. In our model, kinetic and activation-type nucleation parameterizations gave similar agreement with observed monthly mean CN concentrations.
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16.
  • 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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17.
  • Martin, S. T., et al. (författare)
  • An overview of the Amazonian Aerosol Characterization Experiment 2008 (AMAZE-08)
  • 2010
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7324. ; 10:23, s. 11415-11438
  • Tidskriftsartikel (refereegranskat)abstract
    • The Amazon Basin provides an excellent environment for studying the sources, transformations, and properties of natural aerosol particles and the resulting links between biological processes and climate. With this framework in mind, the Amazonian Aerosol Characterization Experiment (AMAZE-08), carried out from 7 February to 14 March 2008 during the wet season in the central Amazon Basin, sought to understand the formation, transformations, and cloud-forming properties of fine-and coarse-mode biogenic aerosol particles, especially as related to their effects on cloud activation and regional climate. Special foci included (1) the production mechanisms of secondary organic components at a pristine continental site, including the factors regulating their temporal variability, and (2) predicting and understanding the cloud-forming properties of biogenic particles at such a site. In this overview paper, the field site and the instrumentation employed during the campaign are introduced. Observations and findings are reported, including the large-scale context for the campaign, especially as provided by satellite observations. New findings presented include: (i) a particle number-diameter distribution from 10 nm to 10 mu m that is representative of the pristine tropical rain forest and recommended for model use; (ii) the absence of substantial quantities of primary biological particles in the submicron mode as evidenced by mass spectral characterization; (iii) the large-scale production of secondary organic material; (iv) insights into the chemical and physical properties of the particles as revealed by thermodenuder-induced changes in the particle number-diameter distributions and mass spectra; and (v) comparisons of ground-based predictions and satellite-based observations of hydrometeor phase in clouds. A main finding of AMAZE-08 is the dominance of secondary organic material as particle components. The results presented here provide mechanistic insight and quantitative parameters that can serve to increase the accuracy of models of the formation, transformations, and cloud-forming properties of biogenic natural aerosol particles, especially as related to their effects on cloud activation and regional climate.
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18.
  • Paasonen, P., et al. (författare)
  • On the roles of sulphuric acid and low-volatility organic vapours in the initial steps of atmospheric new particle formation
  • 2010
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 10:22, s. 11223-11242
  • Tidskriftsartikel (refereegranskat)abstract
    • Sulphuric acid and organic vapours have been identified as the key components in the ubiquitous secondary new particle formation in the atmosphere. In order to assess their relative contribution and spatial variability, we analysed altogether 36 new particle formation events observed at four European measurement sites during EUCAARI campaigns in 2007-2009. We tested models of several different nucleation mechanisms coupling the formation rate of neutral particles (J) with the concentration of sulphuric acid ([H2SO4]) or low-volatility organic vapours ([org]) condensing on sub-4 nm particles, or with a combination of both concentrations. Furthermore, we determined the related nucleation coefficients connecting the neutral nucleation rate J with the vapour concentrations in each mechanism. The main goal of the study was to identify the mechanism of new particle formation and subsequent growth that minimizes the difference between the modelled and measured nucleation rates. At three out of four measurement sites - Hyytiala (Finland), Melpitz (Germany) and San Pietro Capofiume (Italy) - the nucleation rate was closely connected to squared sulphuric acid concentration, whereas in Hohenpeissenberg (Germany) the low-volatility organic vapours were observed to be dominant. However, the nucleation rate at the sulphuric acid dominant sites could not be described with sulphuric acid concentration and a single value of the nucleation coefficient, as K in J=K [H2SO4](2), but the median coefficients for different sites varied over an order of magnitude. This inter-site variation was substantially smaller when the heteromolecular homogenous nucleation between H2SO4 and organic vapours was assumed to take place in addition to homogenous nucleation of H2SO4 alone, i.e., J=K-SA1[H2SO4](2)+K-SA2[H2SO4][org]. By adding in this equation a term describing homomolecular organic vapour nucleation, K-s3[org](2), equally good results were achieved. In general, our results suggest that organic vapours do play a role, not only in the condensational growth of the particles, but also in the nucleation process, with a site-specific degree.
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19.
  • 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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20.
  • Hermann, M, et al. (författare)
  • Submicrometer aerosol particle distributions in the upper troposphere over the mid-latitude North Atlantic - Results from the third route of 'CARIBIC'
  • 2008
  • Ingår i: Tellus. Series B: Chemical and Physical Meteorology. - : Stockholm University Press. - 0280-6509 .- 1600-0889. ; 60:1, s. 106-117
  • Tidskriftsartikel (refereegranskat)abstract
    • Particle number and mass concentrations of submicrometer aerosol particles were determined for the upper troposphere over the mid-latitude North Atlantic within the Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container project (CARIBIC, http://www.caribic-atmospheric.com). Between May 2001 and April 2002, 22 flights from Germany to the Caribbean were conducted using an automated measurement container on a B767 passenger aircraft. Spatial and seasonal probability distributions for ultrafine and Aitken mode particles as well as mass concentrations of particulate sulphur in 8-12 km altitude are presented. High particle number concentrations (mostly 2500-15 000 particles cm(-3) STP) are particularly found in summer over the western North Atlantic Ocean close to the North American continent. The distributions together with an analysis of particle source processes show that deep vertical transport is the dominant process leading to most of the events with high particle number concentrations (greater than or similar to 8000 particles cm(-3) STP) for ultrafine particles as well as for Aitken mode particles. This study emphasizes the importance of deep vertical transport and cloud processing for the concentration of aerosol particles in the upper troposphere.
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21.
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22.
  • Achtert, Peggy, 1982-, et al. (författare)
  • Hygroscopic growth of tropospheric particle number size distributions over the North China Plain
  • 2009
  • Ingår i: Journal of Geophysical Research. - 0148-0227 .- 2156-2202. ; 114, s. D00G07-
  • Tidskriftsartikel (refereegranskat)abstract
    • The hygroscopic growth of atmospheric submicrometer particle size distributions (diameter D-p ranging from 22 to 900 nm) was studied at a rural/suburban site in the North China Plain within the framework of the international Campaigns of Air Quality Research in Beijing and Surrounding Region 2006 (CAREBeijing-2006) research project. The goal was to characterize the regional aerosol in the polluted northeastern plain in China. Size descriptive hygroscopic growth factors (DHGFs) were determined as a function of relative humidity (RH) by relating the particle number size distribution at a dry condition ( 100 nm), the DHGF are substantially higher than in the Aitken particle mode (D-p < 100 nm) as a result of different chemical composition. The size-dependent behavior of the DHGF highlights the relevance of particulate sulfate production over the North China Plain, accomplished by secondary formation from the gas phase and, potentially, liquid phase processes in convective clouds. Furthermore, all results concerning the DHGF show a significant dependency on meteorological air masses. The hygroscopic growth of accumulation mode particles correlates significantly with the PM1-mass fraction of sulfate ions determined by chemical analysis. Finally, this investigation provides a parameterization of the hygroscopic growth of 250-nm particles, which might be useful when predicting visibility and radiative forcing and performing atmospheric aerosol model validations.
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23.
  • Dusek, U., et al. (författare)
  • Water uptake by biomass burning aerosol at sub- and supersaturated conditions: closure studies and implications for the role of organics
  • 2011
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7324. ; 11, s. 9519-9532
  • Tidskriftsartikel (refereegranskat)abstract
    • We investigate the CCN activity of freshly emitted biomass burning particles and their hygroscopic growth at a relative humidity (RH) of 85%. The particles were produced in the Mainz combustion laboratory by controlled burning of various wood types. The water uptake at sub- and supersaturations is parameterized by the hygroscopicity parameter, κ (c.f. Petters and Kreidenweis, 2007). For the wood burns, κ is low, generally around 0.06. The main emphasis of this study is a comparison of κ derived from measurements at sub- and supersaturated conditions (κG and κCCN), in order to see whether the water uptake at 85% RH can predict the CCN properties of the biomass burning particles. Differences in κGand κCCN can arise through solution non-idealities, the presence of slightly soluble or surface active compounds, or non-spherical particle shape. We find that κG and κCCN agree within experimental uncertainties (of around 30%) for particle sizes of 100 and 150 nm; only for 50 nm particles is κCCN larger than κG by a factor of 2. The magnitude of this difference and its dependence on particle size is consistent with the presence of surface active organic compounds. These compounds mainly facilitate the CCN activation of small particles, which form the most concentrated solution droplets at the point of activation. The 50 nm particles, however, are only activated at supersaturations higher than 1% and are therefore of minor importance as CCN in ambient clouds. By comparison with the actual chemical composition of the biomass burning particles, we estimate that the hygroscopicity of the water-soluble organic carbon (WSOC) fraction can be represented by a κWSOC value of approximately 0.2. The effective hygroscopicity of a typical wood burning particle can therefore be represented by a linear mixture of an inorganic component with κ ≅ 0.6, a WSOC component with κ ≅ 0.2, and an insoluble component with κ = 0.
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24.
  • Fountoukis, C., et al. (författare)
  • Simulating ultrafine particle formation in Europe using a regional ctm : contribution of primary emissions versus secondary formation to aerosol number concentrations
  • 2012
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:18, s. 8663-8677
  • Tidskriftsartikel (refereegranskat)abstract
    • A three-dimensional regional chemical transport model (CTM) with detailed aerosol microphysics, PMCAMx-UF, was applied to the European domain to simulate the contribution of direct emissions and secondary formation to total particle number concentrations during May 2008. PMCAMx-UF uses the Dynamic Model for Aerosol Nucleation and the Two-Moment Aerosol Sectional (TOMAS) algorithm to track both aerosol number and mass concentration using a sectional approach. The model predicts nucleation events that occur over scales of hundreds up to thousands of kilometers especially over the Balkans and Southeast Europe. The model predictions were compared against measurements from 7 sites across Europe. The model reproduces more than 70% of the hourly concentrations of particles larger than 10 nm (N-10) within a factor of 2. About half of these particles are predicted to originate from nucleation in the lower troposphere. Regional nucleation is predicted to increase the total particle number concentration by approximately a factor of 3. For particles larger than 100 nm the effect varies from an increase of 20% in the eastern Mediterranean to a decrease of 20% in southern Spain and Portugal resulting in a small average increase of around 1% over the whole domain. Nucleation has a significant effect in the predicted N-50 levels (up to a factor of 2 increase) mainly in areas where there are condensable vapors to grow the particles to larger sizes. A semi-empirical ternary sulfuric acid-ammonia-water parameterization performs better than the activation or the kinetic parameterizations in reproducing the observations. Reducing emissions of ammonia and sulfur dioxide affects certain parts of the number size distribution.
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25.
  • Genberg, Johan, et al. (författare)
  • Light-absorbing carbon in Europe - measurement and modelling, with a focus on residential wood combustion emissions
  • 2013
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 13:17, s. 8719-8738
  • Tidskriftsartikel (refereegranskat)abstract
    • The atmospheric concentration of elemental carbon (EC) in Europe during the six-year period 2005-2010 has been simulated with the EMEP MSC-W model. The model bias compared to EC measurements was less than 20% for most of the examined sites. The model results suggest that fossil fuel combustion is the dominant source of EC in most of Europe but that there are important contributions also from residential wood burning during the cold seasons and, during certain episodes, also from open biomass burning (wildfires and agricultural fires). The modelled contributions from open biomass fires to ground level concentrations of EC were small at the sites included in the present study, <3% of the long-term average of EC in PM10. The modelling of this EC source is subject to many uncertainties, and it was likely underestimated for some episodes. EC measurements and modelled EC were also compared to optical measurements of black carbon (BC). The relationships between EC and BC (as given by mass absorption cross section, MAC, values) differed widely between the sites, and the correlation between observed EC and BC is sometimes poor, making it difficult to compare results using the two techniques and limiting the comparability of BC measurements to model EC results. A new bottom-up emission inventory for carbonaceous aerosol from residential wood combustion has been applied. For some countries the new inventory has substantially different EC emissions compared to earlier estimates. For northern Europe the most significant changes are much lower emissions in Norway and higher emissions in neighbouring Sweden and Finland. For Norway and Sweden, comparisons to source-apportionment data from winter campaigns indicate that the new inventory may improve model-calculated EC from wood burning. Finally, three different model setups were tested with variable atmospheric lifetimes of EC in order to evaluate the model sensitivity to the assumptions regarding hygroscopicity and atmospheric ageing of EC. The standard ageing scheme leads to a rapid transformation of the emitted hydrophobic EC to hygroscopic particles, and generates similar results when assuming that all EC is aged at the point of emission. Assuming hydrophobic emissions and no ageing leads to higher EC concentrations. For the more remote sites, the observed EC concentration was in between the modelled EC using standard ageing and the scenario treating EC as hydrophobic. This could indicate too-rapid EC ageing in the model in relatively clean parts of the atmosphere.
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26.
  • Kulmala, M., et al. (författare)
  • Introduction: European Integrated Project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) : integrating aerosol research from nano to global scales
  • 2009
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 9, s. 2825-2841
  • Tidskriftsartikel (refereegranskat)abstract
    • The European Aerosol Cloud Climate and Air Quality Interactions project EUCAARI is an EU Research Framework 6 integrated project focusing on understanding the interactions of climate and air pollution. EUCAARI works in an integrative and multidisciplinary way from nano-to global scale. EUCAARI brings together several leading European research groups, state-of-the-art infrastructure and some key scientists from third countries to investigate the role of aerosol on climate and air quality. Altogether 48 partners from 25 countries are participating in EUCAARI. During the first 16 months EUCAARI has built operational systems, e. g. established pan-European measurement network for Lagrangian studies and four stations in developing countries. Also an improved understanding of nanoscale processes (like nucleation) has been implemented in global models. Here we present the research methods, organisation, operations and first results of EUCAARI.
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27.
  • Laj, Paolo, et al. (författare)
  • A global analysis of climate-relevant aerosol properties retrieved from the network of Global Atmosphere Watch (GAW) near-surface observatories
  • 2020
  • Ingår i: Atmospheric Measurement Techniques. - : Copernicus GmbH. - 1867-1381 .- 1867-8548. ; 13:8, s. 4353-4392
  • Tidskriftsartikel (refereegranskat)abstract
    • Aerosol particles are essential constituents of the Earth's atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence times, resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in situ near-surface segment of the atmospheric observation system. This paper will provide the widest effort so far to document variability of climate-relevant in situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High-quality data from almost 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single-scattering albedo, and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information, including data provision procedures, quality control and analysis, data policy, and usage of the ground-based aerosol measurement network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system.
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28.
  • Massling, A., et al. (författare)
  • Results and recommendations from an intercomparison of six Hygroscopicity-TDMA systems
  • 2011
  • Ingår i: Atmospheric Measurement Techniques. - : Copernicus GmbH. - 1867-1381 .- 1867-8548. ; 4:3, s. 485-497
  • Tidskriftsartikel (refereegranskat)abstract
    • The performance of six custom-built Hygrocopicity-Tandem Differential Mobility Analyser (H-TDMA) systems was investigated in the frame of an international calibration and intercomparison workshop held in Leipzig, February 2006. The goal of the workshop was to harmonise H-TDMA measurements and develop recommendations for atmospheric measurements and their data evaluation. The H-TDMA systems were compared in terms of the sizing of dry particles, relative humidity (RH) uncertainty, and consistency in determination of number fractions of different hygroscopic particle groups. The experiments were performed in an air-conditioned laboratory using ammonium sulphate particles or an external mixture of ammonium sulphate and soot particles. The sizing of dry particles of the six H-TDMA systems was within 0.2 to 4.2% of the selected particle diameter depending on investigated size and individual system. Measurements of ammonium sulphate aerosol found deviations equivalent to 4.5% RH from the set point of 90% RH compared to results from previous experiments in the literature. Evaluation of the number fraction of particles within the clearly separated growth factor modes of a laboratory generated externally mixed aerosol was done. The data from the H-TDMAs was analysed with a single fitting routine to investigate differences caused by the different data evaluation procedures used for each H-TDMA. The differences between the H-TDMAs were reduced from +12/-13% to +8/-6% when the same analysis routine was applied. We conclude that a common data evaluation procedure to determine number fractions of externally mixed aerosols will improve the comparability of H-TDMA measurements. It is recommended to ensure proper calibration of all flow, temperature and RH sensors in the systems. It is most important to thermally insulate the aerosol humidification unit and the second DMA and to monitor these temperatures to an accuracy of 0.2 degrees C. For the correct determination of external mixtures, it is necessary to take into account size-dependent losses due to diffusion in the plumbing between the DMAs and in the aerosol humidification unit.
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29.
  • Rizzo, L. V., et al. (författare)
  • Long term measurements of aerosol optical properties at a primary forest site in Amazonia
  • 2013
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7324. ; 13:5, s. 2391-2413
  • Tidskriftsartikel (refereegranskat)abstract
    • A long term experiment was conducted in a primary forest area in Amazonia, with continuous in-situ measurements of aerosol optical properties between February 2008 and April 2011, comprising, to our knowledge, the longest database ever in the Amazon Basin. Two major classes of aerosol particles, with significantly different optical properties were identified: coarse mode predominant biogenic aerosols in the wet season (January-June), naturally released by the forest metabolism, and fine mode dominated biomass burning aerosols in the dry season (July-December), transported from regional fires. Dry particle median scattering coefficients at the wavelength of 550 nm increased from 6.3 Mm(-1) to 22 Mm(-1), whereas absorption at 637 nm increased from 0.5 Mm(-1) to 2.8 Mm(-1) from wet to dry season. Most of the scattering in the dry season was attributed to the predominance of fine mode (PM2) particles (40-80% of PM10 mass), while the enhanced absorption coefficients are attributed to the presence of light absorbing aerosols from biomass burning. As both scattering and absorption increased in the dry season, the single scattering albedo (SSA) did not show a significant seasonal variability, in average 0.86 +/- 0.08 at 637 nm for dry aerosols. Measured particle optical properties were used to estimate the aerosol forcing efficiency at the top of the atmosphere. Results indicate that in this primary forest site the radiative balance was dominated by the cloud cover, particularly in the wet season. Due to the high cloud fractions, the aerosol forcing efficiency absolute values were below -3.5 Wm(-2) in 70% of the wet season days and in 46% of the dry season days. Besides the seasonal variation, the influence of out-of-Basin aerosol sources was observed occasionally. Periods of influence of the Manaus urban plume were detected, characterized by a consistent increase on particle scattering (factor 2.5) and absorption coefficients (factor 5). Episodes of biomass burning and mineral dust particles advected from Africa were observed between January and April, characterized by enhanced concentrations of crustal elements (Al, Si, Ti, Fe) and potassium in the fine mode. During these episodes, median particle absorption coefficients increased by a factor of 2, whereas median SSA values decreased by 7 %, in comparison to wet season conditions.
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30.
  • 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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31.
  • Swietlicki, Erik, et al. (författare)
  • Hygroscopic properties of submicrometer atmospheric aerosol particles measured with H-TDMA instruments in various environments : a review
  • 2008
  • Ingår i: Tellus. Series B, Chemical and physical meteorology. - : Stockholm University Press. - 0280-6509 .- 1600-0889. ; 60:3, s. 432-469
  • Forskningsöversikt (refereegranskat)abstract
    • The hygroscopic properties play a vital role for the direct and indirect effects of aerosols on climate, as well as the health effects of particulate matter (PM) by modifying the deposition pattern of inhaled particles in the humid human respiratory tract. Hygroscopic Tandem Differential Mobility Analyzer (H-TDMA) instruments have been used in field campaigns in various environments globally over the last 25 yr to determine the water uptake on submicrometre particles at subsaturated conditions. These investigations have yielded valuable and comprehensive information regarding the particle hygroscopic properties of the atmospheric aerosol, including state of mixing. These properties determine the equilibrium particle size at ambient relative humidities and have successfully been used to calculate the activation of particles at water vapour supersaturation. This paper summarizes the existing published H-TDMA results on the size-resolved submicrometre aerosol particle hygroscopic properties obtained from ground-based measurements at multiple marine, rural, urban and free tropospheric measurement sites. The data is classified into groups of hygroscopic growth indicating the external mixture, and providing clues to the sources and processes controlling the aerosol. An evaluation is given on how different chemical and physical properties affect the hygroscopic growth.
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32.
  • Wang, Z. B., et al. (författare)
  • Contributions of volatile and nonvolatile compounds (at 300 degrees C) to condensational growth of atmospheric nanoparticles: An assessment based on 8.5 years of observations at the Central Europe background site Melpitz
  • 2017
  • Ingår i: Journal of Geophysical Research-Atmospheres. - : American Geophysical Union (AGU). - 2169-897X. ; 122:1, s. 485-497
  • Tidskriftsartikel (refereegranskat)abstract
    • Long-term measurements of particle number size distributions in combination with thermodenuder analysis have been performed since July 2003 at the Central European station of Melpitz, Germany. Up to the end of 2011, 20% of all investigated days during the 8.5 years of measurements showed new particle formation and subsequent growth. To investigate the role of various chemical compound candidates for condensational nanoparticle growth, we focused on nucleation events in which the measured size distributions with and without thermodesorption both showed growth patterns (accounting for up to similar to 85% of all nucleation events). In this study, particulate compounds that volatilize at 300 degrees C were specifically defined as "volatile," in contrast to "nonvolatile" compounds, which remain in the particulate phase after being heated to 300 degrees C. A strong correlation between ambient temperature and growth rate associated with volatile substances (except gaseous sulfuric acid) was found, which implies the importance of organics (possibly oxidized biogenic organic compounds) in particle growth at Melpitz. The contributions of the volatile compounds to the growth rate due to condensation of gaseous sulfuric acid and organics were found to be about 19% and 47%, respectively. The remaining similar to 25% was attributed to nonvolatile residuals, which appear to form gradually during the particle growth process and are characterized as extremely low-volatility compounds. The growth rate associated with volatile components exhibited significant seasonal variation, with the highest value during summertime, whereas the growth rate associated with the nonvolatile fraction showed less fluctuation.
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33.
  • Zanatta, M., et al. (författare)
  • A European aerosol phenomenology-5 : Climatology of black carbon optical properties at 9 regional background sites across Europe
  • 2016
  • Ingår i: Atmospheric Environment. - : Elsevier BV. - 1352-2310 .- 1873-2844. ; 145, s. 346-364
  • Tidskriftsartikel (refereegranskat)abstract
    • A reliable assessment of the optical properties of atmospheric black carbon is of crucial importance for an accurate estimation of radiative forcing. In this study we investigated the spatio-temporal variability of the mass absorption cross-section (MAC) of atmospheric black carbon, defined as light absorption coefficient (sigma(ap)) divided by elemental carbon mass concentration (m(EC)). sigma(ap) and m(EC) have been monitored at supersites of the ACTRIS network for a minimum period of one year. The 9 rural background sites considered in this study cover southern Scandinavia, central Europe and the Mediterranean. sigma(ap) was determined using filter based absorption photometers and m(EC) using a thermal-optical technique. Homogeneity of the data-set was ensured by harmonization of all involved methods and instruments during extensive intercomparison exercises at the European Center for Aerosol Calibration (ECAC). Annual mean values of sigma(ap) at a wavelength of 637 nm vary between 0.66 and 1.3 Mm(-1) in southern Scandinavia, 3.7-11 Mm(-1) in Central Europe and the British Isles, and 2.3-2.8 Mm(-1) in the Mediterranean. Annual mean values of mEC vary between 0.084 and 0.23 mu g m(-3) in southern Scandinavia, 0.28 -1.1 in Central Europe and the British Isles, and 0.22-0.26 in the Mediterranean. Both sigma(ap) and mEC in southern Scandinavia and Central Europe have a distinct seasonality with maxima during the cold season and minima during summer, whereas at the Mediterranean sites an opposite trend was observed. Annual mean MAC values were quite similar across all sites and the seasonal variability was small at most sites. Consequently, a MAC value of 10.0 m(2) g(-1) (geometric standard deviation = 133) at a wavelength of 637 nm can be considered to be representative of the mixed boundary layer at European background sites, where BC is expected to be internally mixed to a large extent. The observed spatial variability is rather small compared to the variability of values in previous literature, indicating that the harmonization efforts resulted in substantially increased precision of the reported MAC. However, absolute uncertainties of the reported MAC values remain as high as +/- 30-70% due to the lack of appropriate reference methods and calibration materials. The mass ratio between elemental carbon and non-light-absorbing matter was used as a proxy for the thickness of coatings around the BC cores, in order to assess the influence of the mixing state on the MAC of BC. Indeed, the MAC was found to increase with increasing values of the coating thickness proxy. This provides evidence that coatings do increase the MAC of atmospheric BC to some extent, which is commonly referred to as lensing effect.
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34.
  • Aliaga, Diego, et al. (författare)
  • Identifying source regions of air masses sampled at the tropical high-altitude site of Chacaltaya using WRF-FLEXPART and cluster analysis
  • 2021
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:21, s. 16453-16477
  • Tidskriftsartikel (refereegranskat)abstract
    • Observations of aerosol and trace gases in the remote troposphere are vital to quantify background concentrations and identify long-term trends in atmospheric composition on large spatial scales. Measurements made at high altitude are often used to study free-tropospheric air; however such high-altitude sites can be influenced by boundary layer air masses. Thus, accurate information on air mass origin and transport pathways to high-altitude sites is required. Here we present a new method, based on the source-receptor relationship (SRR) obtained from backwards WRF-FLEXPART simulations and a k-means clustering approach, to identify source regions of air masses arriving at measurement sites. Our method is tailored to areas of complex terrain and to stations influenced by both local and long-range sources. We have applied this method to the Chacaltaya (CHC) GAW station (5240 m a.s.l.; 16.35 degrees S, 68.13 degrees W) for the 6-month duration of the Southern Hemisphere high-altitude experiment on particle nucleation and growth (SALILNA) to identify where sampled air masses originate and to quantify the influence of the surface and the free troposphere. A key aspect of our method is that it is probabilistic, and for each observation time, more than one air mass (cluster) can influence the station, and the percentage influence of each air mass can be quantified. This is in contrast to binary methods, which label each observation time as influenced by either boundary layer or free-troposphere air masses. Air sampled at CHC is a mix of different provenance. We find that on average 9 % of the air, at any given observation time, has been in contact with the surface within 4 d prior to arriving at CHC. Furthermore, 24 % of the air has been located within the first 1.5 km above ground level (surface included). Consequently, 76 % of the air sampled at CHC originates from the free troposphere. However, pure free-tropospheric influences are rare, and often samples are concurrently influenced by both boundary layer and free-tropospheric air masses. A clear diurnal cycle is present, with very few air masses that have been in contact with the surface being detected at night. The 6-month analysis also shows that the most dominant air mass (cluster) originates in the Amazon and is responsible for 29 % of the sampled air. Furthermore, short-range clusters (origins within 100 km of CHC) have high temporal frequency modulated by local meteorology driven by the diurnal cycle, whereas the mid- and long-range clusters' (> 200 km) variability occurs on timescales governed by synoptic-scale dynamics. To verify the reliability of our method, in situ sulfate observations from CHC are combined with the SRR clusters to correctly identify the (pre-known) source of the sulfate: the Sabancaya volcano located 400 km north-west from the station.
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35.
  • Hamburger, Thomas, et al. (författare)
  • Long-term in situ observations of biomass burning aerosol at a high altitude station in Venezuela - sources, impacts and interannual variability
  • 2013
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 13:19, s. 9837-9853
  • Tidskriftsartikel (refereegranskat)abstract
    • First long-term observations of South American biomass burning aerosol within the tropical lower free troposphere are presented. The observations were conducted between 2007 and 2009 at a high altitude station (4765 m a.s.l.) on the Pico Espejo, Venezuela. Sub-micron particle volume, number concentrations of primary particles and particle absorption were observed. Orographic lifting and shallow convection leads to a distinct diurnal cycle at the station. It enables measurements within the lower free troposphere during night-time and observations of boundary layer air masses during daytime and at their transitional regions. The seasonal cycle is defined by a wet rainy season and a dry biomass burning season. The particle load of biomass burning aerosol is dominated by fires in the Venezuelan savannah. Increases of aerosol concentrations could not be linked to long-range transport of biomass burning plumes from the Amazon basin or Africa due to effective wet scavenging of particles. Highest particle concentrations were observed within boundary layer air masses during the dry season. Ambient sub-micron particle volume reached 1.4 +/- 1.3 mu m(3) cm(-3), refractory particle number concentrations (at 300 degrees C) 510+/-420 cm(-3) and the absorption coefficient 0.91+/-1.2 Mm(-1). The respective concentrations were lowest within the lower free troposphere during the wet season and averaged at 0.19+/-0.25 mu m(3) cm-3, 150+/-94 cm(-3) and 0.15+/-0.26 Mm(-1). A decrease of particle concentrations during the dry seasons from 2007-2009 could be connected to a decrease in fire activity in the wider region of Venezuela using MODIS satellite observations. The variability of biomass burning is most likely linked to the El Nino-Southern Oscillation (ENSO). Low biomass burning activity in the Venezuelan savannah was observed to follow La Nina conditions, high biomass burning activity followed El Nino conditions.
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36.
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37.
  • Hermann, Markus, et al. (författare)
  • An optical particle size spectrometer for aircraft-borne measurements in IAGOS-CARIBIC
  • 2016
  • Ingår i: Atmospheric Measurement Techniques. - : Copernicus GmbH. - 1867-1381 .- 1867-8548. ; 9:5, s. 2179-2194
  • Tidskriftsartikel (refereegranskat)abstract
    • The particle number size distribution is an important parameter to characterize the atmospheric aerosol and its influence on the Earth's climate. Here we describe a new optical particle size spectrometer (OPSS) for measurements of the accumulation mode particle number size distribution in the tropopause region on board a passenger aircraft (IAGOS-CARIBIC observatory: In-service Aircraft for a Global Observing System - Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container). A modified KS93 particle sensor from RION Co., Ltd., together with a new airflow system and a dedicated data acquisition system, is the key component of the CARIBIC OPSS. The instrument records individual particle pulse signal curves in the particle size range 130-1110 nm diameter (for a particle refractive index of 1.47-i0.006) together with a time stamp and thus allows the post-flight choice of the time resolution and the size distribution bin width. The CARIBIC OPSS has a 50 % particle detection diameter of 152 nm and a maximum asymptotic counting efficiency of 98 %. The instrument's measurement performance shows no pressure dependency and no particle coincidence for free tropospheric conditions. The size response function of the CARIBIC OPSS was obtained by a polystyrene latex calibration in combination with model calculations. Particle number size distributions measured with the new OPSS in the lowermost stratosphere agreed within a factor of 2 in concentration with balloon-borne measurements over western North America. Since June 2010 the CARIBIC OPSS is deployed once per month in the IAGOS-CARIBIC observatory.
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38.
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39.
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40.
  • Martinsson, Bengt G., et al. (författare)
  • Droplet nucleation and growth in orographic clouds in relation to the aerosol population
  • 1999
  • Ingår i: Atmospheric Research. - 0169-8095. ; 50:3-4, s. 289-315
  • Tidskriftsartikel (refereegranskat)abstract
    • The formation and development of orographic clouds was studied in a field experiment comprising several measurement sites at a mountain ridge. The influence of the aerosol population present on the cloud microstructure was studied in relation to the dynamics in the cloud formation. Droplet nucleation scavenging was investigated by the introduction of a non-dimensional particle diameter related to the process, and it was found that the scavenging rose rapidly in a relatively narrow particle size interval. The size dependency of the scavenging could partly be explained by external mixture of the aerosol. The large particles in the cloud interstitial aerosol was found to be of a chemical nature which allows for only a very weak uptake of water, implying that the chemical composition of these particles rather than entrainment of dry air prevented the droplet nucleation. The aerosol particle number concentration was found to strongly influence the cloud microstructure. Droplet number concentrations up to approximately 2000 cm-3 were observed together with a substantially reduced effective droplet diameter. The observed effect of elevated particle number concentrations in orographic clouds was generalised to the climatologically more important stratiform clouds by the use of a cloud model. It was found that the microstructure of stratiform clouds was strongly dependent on the aerosol population present as well on the dynamics in the cloud formation.
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41.
  • Martinsson, Bengt G., et al. (författare)
  • Elemental composition of fog interstitial particle size fractions and hydrophobic fractions related to fog droplet nucleation scavenging
  • 1992
  • Ingår i: Tellus. Series B: Chemical and Physical Meteorology. - : Stockholm University Press. - 0280-6509. ; 44:5, s. 593-603
  • Tidskriftsartikel (refereegranskat)abstract
    • The cloud nucleation scavenging process was studied during a joint campaign of the EUROTRAC sub‐project Ground‐based Cloud Experiment. It was found that the particle size has a strong influence on the partitioning of particles between the cloud droplet and the interstitial aerosol reservoirs. A new aerosol sampling unit, the relative humidity processing system, was employed for the extraction of particles with a low growth‐ability with respect to increased relative humidity. The system supplied tracer elements on the particle growth‐ability. These elements could be used to identify a factor related to particle hygroscopic properties, which was in effect as a selector of cloud condensation nuclei.
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42.
  • Martinsson, B. G., et al. (författare)
  • Experimental determination of the connection between cloud droplet size and its dry residue size
  • 1997
  • Ingår i: Atmospheric Environment. - 1352-2310. ; 31:16, s. 2477-2490
  • Tidskriftsartikel (refereegranskat)abstract
    • The droplet activation process and droplet growth was studied during early stages of the formation of orographically-induced clouds. The experimental results were compared with the results obtained with a closed parcel, adiabatic cloud model. Good agreement was in most cases found between model and measurements with respect to cloud droplet number concentration, cloud droplet solute concentration and particle sizes scavenged due to cloud droplet nucleation. The experimental results were mainly obtained with a new instrument, the droplet aerosol analyser (DAA), which allows the determination of ambient sizes of cloud droplets and interstitial aerosol particles directly connected with the size of its dry residue in a two-parameter data acquisition. The resulting three-dimensional data set (ambient size, dry size, number concentration) was utilised to determine several cloud/aerosol properties, whereof some unique.
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43.
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44.
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45.
  • Rose, C., et al. (författare)
  • Frequent nucleation events at the high altitude station of Chacaltaya (5240 m a.s.l.), Bolivia
  • 2015
  • Ingår i: Atmospheric Environment. - : Elsevier BV. - 1352-2310 .- 1873-2844. ; 102, s. 18-29
  • Tidskriftsartikel (refereegranskat)abstract
    • While nucleation may represent one of the major processes responsible for the total aerosol number burden in the atmosphere, and especially at high altitude, new particle formation (NPF) events occurring in the upper part of the troposphere are poorly documented in the literature, particularly in the southern hemisphere. NPF events were detected and analyzed at the highest measurement site in the world, Chacaltaya (5240 m a.s.l.), Bolivia between January 1 and December 31 2012, using a Neutral Aerosol and Ion Spectrometer (NAIS) that detects clusters down to 0.4 nm. NPF frequency at Chacaltaya is one of the highest reported so far (63.9%) and shows a clear seasonal dependency with maximum up to 100% during the dry season. This high seasonality of the NPF events frequency was found to be likely linked to the presence of clouds in the vicinity of the station during the wet season. Multiple NPF events are seen on almost 50% of event days and can reach up to 6 events per day, increasing the potential of nucleation to be the major contributor to the particle number concentrations in the upper troposphere. Ion-induced nucleation (IIN) was 14.8% on average, which is higher than the IIN fractions reported for boundary layer stations. The median formation rate of 2 nm particles computed for first position events is increased during the dry season (1.90 cm(-3) s(-1)) compared to the wet season (1.02 cm(-3) s(-1)), showing that events are more intense, on top of being more frequent during the dry season. On the contrary, particle growth rates (GRs) are on average enhanced during the wet season, which could be explained by higher amount of biogenic volatile organic compounds transported from the Amazon rainforest. The NPF events frequency is clearly enhanced when air masses originate from the oceanic sector, with a frequency of occurrence close to 1. However, based on the particle GRs, we calculate that particles most likely nucleate after the oceanic air masses reach the land and are presumably not originating from the marine free troposphere. The high frequency of NPF events, the occurrence of multiple events per day, and the relatively high formation rates observed at Chacaltaya imply that nucleation and growth are likely to be the major mechanism feeding the upper atmosphere with aerosol particles in this part of the continent.
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46.
  • Schmeissner, T., et al. (författare)
  • Analysis of number size distributions of tropical free tropospheric = rosol particles observed at Pico Espejo (4765 m a.s.l.), Venezuela
  • 2011
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:7, s. 3319-3332
  • Tidskriftsartikel (refereegranskat)abstract
    • The first long-term measurements of aerosol number and size distributions in South-American tropical free troposphere (FT) were performed from March 2007 until March 2009. The measurements took place at the high altitude Atmospheric Research Station Alexander von Humboldt. The station is located on top of the Sierra Nevada mountain ridge at 4765 m a.s.l. nearby the city of Merida, Venezuela. Aerosol size distribution and number concentration data was obtained with a custom-built Differential Mobility Particle Sizer (DMPS) system and a Condensational Particle Counter (CPC). The analysis of the annual and diurnal variability of the tropical FT aerosol focused mainly on possible links to the atmospheric general circulation in the tropics. Considerable annual and diurnal cycles of the particle number concentration were observed. Highest total particle number concentrations were measured during the dry season (January-March, 519+/-613 cm(-3)), lowest during the wet season (July September, 318+/-194 cm(-3)). The more humid FT (relative humidity (RH) range 50-95 %) contained generally higher aerosol particle number concentrations (573+/-768 cm(-3) during dry season, 320+/-195 cm(-3) during wet season) than the dry FT (RH <50 %, 454+/-332 cm(-3) during dry season, 275+/-172 cm(-3) during wet season), indicating the importance of convection for aerosol distributions in the tropical FT. The diurnal cycle in the variability of the particle number concentration was mainly driven by local orography.
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47.
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48.
  • Titos, Gloria, et al. (författare)
  • A global study of hygroscopicity-driven light-scattering enhancement in the context of other in situ aerosol optical properties
  • 2021
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:17, s. 13031-13050
  • Tidskriftsartikel (refereegranskat)abstract
    • The scattering and backscattering enhancement factors (f(RH) and fb(RH)) describe how aerosol particle light scattering and backscattering, respectively, change with relative humidity (RH). They are important parameters in estimating direct aerosol radiative forcing (DARF). In this study we use the dataset presented in Burgos et al. (2019) that compiles f(RH) and fb(RH) measurements at three wavelengths (i.e., 450, 550 and 700 nm) performed with tandem nephelometer systems at multiple sites around the world. We present an overview of f(RH) and fb(RH) based on both long-term and campaign observations from 23 sites representing a range of aerosol types. The scattering enhancement shows a strong variability from site to site, with no clear pattern with respect to the total scattering coefficient. In general, higher f(RH) is observed at Arctic and marine sites, while lower values are found at urban and desert sites, although a consistent pattern as a function of site type is not observed. The backscattering enhancement fb(RH) is consistently lower than f(RH) at all sites, with the difference between f(RH) and fb(RH) increasing for aerosol with higher f(RH). This is consistent with Mie theory, which predicts higher enhancement of the light scattering in the forward than in the backward direction as the particle takes up water. Our results show that the scattering enhancement is higher for PM1 than PM10 at most sites, which is also supported by theory due to the change in scattering efficiency with the size parameter that relates particle size and the wavelength of incident light. At marine-influenced sites this difference is enhanced when coarse particles (likely sea salt) predominate. For most sites, f(RH) is observed to increase with increasing wavelength, except at sites with a known dust influence where the spectral dependence of f(RH) is found to be low or even exhibit the opposite pattern. The impact of RH on aerosol properties used to calculate radiative forcing (e.g., single-scattering albedo, ω0, and backscattered fraction, b) is evaluated. The single-scattering albedo generally increases with RH, while b decreases. The net effect of aerosol hygroscopicity on radiative forcing efficiency (RFE) is an increase in the absolute forcing effect (negative sign) by a factor of up to 4 at RH = 90 % compared to dry conditions (RH < 40 %). Because of the scarcity of scattering enhancement measurements, an attempt was made to use other more commonly available aerosol parameters (i.e., ω0 and scattering Ångström exponent, αsp) to parameterize f(RH). The majority of sites (75 %) showed a consistent trend with ω0 (higher f(RH = 85 %) for higher ω0), while no clear pattern was observed between f(RH = 85 %) and αsp. This suggests that aerosol ω0 is more promising than αsp as a surrogate for the scattering enhancement factor, although neither parameter is ideal. Nonetheless, the qualitative relationship observed between ω0 and f(RH) could serve as a constraint on global model simulations.
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49.
  • Wang, Z. B., et al. (författare)
  • Characteristics of regional new particle formation in urban and regional background environments in the North China Plain
  • 2013
  • Ingår i: Atmos. Chem. Phys.. - : Copernicus Publications. - 1680-7324. ; 13:24, s. 12495-12506
  • Tidskriftsartikel (refereegranskat)abstract
    • Long-term measurements of particle number size distributions were carried out both at an urban background site (Peking University, PKU) and a regional Global Atmospheric Watch station (Shangdianzi, SDZ) from March to November in 2008. In total, 52 new particle formation (NPF) events were observed simultaneously at both sites, indicating that this is a regional phenomenon in the North China Plain. On average, the mean condensation sink value before the nucleation events started was 0.025 s−1 in the urban environment, which was 1.6 times higher than that at regional site. However, higher particle formation and growth rates were observed at PKU (10.8 cm−3 s−1 and 5.2 nm h−1) compared with those at SDZ (4.9 cm−3 s−1 and 4.0 nm h−1). These results implied that precursors were much more abundant in the polluted urban environment. Different from the observations in cleaner environments, the background conditions of the observed particle homogeneous nucleation events in the North China Plain could be characterized as the co-existing of a stronger source of precursor gases and a higher condensational sink of pre-existing aerosol particles. Secondary aerosol formation following nucleation events results in an increase of particle mass concentration, particle light scattering coefficient, and cloud condensation nuclei (CCN) number concentration, with consequences on visibility, radiative effects, and air quality. Typical regional NPF events with significant particle nucleation rates and subsequent particle growth over a sufficiently long time period at both sites were chosen to investigate the influence of NPF on the number concentration of "potential" CCN. As a result, the NPF and the subsequent condensable growth increased the CCN number concentration in the North China Plain by factors in the range from 5.6 to 8.7. Moreover, the potential contribution of anthropogenic emissions to the CCN number concentration was more than 50%, to which more attention should be drawn in regional and global climate modeling, especially in the polluted urban areas.
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50.
  • Wang, Z. B., et al. (författare)
  • Connection of organics to atmospheric new particle formation and growth at an urban site of Beijing
  • 2015
  • Ingår i: Atmospheric Environment. - : Elsevier BV. - 1352-2310. ; 103, s. 7-17
  • Tidskriftsartikel (refereegranskat)abstract
    • In the present work, we aim to elucidate the roles of low-volatility organic vapors in atmospheric new particle formation in urban Beijing. Proposed organic molecules are derived from both the ambient measurement and the reasonable proxy. Several representations for the nucleation theories involving sulfuric acid and organic vapors are evaluated. The particle nucleation rates show good correlations both with sulfuric acid and organic vapors, suggesting that both play an important role in the atmospheric new particle formation. For the entire data set, the best fit (R=0.79, slope=1.1) between the observed and modeled particle nucleation rates is achieved with the homogenous nucleation theory of sulfuric acid (both homomolecularly and heteromolecularly) with separate coefficients in J=KSA1[H2SO4]2+KSA2[H2SO4][Org]. In addition, sulfuric acid concentration only contributes a small fraction (<15%) to the total observed growth rate. The growth rates of 7–30nm particles show positive correlation with the organic vapors oxidized by ozone, suggesting that particle nucleation may be controlled by the light intensity or OH concentration, while the growth of nucleation mode particles seems to be limited more by the concentrations of the organic precursors.
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