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  • 1
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    Atmospheric nucleation: highlights of the EUCAARI project and future directions
    Copernicus GmbH ; 2010
    In:  Atmospheric Chemistry and Physics Vol. 10, No. 22 ( 2010-11-18), p. 10829-10848
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 10, No. 22 ( 2010-11-18), p. 10829-10848
    Abstract: Abstract. Within the project EUCAARI (European Integrated project on Aerosol Cloud Climate and Air Quality interactions), atmospheric nucleation was studied by (i) developing and testing new air ion and cluster spectrometers, (ii) conducting homogeneous nucleation experiments for sulphate and organic systems in the laboratory, (iii) investigating atmospheric nucleation mechanism under field conditions, and (iv) applying new theoretical and modelling tools for data interpretation and development of parameterisations. The current paper provides a synthesis of the obtained results and identifies the remaining major knowledge gaps related to atmospheric nucleation. The most important technical achievement of the project was the development of new instruments for measuring sub-3 nm particle populations, along with the extensive application of these instruments in both the laboratory and the field. All the results obtained during EUCAARI indicate that sulphuric acid plays a central role in atmospheric nucleation. However, also vapours other than sulphuric acid are needed to explain the nucleation and the subsequent growth processes, at least in continental boundary layers. Candidate vapours in this respect are some organic compounds, ammonia, and especially amines. Both our field and laboratory data demonstrate that the nucleation rate scales to the first or second power of the nucleating vapour concentration(s). This agrees with the few earlier field observations, but is in stark contrast with classical thermodynamic nucleation theories. The average formation rates of 2-nm particles were found to vary by almost two orders of magnitude between the different EUCAARI sites, whereas the formation rates of charged 2-nm particles varied very little between the sites. Overall, our observations are indicative of frequent, yet moderate, ion-induced nucleation usually outweighed by much stronger neutral nucleation events in the continental lower troposphere. The most concrete outcome of the EUCAARI nucleation studies are the new semi-empirical nucleation rate parameterizations based on field observations, along with updated aerosol formation parameterizations.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    DOI: 10.5194/acp-10-10829-2010
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2010
    detail.hit.zdb_id: 2092549-9
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  • 2
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    General overview: European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) – integrating aerosol research from nano to global scales
    Copernicus GmbH ; 2011
    In:  Atmospheric Chemistry and Physics Vol. 11, No. 24 ( 2011-12-21), p. 13061-13143
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 11, No. 24 ( 2011-12-21), p. 13061-13143
    Abstract: Abstract. In this paper we describe and summarize the main achievements of the European Aerosol Cloud Climate and Air Quality Interactions project (EUCAARI). EUCAARI started on 1 January 2007 and ended on 31 December 2010 leaving a rich legacy including: (a) a comprehensive database with a year of observations of the physical, chemical and optical properties of aerosol particles over Europe, (b) comprehensive aerosol measurements in four developing countries, (c) a database of airborne measurements of aerosols and clouds over Europe during May 2008, (d) comprehensive modeling tools to study aerosol processes fron nano to global scale and their effects on climate and air quality. In addition a new Pan-European aerosol emissions inventory was developed and evaluated, a new cluster spectrometer was built and tested in the field and several new aerosol parameterizations and computations modules for chemical transport and global climate models were developed and evaluated. These achievements and related studies have substantially improved our understanding and reduced the uncertainties of aerosol radiative forcing and air quality-climate interactions. The EUCAARI results can be utilized in European and global environmental policy to assess the aerosol impacts and the corresponding abatement strategies.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    DOI: 10.5194/acp-11-13061-2011
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2011
    detail.hit.zdb_id: 2092549-9
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  • 3
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    Reactive Halogens in the Marine Boundary Layer (RHaMBLe): the tropical North Atlantic experiments
    Copernicus GmbH ; 2010
    In:  Atmospheric Chemistry and Physics Vol. 10, No. 3 ( 2010-02-01), p. 1031-1055
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 10, No. 3 ( 2010-02-01), p. 1031-1055
    Abstract: Abstract. The NERC UK SOLAS-funded Reactive Halogens in the Marine Boundary Layer (RHaMBLe) programme comprised three field experiments. This manuscript presents an overview of the measurements made within the two simultaneous remote experiments conducted in the tropical North Atlantic in May and June 2007. Measurements were made from two mobile and one ground-based platforms. The heavily instrumented cruise D319 on the RRS Discovery from Lisbon, Portugal to São Vicente, Cape Verde and back to Falmouth, UK was used to characterise the spatial distribution of boundary layer components likely to play a role in reactive halogen chemistry. Measurements onboard the ARSF Dornier aircraft were used to allow the observations to be interpreted in the context of their vertical distribution and to confirm the interpretation of atmospheric structure in the vicinity of the Cape Verde islands. Long-term ground-based measurements at the Cape Verde Atmospheric Observatory (CVAO) on São Vicente were supplemented by long-term measurements of reactive halogen species and characterisation of additional trace gas and aerosol species during the intensive experimental period. This paper presents a summary of the measurements made within the RHaMBLe remote experiments and discusses them in their meteorological and chemical context as determined from these three platforms and from additional meteorological analyses. Air always arrived at the CVAO from the North East with a range of air mass origins (European, Atlantic and North American continental). Trace gases were present at stable and fairly low concentrations with the exception of a slight increase in some anthropogenic components in air of North American origin, though NOx mixing ratios during this period remained below 20 pptv (note the non-IUPAC adoption in this manuscript of pptv and ppbv, equivalent to pmol mol−1 and nmol mol−1 to reflect common practice). Consistency with these air mass classifications is observed in the time series of soluble gas and aerosol composition measurements, with additional identification of periods of slightly elevated dust concentrations consistent with the trajectories passing over the African continent. The CVAO is shown to be broadly representative of the wider North Atlantic marine boundary layer; measurements of NO, O3 and black carbon from the ship are consistent with a clean Northern Hemisphere marine background. Aerosol composition measurements do not indicate elevated organic material associated with clean marine air. Closer to the African coast, black carbon and NO levels start to increase, indicating greater anthropogenic influence. Lower ozone in this region is possibly associated with the increased levels of measured halocarbons, associated with the nutrient rich waters of the Mauritanian upwelling. Bromide and chloride deficits in coarse mode aerosol at both the CVAO and on D319 and the continuous abundance of inorganic gaseous halogen species at CVAO indicate significant reactive cycling of halogens. Aircraft measurements of O3 and CO show that surface measurements are representative of the entire boundary layer in the vicinity both in diurnal variability and absolute levels. Above the inversion layer similar diurnal behaviour in O3 and CO is observed at lower mixing ratios in the air that had originated from south of Cape Verde, possibly from within the ITCZ. ECMWF calculations on two days indicate very different boundary layer depths and aircraft flights over the ship replicate this, giving confidence in the calculated boundary layer depth.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    DOI: 10.5194/acp-10-1031-2010
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2010
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  • 4
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    EUCAARI ion spectrometer measurements at 12 European sites – analysis of new particle formation events
    Copernicus GmbH ; 2010
    In:  Atmospheric Chemistry and Physics Vol. 10, No. 16 ( 2010-08-25), p. 7907-7927
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 10, No. 16 ( 2010-08-25), p. 7907-7927
    Abstract: Abstract. We present comprehensive results on continuous atmospheric cluster and particle measurements in the size range ~1–42 nm within the European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) project. We focused on characterizing the spatial and temporal variation of new particle formation events and relevant particle formation parameters across Europe. Different types of air ion and cluster mobility spectrometers were deployed at 12 field sites across Europe from March 2008 to May 2009. The measurements were conducted in a wide variety of environments, including coastal and continental locations as well as sites at different altitudes (both in the boundary layer and the free troposphere). New particle formation events were detected at all of the 12 field sites during the year-long measurement period. From the data, nucleation and growth rates of newly formed particles were determined for each environment. In a case of parallel ion and neutral cluster measurements, we could also estimate the relative contribution of ion-induced and neutral nucleation to the total particle formation. The formation rates of charged particles at 2 nm accounted for 1–30% of the corresponding total particle formation rates. As a significant new result, we found out that the total particle formation rate varied much more between the different sites than the formation rate of charged particles. This work presents, so far, the most comprehensive effort to experimentally characterize nucleation and growth of atmospheric molecular clusters and nanoparticles at ground-based observation sites on a continental scale.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    DOI: 10.5194/acp-10-7907-2010
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2010
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  • 5
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    ACTRIS ACSM intercomparison – Part 1: Reproducibility of concentration and fragment results from 13 individual Quadrupole Aerosol Chemical Speciation Monitors (Q-ACSM) and consistency with co-located instruments
    Copernicus GmbH ; 2015
    In:  Atmospheric Measurement Techniques Vol. 8, No. 12 ( 2015-12-02), p. 5063-5087
    Details
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 8, No. 12 ( 2015-12-02), p. 5063-5087
    Abstract: Abstract. As part of the European ACTRIS project, the first large Quadrupole Aerosol Chemical Speciation Monitor (Q-ACSM) intercomparison study was conducted in the region of Paris for 3 weeks during the late-fall – early-winter period (November–December 2013). The first week was dedicated to the tuning and calibration of each instrument, whereas the second and third were dedicated to side-by-side comparison in ambient conditions with co-located instruments providing independent information on submicron aerosol optical, physical, and chemical properties. Near real-time measurements of the major chemical species (organic matter, sulfate, nitrate, ammonium, and chloride) in the non-refractory submicron aerosols (NR-PM1) were obtained here from 13 Q-ACSM. The results show that these instruments can produce highly comparable and robust measurements of the NR-PM1 total mass and its major components. Taking the median of the 13 Q-ACSM as a reference for this study, strong correlations (r2 〉 0.9) were observed systematically for each individual Q-ACSM across all chemical families except for chloride for which three Q-ACSMs showing weak correlations partly due to the very low concentrations during the study. Reproducibility expanded uncertainties of Q-ACSM concentration measurements were determined using appropriate methodologies defined by the International Standard Organization (ISO 17025, 1999) and were found to be 9, 15, 19, 28, and 36 % for NR-PM1, nitrate, organic matter, sulfate, and ammonium, respectively. However, discrepancies were observed in the relative concentrations of the constituent mass fragments for each chemical component. In particular, significant differences were observed for the organic fragment at mass-to-charge ratio 44, which is a key parameter describing the oxidation state of organic aerosol. Following this first major intercomparison exercise of a large number of Q-ACSMs, detailed intercomparison results are presented, along with a discussion of some recommendations about best calibration practices, standardized data processing, and data treatment.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    URL: Article
    URL: Article
    DOI: 10.5194/amt-8-5063-2015
    DOI: 10.5194/amt-8-5063-2015-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2015
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  • 6
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    Formation of organic aerosol in the Paris region during the MEGAPOLI summer campaign: evaluation of the volatility-basis-set approach within the CHIMERE model
    Copernicus GmbH ; 2013
    In:  Atmospheric Chemistry and Physics Vol. 13, No. 11 ( 2013-06-14), p. 5767-5790
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 13, No. 11 ( 2013-06-14), p. 5767-5790
    Abstract: Abstract. Simulations with the chemistry transport model CHIMERE are compared to measurements performed during the MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) summer campaign in the Greater Paris region in July 2009. The volatility-basis-set approach (VBS) is implemented into this model, taking into account the volatility of primary organic aerosol (POA) and the chemical aging of semi-volatile organic species. Organic aerosol is the main focus and is simulated with three different configurations with a modified treatment of POA volatility and modified secondary organic aerosol (SOA) formation schemes. In addition, two types of emission inventories are used as model input in order to test the uncertainty related to the emissions. Predictions of basic meteorological parameters and primary and secondary pollutant concentrations are evaluated, and four pollution regimes are defined according to the air mass origin. Primary pollutants are generally overestimated, while ozone is consistent with observations. Sulfate is generally overestimated, while ammonium and nitrate levels are well simulated with the refined emission data set. As expected, the simulation with non-volatile POA and a single-step SOA formation mechanism largely overestimates POA and underestimates SOA. Simulation of organic aerosol with the VBS approach taking into account the aging of semi-volatile organic compounds (SVOC) shows the best correlation with measurements. High-concentration events observed mostly after long-range transport are well reproduced by the model. Depending on the emission inventory used, simulated POA levels are either reasonable or underestimated, while SOA levels tend to be overestimated. Several uncertainties related to the VBS scheme (POA volatility, SOA yields, the aging parameterization), to emission input data, and to simulated OH levels can be responsible for this behavior. Despite these uncertainties, the implementation of the VBS scheme into the CHIMERE model allowed for much more realistic organic aerosol simulations for Paris during summertime. The advection of SOA from outside Paris is mostly responsible for the highest OA concentration levels. During advection of polluted air masses from northeast (Benelux and Central Europe), simulations indicate high levels of both anthropogenic and biogenic SOA fractions, while biogenic SOA dominates during periods with advection from Southern France and Spain.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-13-5767-2013
    DOI: 10.5194/acp-13-5767-2013-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2013
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  • 7
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    A European aerosol phenomenology - 7: High-time resolution chemical characteristics of submicron particulate matter across Europe
    Elsevier BV ; 2021
    In:  Atmospheric Environment: X Vol. 10 ( 2021-04), p. 100108-
    Details
    In: Atmospheric Environment: X, Elsevier BV, Vol. 10 ( 2021-04), p. 100108-
    Type of Medium: Online Resource
    ISSN: 2590-1621
    URL: Article
    DOI: 10.1016/j.aeaoa.2021.100108
    Language: English
    Publisher: Elsevier BV
    Publication Date: 2021
    detail.hit.zdb_id: 2967860-2
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  • 8
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    In situ, satellite measurement and model evidence on the dominant regional contribution to fine particulate matter levels in the Paris megacity
    Copernicus GmbH ; 2015
    In:  Atmospheric Chemistry and Physics Vol. 15, No. 16 ( 2015-08-27), p. 9577-9591
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 15, No. 16 ( 2015-08-27), p. 9577-9591
    Abstract: Abstract. A detailed characterization of air quality in the megacity of Paris (France) during two 1-month intensive campaigns and from additional 1-year observations revealed that about 70 % of the urban background fine particulate matter (PM) is transported on average into the megacity from upwind regions. This dominant influence of regional sources was confirmed by in situ measurements during short intensive and longer-term campaigns, aerosol optical depth (AOD) measurements from ENVISAT, and modeling results from PMCAMx and CHIMERE chemistry transport models. While advection of sulfate is well documented for other megacities, there was surprisingly high contribution from long-range transport for both nitrate and organic aerosol. The origin of organic PM was investigated by comprehensive analysis of aerosol mass spectrometer (AMS), radiocarbon and tracer measurements during two intensive campaigns. Primary fossil fuel combustion emissions constituted less than 20 % in winter and 40 % in summer of carbonaceous fine PM, unexpectedly small for a megacity. Cooking activities and, during winter, residential wood burning are the major primary organic PM sources. This analysis suggests that the major part of secondary organic aerosol is of modern origin, i.e., from biogenic precursors and from wood burning. Black carbon concentrations are on the lower end of values encountered in megacities worldwide, but still represent an issue for air quality. These comparatively low air pollution levels are due to a combination of low emissions per inhabitant, flat terrain, and a meteorology that is in general not conducive to local pollution build-up. This revised picture of a megacity only being partially responsible for its own average and peak PM levels has important implications for air pollution regulation policies.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-15-9577-2015
    DOI: 10.5194/acp-15-9577-2015-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2015
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  • 9
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    Characterization and intercomparison of aerosol absorption photometers: result of two intercomparison workshops
    Copernicus GmbH ; 2011
    In:  Atmospheric Measurement Techniques Vol. 4, No. 2 ( 2011-02-10), p. 245-268
    Details
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 4, No. 2 ( 2011-02-10), p. 245-268
    Abstract: 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.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    URL: Article
    DOI: 10.5194/amt-4-245-2011
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2011
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  • 10
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    Aerosol decadal trends – Part 2: In-situ aerosol particle number concentrations at GAW and ACTRIS stations
    Copernicus GmbH ; 2013
    In:  Atmospheric Chemistry and Physics Vol. 13, No. 2 ( 2013-01-22), p. 895-916
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 13, No. 2 ( 2013-01-22), p. 895-916
    Abstract: 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.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-13-895-2013
    DOI: 10.5194/acp-13-895-2013-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2013
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