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  • 1
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    What can we learn about ship emission inventories from measurements of air pollutants over the Mediterranean Sea?
    Copernicus GmbH ; 2009
    In:  Atmospheric Chemistry and Physics Vol. 9, No. 18 ( 2009-09-18), p. 6815-6831
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 9, No. 18 ( 2009-09-18), p. 6815-6831
    Abstract: Abstract. Ship emission estimates diverge widely for all chemical compounds for several reasons: use of different methodologies (bottom-up or top-down), activity data and emission factors can easily result in a difference ranging from a factor of 1.5 to even an order of magnitude. Combining three sets of observational data – ozone and black carbon measurements sampled at three coastal sites and on board of a Mediterranean cruise ship, as well as satellite observations of atmospheric NO2 column concentration over the same area – we assess the accuracy of the three most commonly used ship emission inventories, EDGAR FT (Olivier et al., 2005), emissions described by Eyring et al. (2005) and emissions reported by EMEP (Vestreng et al., 2007). Our tool is a global atmospheric chemistry transport model which simulates the chemical state of the Mediterranean atmosphere applying different ship emission inventories. The simulated contributions of ships to air pollutant levels in the Mediterranean atmosphere are significant but strongly depend on the inventory applied. Close to the major shipping routes relative contributions vary from 10 to 50% for black carbon and from 2 to 12% for ozone in the surface layer, as well as from 5 to 20% for nitrogen dioxide atmospheric column burden. The relative contributions are still significant over the North African coast, but less so over the South European coast because densely populated regions with significant human activity contribute relatively more to air pollution than ships, even if these regions attract a lot of ship traffic. The observations poorly constrain the ship emission inventories in the Eastern Mediterranean where the influence of uncertain land based emissions, the model transport and wet deposition are at least as important as the signal from ships. In the Western Mediterranean, the regional EMEP emission inventory gives the best match with most measurements, followed by Eyring for NO2 and ozone and by EDGAR for black carbon. Given the uncertainty of the measurements and the model, each of the three emission inventories could actually be right, implying that large uncertainties in ship emissions need to be considered for future scenario analysis.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    DOI: 10.5194/acp-9-6815-2009
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2009
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  • 2
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    Ozone over the Western Mediterranean Sea – results from two years of shipborne measurements
    Copernicus GmbH ; 2011
    In:  Atmospheric Chemistry and Physics Vol. 11, No. 2 ( 2011-01-24), p. 675-688
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 11, No. 2 ( 2011-01-24), p. 675-688
    Abstract: Abstract. Ozone, along with other air pollutants, has been measured for two years from a monitoring station placed on a cruise ship that follows a regular track in the Western Mediterranean between April and October. Conditions favouring high ozone levels have been studied by analysis of weather maps and back trajectories. This analysis was focused on a transect over the open sea in the South Western Mediterranean between Tunis and Palma de Mallorca. High ozone levels were found in situations with an anticyclonic circulation over the Western Mediterranean when subsidence brings air masses down from altitudes between 1000 and 3500 m a.s.l. Analysis of composite meteorological maps suggests a relevant contribution of breeze circulation to subsidence during events with high surface ozone concentrations; this points to an important contribution from local ozone formation. A detailed back trajectory analysis of the origin of air masses with high ozone concentrations was carried out for two "hot spots" for ozone pollution, in the Gulf of Genoa and between Naples and Palermo, respectively. The main cause of high ozone levels in the Gulf of Genoa was found to be outflow from the Po Valley and the Genoa area while such episodes along the Naples-Palermo transect were most often associated with trajectories from the Rome or Naples areas. Analysis of the relationship between measured concentrations of Black Carbon and ozone allowed to evaluate the degree of photochemical "ageing" of the air masses encountered along the route of the cruise ship.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    DOI: 10.5194/acp-11-675-2011
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2011
    detail.hit.zdb_id: 2092549-9
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  • 3
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    Better constraints on sources of carbonaceous aerosols using a combined 〈sup〉14〈/sup〉C – macro tracer analysis in a European rural background site
    Copernicus GmbH ; 2011
    In:  Atmospheric Chemistry and Physics Vol. 11, No. 12 ( 2011-06-20), p. 5685-5700
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 11, No. 12 ( 2011-06-20), p. 5685-5700
    Abstract: Abstract. The source contributions to carbonaceous PM2.5 aerosol were investigated at a European background site at the edge of the Po Valley, in Northern Italy, during the period January–December 2007. Carbonaceous aerosol was described as the sum of 8 source components: primary (1) and secondary (2) biomass burning organic carbon, biomass burning elemental carbon (3), primary (4) and secondary (5) fossil organic carbon, fossil fuel burning elemental carbon (6), primary (7) and secondary (8) biogenic organic carbon. The mass concentration of each component was quantified using a set of macro tracers (organic carbon OC, elemental carbon EC, and levoglucosan), micro tracers (arabitol and mannitol), and 14C measurements. This was the first time that 14C measurements covered a full annual cycle with daily resolution. This set of 6 tracers, together with assumed uncertainty ranges of the ratios of OC-to-EC, and the reference fraction of modern carbon in the 8 source categories, provides strong constraints to the source contributions to carbonaceous aerosol. The uncertainty of contributions was assessed with a Quasi-Monte Carlo (QMC) method accounting for the variability of OC and EC emission factors, the uncertainty of reference fractions of modern carbon, and the measurement uncertainty. During winter, biomass burning composed 64 % (±15 %) of the total carbon (TC) concentration, while in summer secondary biogenic OC accounted for 50 % (±16 %) of TC. The contribution of primary biogenic aerosol particles was negligible during the entire year. Moreover, aerosol associated with fossil sources represented 27 % (±16 %) and 41 % (±26 %) of TC in winter and summer, respectively. The contribution of secondary organic aerosol (SOA) to the organic mass (OM) was significant during the entire year. SOA accounted for 30 % (±16 %) and 85 % (±12 %) of OM during winter and summer, respectively. While the summer SOA was dominated by biogenic sources, winter SOA was mainly due to biomass burning and fossil sources. This indicates that the oxidation of semi-volatile and intermediate volatility organic compounds co-emitted with primary organics is a significant source of SOA, as suggested by recent model results and Aerosol Mass Spectrometer measurements. Comparison with previous global model simulations, indicates a strong underestimate of wintertime primary aerosol emissions in this region. The comparison of source apportionment results in different urban and rural areas showed that the sampling site was mainly affected by local aerosol sources during winter and regional air masses from the nearby Po Valley in summer. This observation was further confirmed by back-trajectory analysis applying the Potential Source Contribution Function method to identify potential source regions.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    DOI: 10.5194/acp-11-5685-2011
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2011
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  • 4
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    North Atlantic Oscillation and tropospheric ozone variability in Europe: model analysis and measurements intercomparison
    Copernicus GmbH ; 2012
    In:  Atmospheric Chemistry and Physics Vol. 12, No. 14 ( 2012-07-23), p. 6357-6376
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 12, No. 14 ( 2012-07-23), p. 6357-6376
    Abstract: Abstract. Ozone pollution represents a serious health and environmental problem. While ozone pollution is mostly produced by photochemistry in summer, elevated ozone concentrations can also be influenced by long range transport driven by the atmospheric circulation and stratospheric ozone intrusions. We analyze the role of large scale atmospheric circulation variability in the North Atlantic basin in determining surface ozone concentrations over Europe. Here, we show, using ground station measurements and a coupled atmosphere-chemistry model simulation for the period 1980–2005, that the North Atlantic Oscillation (NAO) does affect surface ozone concentrations – on a monthly timescale, over 10 ppbv in southwestern, central and northern Europe – during all seasons except fall. The commonly used NAO index is able to capture the link existing between atmospheric dynamics and surface ozone concentrations in winter and spring but it fails in summer. We find that the first Principal Component, computed from the time variation of the sea level pressure (SLP) field, detects the atmosphere circulation/ozone relationship not only in winter and spring but also during summer, when the atmospheric circulation weakens and regional photochemical processes peak. Given the NAO forecasting skill at intraseasonal time scale, the first Principal Component of the SLP field could be used as an indicator to identify areas more exposed to forthcoming ozone pollution events. Finally, our results suggest that the increasing baseline ozone in western and northern Europe during the 1990s could be related to the prevailing positive phase of the NAO in that period.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    DOI: 10.5194/acp-12-6357-2012
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2012
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  • 5
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    Global scale emission and distribution of sea-spray aerosol: Sea-salt and organic enrichment
    Elsevier BV ; 2010
    In:  Atmospheric Environment Vol. 44, No. 5 ( 2010-02), p. 670-677
    Details
    In: Atmospheric Environment, Elsevier BV, Vol. 44, No. 5 ( 2010-02), p. 670-677
    Type of Medium: Online Resource
    ISSN: 1352-2310
    URL: Article
    DOI: 10.1016/j.atmosenv.2009.11.013
    Language: English
    Publisher: Elsevier BV
    Publication Date: 2010
    detail.hit.zdb_id: 216368-8
    detail.hit.zdb_id: 1499889-0
    SSG: 14
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  • 6
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    The sensitivity of aerosol in Europe to two different emission inventories and temporal distribution of emissions
    Copernicus GmbH ; 2006
    In:  Atmospheric Chemistry and Physics Vol. 6, No. 12 ( 2006-09-25), p. 4287-4309
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 6, No. 12 ( 2006-09-25), p. 4287-4309
    Abstract: Abstract. The sensitivity to two different emission inventories, injection altitude and temporal variations of anthropogenic emissions in aerosol modelling is studied, using the two way nested global transport chemistry model TM5 focussing on Europe in June and December 2000. The simulations of gas and aerosol concentrations and aerosol optical depth (AOD) with the EMEP and AEROCOM emission inventories are compared with EMEP gas and aerosol surface based measurements, AERONET sun photometers retrievals and MODIS satellite data. For the aerosol precursor gases SO2 and NOx in both months the model results calculated with the EMEP inventory agree better (overestimated by a factor 1.3 for both SO2 and NOx) with the EMEP measurements than the simulation with the AEROCOM inventory (overestimated by a factor 2.4 and 1.9, respectively). Besides the differences in total emissions between the two inventories, an important role is also played by the vertical distribution of SO2 and NOx emissions in understanding the differences between the EMEP and AEROCOM inventories. In December NOx and SO2 from both simulations agree within 50% with observations. In June SO4= evaluated with the EMEP emission inventory agrees slightly better with surface observations than the AEROCOM simulation, whereas in December the use of both inventories results in an underestimate of SO4 with a factor 2. Nitrate aerosol measured in summer is not reliable, however in December nitrate aerosol calculations with the EMEP and AEROCOM emissions agree with 30%, and 60%, respectively with the filter measurements. Differences are caused by the total emissions and the temporal distribution of the aerosol precursor gases NOx and NH3. Despite these differences, we show that the column integrated AOD is less sensitive to the underlying emission inventories. Calculated AOD values with both emission inventories underestimate the observed AERONET AOD values by 20–30%, whereas a case study using MODIS data shows a high spatial agreement. Our evaluation of the role of temporal distribution of anthropogenic emissions on aerosol calculations shows that the daily and weekly temporal distributions of the emissions are only important for NOx, NH3 and aerosol nitrate. However, for all aerosol species SO4=, NH4+, POM, BC, as well as for AOD, the seasonal temporal variations used in the emission inventory are important. Our study shows the value of including at least seasonal information on anthropogenic emissions, although from a comparison with a range of measurements it is often difficult to firmly identify the superiority of specific emission inventories, since other modelling uncertainties, e.g. related to transport, aerosol removal, water uptake, and model resolution, play a dominant role.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-6-4287-2006
    DOI: 10.5194/acp-6-4287-2006-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2006
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  • 7
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    The European aerosol budget in 2006
    Copernicus GmbH ; 2011
    In:  Atmospheric Chemistry and Physics Vol. 11, No. 3 ( 2011-02-09), p. 1117-1139
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 11, No. 3 ( 2011-02-09), p. 1117-1139
    Abstract: Abstract. This paper presents the aerosol budget over Europe in 2006 calculated with the global transport model TM5 coupled to the size-resolved aerosol module M7. Comparison with ground observations indicates that the model reproduces the observed concentrations quite well with an expected slight underestimation of PM10 due to missing emissions (e.g. resuspension). We model that a little less than half of the anthropogenic aerosols emitted in Europe are exported and the rest is removed by deposition. The anthropogenic aerosols are removed mostly by rain (95%) and only 5% is removed by dry deposition. For the larger natural aerosols, especially sea salt, a larger fraction is removed by dry processes (sea salt: 70%, mineral dust: 35%). We model transport of aerosols in the jet stream in the higher atmosphere and an import of Sahara dust from the south at high altitudes. Comparison with optical measurements shows that the model reproduces the Ångström parameter very well, which indicates a correct simulation of the aerosol size distribution. However, we underestimate the aerosol optical depth. Because the surface concentrations are close to the observations, the shortage of aerosol in the model is probably at higher altitudes. We show that the discrepancies are mainly caused by an overestimation of wet-removal rates. To match the observations, the wet-removal rates have to be scaled down by a factor of about 5. In that case the modelled ground-level concentrations of sulphate and sea salt increase by 50% (which deteriorates the match), while other components stay roughly the same. Finally, it is shown that in particular events, improved fire emission estimates may significantly improve the ability of the model to simulate the aerosol optical depth. We stress that discrepancies in aerosol models can be adequately analysed if all models would provide (regional) aerosol budgets, as presented in the current study.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    DOI: 10.5194/acp-11-1117-2011
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2011
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  • 8
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    Re-analysis of tropospheric sulfate aerosol and ozone for the period 1980–2005 using the aerosol-chemistry-climate model ECHAM5-HAMMOZ
    Copernicus GmbH ; 2011
    In:  Atmospheric Chemistry and Physics Vol. 11, No. 18 ( 2011-09-16), p. 9563-9594
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 11, No. 18 ( 2011-09-16), p. 9563-9594
    Abstract: Abstract. Understanding historical trends of trace gas and aerosol distributions in the troposphere is essential to evaluate the efficiency of existing strategies to reduce air pollution and to design more efficient future air quality and climate policies. We performed coupled photochemistry and aerosol microphysics simulations for the period 1980–2005 using the aerosol-chemistry-climate model ECHAM5-HAMMOZ, to assess our understanding of long-term changes and inter-annual variability of the chemical composition of the troposphere, and in particular of ozone and sulfate concentrations, for which long-term surface observations are available. In order to separate the impact of the anthropogenic emissions and natural variability on atmospheric chemistry, we compare two model experiments, driven by the same ECMWF re-analysis data, but with varying and constant anthropogenic emissions, respectively. Our model analysis indicates an increase of ca. 1 ppbv (0.055 ± 0.002 ppbv yr−1) in global average surface O3 concentrations due to anthropogenic emissions, but this trend is largely masked by the larger O3 anomalies due to the variability of meteorology and natural emissions. The changes in meteorology (not including stratospheric variations) and natural emissions account for the 75 % of the total variability of global average surface O3 concentrations. Regionally, annual mean surface O3 concentrations increased by 1.3 and 1.6 ppbv over Europe and North America, respectively, despite the large anthropogenic emission reductions between 1980 and 2005. A comparison of winter and summer O3 trends with measurements shows a qualitative agreement, except in North America, where our model erroneously computed a positive trend. Simulated O3 increases of more than 4 ppbv in East Asia and 5 ppbv in South Asia can not be corroborated with long-term observations. Global average sulfate surface concentrations are largely controlled by anthropogenic emissions. Globally natural emissions are an important driver determining AOD variations. Regionally, AOD decreased by 28 % over Europe, while it increased by 19 % and 26 % in East and South Asia. The global radiative perturbation calculated in our model for the period 1980–2005 was rather small (0.05 W m−2 for O3 and 0.02 W m−2 for total aerosol direct effect), but larger perturbations ranging from −0.54 to 1.26 W m−2 are estimated in those regions where anthropogenic emissions largely varied.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    DOI: 10.5194/acp-11-9563-2011
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2011
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  • 9
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    Formation of secondary organic aerosol from isoprene oxidation over Europe
    Copernicus GmbH ; 2009
    In:  Atmospheric Chemistry and Physics Vol. 9, No. 18 ( 2009-09-22), p. 7003-7030
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 9, No. 18 ( 2009-09-22), p. 7003-7030
    Abstract: Abstract. The role of isoprene as a precursor to secondary organic aerosol (SOA) over Europe is studied with the two-way nested global chemistry transport model TM5. The inclusion of the formation of SOA from isoprene oxidation in our model almost doubles the atmospheric burden of SOA over Europe compared to SOA formation from terpenes and aromatics. The reference simulation, which considers SOA formation from isoprene, terpenes and aromatics, predicts a yearly European production rate of 1.0 Tg SOA yr−1 and an annual averaged atmospheric burden of about 50 Gg SOA over Europe. A fraction of 35% of the SOA produced in the boundary layer over Europe is transported to higher altitudes or to other world regions. Summertime measurements of organic matter (OM) during the extensive EMEP OC/EC campaign 2002/2003 are better reproduced when SOA formation from isoprene is taken into account, reflecting also the strong seasonality of isoprene and other biogenic volatile organic compounds (BVOC) emissions from vegetation. However, during winter, our model strongly underestimates OM, likely caused by missing wood burning in the emission inventories. Uncertainties in the parameterisation of isoprene SOA formation have been investigated. Maximum SOA production is found for irreversible sticking (non-equilibrium partitioning) of condensable vapours on particles, with tropospheric SOA production over Europe increased by a factor of 4 in summer compared to the reference case. Completely neglecting SOA formation from isoprene results in the lowest estimate (0.51 Tg SOA yr−1). The amount and the nature of the absorbing matter are shown to be another key uncertainty when predicting SOA levels. Consequently, smog chamber experiments on SOA formation should be performed with different types of seed aerosols and without seed aerosols in order to derive an improved treatment of the absorption of SOA in the models. Consideration of a number of recent insights in isoprene SOA formation mechanisms reduces the tropospheric production of isoprene derived SOA over Europe from 0.4 Tg yr−1 in our reference simulation to 0.1 Tg yr−1.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-9-7003-2009
    DOI: 10.5194/acp-9-7003-2009-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2009
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  • 10
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    Online Resource
    Organic aerosol and global climate modelling: a review
    Copernicus GmbH ; 2005
    In:  Atmospheric Chemistry and Physics Vol. 5, No. 4 ( 2005-03-30), p. 1053-1123
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 5, No. 4 ( 2005-03-30), p. 1053-1123
    Abstract: Abstract. The present paper reviews existing knowledge with regard to Organic Aerosol (OA) of importance for global climate modelling and defines critical gaps needed to reduce the involved uncertainties. All pieces required for the representation of OA in a global climate model are sketched out with special attention to Secondary Organic Aerosol (SOA): The emission estimates of primary carbonaceous particles and SOA precursor gases are summarized. The up-to-date understanding of the chemical formation and transformation of condensable organic material is outlined. Knowledge on the hygroscopicity of OA and measurements of optical properties of the organic aerosol constituents are summarized. The mechanisms of interactions of OA with clouds and dry and wet removal processes parameterisations in global models are outlined. This information is synthesized to provide a continuous analysis of the flow from the emitted material to the atmosphere up to the point of the climate impact of the produced organic aerosol. The sources of uncertainties at each step of this process are highlighted as areas that require further studies.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    DOI: 10.5194/acp-5-1053-2005
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2005
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