ALBERT

Description: The second generation Collection 005 (C005) MODIS operational algorithm for retrieval of aerosol properties was evaluated and validated for the greater Mediterranean basin (29.5° N–46.5° N and 10.5° W–38.5° E), a region with an atmosphere under siege by air pollution and diminishing water resources that are exacerbated by high aerosol loads and climatic change. The present study aims to quantify the differences between the C005 and the previous (C004) MODIS collections, and re-assess the results of previous studies that have been performed for the region using MODIS C004 aerosol optical depth (AOD) products. Daily data of AOD from EOS-Terra covering the 6-year period 2000–2006 were taken from both C005 and C004 Level-3 datasets, and were inter-compared and validated against ground-based measurements from 29 AERONET stations. The C005 data were found to significantly better agree with the AERONET data than those of C004. The correlation coefficient between MODIS and AERONET was found to increase from 0.66 to 0.76 and the slope of linear regression MODIS/AERONET from 0.79 to 0.85. The MODIS C005 data still overestimate/underestimate the AERONET AOD values smaller/larger than 0.25, but to a much smaller extent than C004 data. The better agreement of C005 with AERONET data arises from the generally lower C005 values, with regional mean AOD values equal to 0.27 and 0.22 for C004 and C005, respectively. This decrease, however, is not uniform over the region and involves a significant decrease over land and a small increase over the ocean for AOD values greater than 0.1 (opposite changes were found under aerosol-clean conditions). Both data sets indicate a decrease in the regional mean AOD over the period 2000–2006, equal to 20% based on C005 and 17% based on C004 datasets, though the intra-annual and inter-annual variation did not change significantly, thus indicating a systematic correction to C004 values.

Description: Glyoxal, the smallest dicarbonyl, which has recently been observed from space, is expected to provide indications on VOC oxidation and secondary aerosol formation in the troposphere. Glyoxal is known to be mostly of natural origin and is produced during biogenic VOC oxidation. However, a number of anthropogenically emitted hydrocarbons, like acetylene and aromatics, have been positively identified as glyoxal precursors. The present study investigates the contribution of pollution emissions to the glyoxal levels by taking into account only the secondary chemical formation of glyoxal from precursors emitted from biogenic, anthropogenic and biomass burning sources. For this purpose, a global 3-dimensional chemistry transport model of the troposphere (TM4) able to simulate the gas phase chemistry coupled with all major aerosol components is used. The model results are compared with satellite observations of glyoxal columns over hot spot areas. According to TM4 model results, the anthropogenic contribution to the glyoxal columns is found to reach 70% in the industrialized areas of the northern hemisphere and up to 20% in the tropics. It is on average three times larger than the secondary production of glyoxal from biomass burning sources. The chemical production of glyoxal is calculated to equal about 56 Tg y−1 with 70% produced from biogenic hydrocarbons oxidation, 17% from acetylene, 11% from aromatic chemistry, and 2% from ethene and propene. Glyoxal is destroyed by reactions mainly with OH radicals (22%) and by photolysis (65%), but it is also removed from the atmosphere through wet (11%) and dry deposition (6%). Secondary organic aerosol potential formation through glyoxal losses on/in aerosols and clouds was neglected here due to the significant uncertainties associated with the underlying chemistry. The global annual mean glyoxal burden and lifetime in the model domain are estimated at 0.02 Tg and 3 h, respectively.

Description: In spite of impressive advances in recent years, our present understanding of organic aerosol (OA) composition, physical and chemical properties, sources and transformation characteristics is still rather limited, and their environmental effects remain highly uncertain. This paper discusses and prioritizes issues related to organic aerosols and their effects on atmospheric processes and climate, providing a basis for future activities in the field. Four main topical areas are addressed: i) sources of OA; ii) formation transformation and removal of OA; iii) physical, chemical and mixing state of OA; iv) atmospheric modelling of OA. Key questions and research priorities regarding these four areas are synthesized in this paper, and outstanding issues for future research are presented for each topical area. In addition, an effort is made to formulate a basic set of consistent and universally applicable terms and definitions for coherent description of atmospheric OA across different scales and disciplines.

Description: A global 3-dimensional chemistry/transport model able to describe O3, NOx, Volatile Organic Compounds (VOC), sulphur and NH3 chemistry has been extended to simulate the temporal and spatial distribution of primary and secondary carbonaceous aerosols in the troposphere focusing on Secondary Organic Aerosol (SOA) formation. A number of global simulations have been performed to determine a possible range of annual global SOA production and investigate uncertainties associated with the model results. The studied uncertainties in the SOA budget have been evaluated to be in decreasing importance: the potentially irreversible sticking of the semi-volatile compounds on aerosols, the enthalpy of vaporization of these compounds, the partitioning of SOA on non-carbonaceous aerosols, the conversion of aerosols from hydrophobic to hydrophilic, the emissions of primary carbonaceous aerosols, the chemical fate of the first generation products and finally the activity coefficient of the condensable species. The large uncertainties associated with the emissions of VOC and the adopted simplification of chemistry have not been investigated in this study. Although not all sources of uncertainties have been investigated, according to our calculations, the above factors within the experimental range of variations could result to an overall uncertainty of about a factor of 20 in the global SOA budget. The global annual SOA production from biogenic VOC might range from 2.5 to 44.5 Tg of organic matter per year, whereas that from anthropogenic VOC ranges from 0.05 to 2.62 Tg of organic matter per year. These estimates can be considered as a lower limit, since partitioning on coarse particles like nitrate, dust or sea-salt, together with the partitioning and the dissociation of the semi-volatile products in aerosol water has been neglected. Comparison of model results to observations, where available, shows a better agreement for the upper budget estimates than for the lower ones.

Description: In order to investigate the variability of the secondary organic aerosol (SOA) distributions and budget and provide a measure for the robustness of the conclusions on human induced changes of SOA, a global 3-dimensional chemistry transport model describing both the gas and the particulate phase chemistry of the troposphere has been applied. The response of the global budget of SOA to temperature and moisture changes as well as to biogenic emission changes over a decade (1984-1993) has been evaluated. The considered emissions of biogenic non-methane volatile organic compounds (VOC) are driven by temperature, light and vegetation. They vary between 756 and 810 Tg Cy-1 and are therefore about 5.5 times higher than the anthropogenic VOC emissions. All secondary aerosols (sulphuric, nitrates and organics) are computed on-line together with the aerosol associated water. Over the studied decade, the computed natural variations (8%) in the chemical SOA production from biogenic VOC oxidation equal the chemical SOA production from anthropogenic VOC oxidation. Maximum values are calculated for 1990 (warmer and drier) and minimum values for 1986 (colder and wetter). The SOA computed variability results from a 7% increase in biogenic VOC emissions from 1986 to 1990 combined with 8.5% and 6% increases in the wet and dry deposition of SOA and leads to about 11.5% increase in the SOA burden of biogenic origin. The present study also demonstrates the importance of the hydrological cycle in determining the built up and fate of SOA in the atmosphere. It also reveals the existence of significant positive and negative feedback mechanisms in the atmosphere responsible for the non linear relationship between emissions of biogenic VOC and SOA burden.

Description: 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.

Description: During the MINOS campaign (28 July-18 August 2001) the nitrate (NO3) radical was measured at Finokalia station, on the north coast of Crete in South-East Europe using a long path (10.4 km) Differential Optical Absorption Spectroscopy instrument (DOAS). Hydroxyl (OH) radical was also measured by a Chemical Ionization Mass-Spectrometer (Berresheim et al., 2003). These datasets represent the first simultaneous measurements of OH and NO3 radicals in the area. NO3 radical concentrations ranged from less than 3x107 up to 9x108 radicals· cm-3 with an average nighttime value of 1.1x108 radicals· cm-3. The observed NO3 mixing ratios are analyzed on the basis of the corresponding meteorological data and the volatile organic compound (VOC) observations which were measured simultaneously at Finokalia station. The importance of the NO3 radical chemistry relatively to that of OH in the dimethylsulfide (DMS) and nitrate cycles is also investigated. The observed NO3 levels regulate the nighttime variation of DMS. The loss of DMS by NO3 during night is about 75% of that by OH radical during day. NO3 and nitrogen pentoxide (N2O5) reactions account for about 21% of the total nitrate (HNO3(g)+NO-3(g)) production.

Description: This is the first study that investigates the seasonal variability of nitrate (NO3) radicals in the marine boundary layer over the East Mediterranean Sea. An extensive data set of NO3 radical observations on the north coast of Crete for more than two years (June 2001–September 2003) is presented here. NO3 radicals follow a distinct seasonal dependency with the highest seasonally average mixing ratios in summer (5.6±1.2 pptv) and the lowest in winter (1.2±1.2 pptv). Episodes with high NO3 mixing ratios have been encountered mainly in polluted air masses originating from mainland Greece, Central and East Europe, and Turkey. Ancillary measurements of ozone, nitrogen dioxide (NO2) and meteorological parameters have been conducted and used to reveal possible relationship with the observed NO3 variability. The acquired NO2 nighttime observations provide the up-to-date most complete overview of NO2 temporal variability in the area. The data show correlations of the NO3 nighttime mixing ratios with temperature (positive), relative humidity (negative) and to a lesser extend with O3 (positive). As inferred from these observations, on average the major sink of NO3 radicals in the area is the heterogeneous reaction of dinitrogen pentoxide (N2O5) on aqueous particles whereas the homogeneous gas phase reactions of NO3 are most important during spring and summer. These observations support a significant contribution of NO3 nighttime chemistry to the oxidizing capacity of the troposphere.

Description: 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.

Description: Megacities are large urban agglomerations with intensive anthropogenic emissions that have significant impacts on local and regional air quality. In the present mesoscale modeling study, the impacts of anthropogenic emissions from the Greater Istanbul Area (GIA) and the Greater Athens Area (GAA) on the air quality in GIA, GAA and the entire East Mediterranean are quantified for typical wintertime (December 2008) and summertime (July 2008) conditions. They are compared to those of the regional anthropogenic and biogenic emissions that are also calculated. Finally, the efficiency of potential country-based emissions mitigation in improving air quality is investigated. The results show that relative contributions from both cities to surface ozone (O3) and aerosol levels in the cities' extended areas are generally higher in winter than in summer. Anthropogenic emissions from GIA depress surface O3 in the GIA by ~ 60% in winter and ~ 20% in summer while those from GAA reduce the surface O3 in the GAA by 30% in winter and by 8% in summer. GIA and GAA anthropogenic emissions contribute to the fine particulate matter (PM2.5) levels inside the cities themselves by up to 75% in winter and by 50% (GIA) and ~ 40% (GAA), in summer. GIA anthropogenic emissions have larger impacts on the domain-mean surface O3 (up to 1%) and PM2.5 (4%) levels compared to GAA anthropogenic emissions (