ALBERT

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 (

Description: This paper evaluates the current status of global modeling of the organic aerosol (OA) in the troposphere and analyzes the differences between models as well as between models and observations. Thirty-one global chemistry transport models (CTMs) and general circulation models (GCMs) have participated in this intercomparison, in the framework of AeroCom phase II. The simulation of OA varies greatly between models in terms of the magnitude of primary emissions, secondary OA (SOA) formation, the number of OA species used (2 to 62), the complexity of OA parameterizations (gas-particle partitioning, chemical aging, multiphase chemistry, aerosol microphysics), and the OA physical, chemical and optical properties. The diversity of the global OA simulation results has increased since earlier AeroCom experiments, mainly due to the increasing complexity of the SOA parameterization in models, and the implementation of new, highly uncertain, OA sources. Diversity of over one order of magnitude exists in the modeled vertical distribution of OA concentrations that deserves a dedicated future study. Furthermore, although the OA / OC ratio depends on OA sources and atmospheric processing, and is important for model evaluation against OA and OC observations, it is resolved only by a few global models. The median global primary OA (POA) source strength is 56 Tg a−1 (range 34–144 Tg a−1) and the median SOA source strength (natural and anthropogenic) is 19 Tg a−1 (range 13–121 Tg a−1). Among the models that take into account the semi-volatile SOA nature, the median source is calculated to be 51 Tg a−1 (range 16–121 Tg a−1), much larger than the median value of the models that calculate SOA in a more simplistic way (19 Tg a−1; range 13–20 Tg a−1, with one model at 37 Tg a−1). The median atmospheric burden of OA is 1.4 Tg (24 models in the range of 0.6–2.0 Tg and 4 between 2.0 and 3.8 Tg), with a median OA lifetime of 5.4 days (range 3.8–9.6 days). In models that reported both OA and sulfate burdens, the median value of the OA/sulfate burden ratio is calculated to be 0.77; 13 models calculate a ratio lower than 1, and 9 models higher than 1. For 26 models that reported OA deposition fluxes, the median wet removal is 70 Tg a−1 (range 28–209 Tg a−1), which is on average 85% of the total OA deposition. Fine aerosol organic carbon (OC) and OA observations from continuous monitoring networks and individual field campaigns have been used for model evaluation. At urban locations, the model–observation comparison indicates missing knowledge on anthropogenic OA sources, both strength and seasonality. The combined model–measurements analysis suggests the existence of increased OA levels during summer due to biogenic SOA formation over large areas of the USA that can be of the same order of magnitude as the POA, even at urban locations, and contribute to the measured urban seasonal pattern. Global models are able to simulate the high secondary character of OA observed in the atmosphere as a result of SOA formation and POA aging, although the amount of OA present in the atmosphere remains largely underestimated, with a mean normalized bias (MNB) equal to −0.62 (−0.51) based on the comparison against OC (OA) urban data of all models at the surface, −0.15 (+0.51) when compared with remote measurements, and −0.30 for marine locations with OC data. The mean temporal correlations across all stations are low when compared with OC (OA) measurements: 0.47 (0.52) for urban stations, 0.39 (0.37) for remote stations, and 0.25 for marine stations with OC data. The combination of high (negative) MNB and higher correlation at urban stations when compared with the low MNB and lower correlation at remote sites suggests that knowledge about the processes that govern aerosol processing, transport and removal, on top of their sources, is important at the remote stations. There is no clear change in model skill with increasing model complexity with regard to OC or OA mass concentration. However, the complexity is needed in models in order to distinguish between anthropogenic and natural OA as needed for climate mitigation, and to calculate the impact of OA on climate accurately.

Description: We model the Penman potential evaporation (PE) over all land areas of the globe for the 25-yr period 1983–2008, relying on radiation transfer models (RTMs) for the shortwave and longwave fluxes. Penman's PE is determined by two factors: available energy for evaporation and ground to atmosphere vapour transfer. Input to the PE model and RTMs comprises satellite cloud and aerosol data, as well as data from reanalyses. PE is closely linked to pan evaporation, whose trends have sparked controversy in the community, since the factors responsible for the observed pan evaporation trends are not determined with consensus. Our particular interest is the temporal evolution of PE, and the provided insight to the observed trends of pan evaporation. We examine the decadal trends of PE and various related physical quantities, such as net solar flux, net longwave flux, water vapour saturation deficit and wind speed. Our findings are the following: Global warming has led to a larger water vapour saturation deficit. The periods 1983–1989, 1990–1999, and 2000–2008 were characterised by decreasing, increasing, and slightly decreasing PE, respectively. In these last 25 yr, global dimming/brightening cycles generally increased the available energy for evaporation. PE trends seem to follow more closely the trends of energy availability than the trends of the atmospheric capability for vapour transfer, at most locations on the globe, with trends in the Northern hemisphere significantly larger than in the Southern. These results support the hypothesis that global potential evaporation trends are attributed primarily to secular changes in the radiation fluxes, and secondarily to vapour transfer considerations.

Description: Changes in temperature due to variability in meteorology and climate change are expected to significantly impact atmospheric composition. The Mediterranean is a climate sensitive region and includes megacities like Istanbul and large urban agglomerations such as Athens. The effect of temperature changes on gaseous air pollutant levels and the atmospheric processes that are controlling them in the Eastern Mediterranean are here investigated. The WRF/CMAQ mesoscale modeling system is used, coupled with the MEGAN model for the processing of biogenic volatile organic compound emissions. A set of temperature perturbations (spanning from 1 to 5 K) is applied on a base case simulation corresponding to July 2004. The results indicate that the Eastern Mediterranean basin acts as a reservoir of pollutants and their precursor emissions from large urban agglomerations. During summer, chemistry is a major sink at these urban areas near the surface, and a minor contributor at downwind areas. On average, the atmospheric processes are more effective within the first 1000 m above ground. Temperature increases lead to increases in biogenic emissions by 9±3% K−1. Ozone mixing ratios increase almost linearly with the increases in ambient temperatures by 1±0.1 ppb O3 K−1 for all studied urban and receptor stations except for Istanbul, where a 0.4±0.1 ppb O3 K−1 increase is calculated, which is about half of the domain-averaged increase of 0.9±0.1 ppb O3 K−1. The computed changes in atmospheric processes are also linearly related with temperature changes.

Description: Organic acids attract increasing attention as contributors to atmospheric acidity, secondary organic aerosol mass and aerosol hygroscopicity. Oxalic acid is globally the most abundant dicarboxylic acid, formed via chemical oxidation of gas-phase precursors in the aqueous phase of aerosols and droplets. Its lifecycle and atmospheric global distribution remain highly uncertain and are the focus of this study. The first global spatial and temporal distribution of oxalate, simulated using a state-of-the-art aqueous-phase chemical scheme embedded within the global 3-dimensional chemistry/transport model TM4-ECPL, is here presented. The model accounts for comprehensive gas-phase chemistry and its coupling with major aerosol constituents (including secondary organic aerosol). Model results are consistent with ambient observations of oxalate at rural and remote locations (slope = 1.16 ± 0.14, r2 = 0.36, N = 114) and suggest that aqueous-phase chemistry contributes significantly to the global atmospheric burden of secondary organic aerosol. In TM4-ECPL most oxalate is formed in-cloud and less than 5 % is produced in aerosol water. About 62 % of the oxalate is removed via wet deposition, 30 % by in-cloud reaction with hydroxyl radical, 4 % by in-cloud reaction with nitrate radical and 4 % by dry deposition. The in-cloud global oxalate net chemical production is calculated to be about 21–37 Tg yr−1 with almost 79 % originating from biogenic hydrocarbons, mainly isoprene. This condensed phase net source of oxalate in conjunction with a global mean turnover time against deposition of about 5 days, maintain oxalate's global tropospheric burden of 0.2–0.3 Tg, i.e. 0.05–0.1 Tg-C that is about 5–9 % of model-calculated water soluble organic carbon burden.

Description: For the first time, the direct radiative effect (DRE) of aerosols on solar radiation is computed over the entire Mediterranean basin, one of the most climatically sensitive world regions, using a deterministic spectral radiation transfer model (RTM). The DRE effects on the outgoing shortwave radiation at the top of atmosphere (TOA), DRETOA, on the absorption of solar radiation in the atmospheric column, DREatm, and on the downward and absorbed surface solar radiation (SSR), DREsurf and DREnetsurf, respectively, are computed separately. The model uses input data for the period 2000–2007 for various surface and atmospheric parameters, taken from satellite (International Satellite Cloud Climatology Project, ISCCP-D2), Global Reanalysis projects (National Centers for Environmental Prediction – National Center for Atmospheric Research, NCEP/NCAR), and other global databases. The spectral aerosol optical properties (aerosol optical depth, AOD, asymmetry parameter, gaer and single scattering albedo, ωaer), are taken from the MODerate resolution Imaging Spectroradiometer (MODIS) of NASA (National Aeronautics and Space Administration) and they are supplemented by the Global Aerosol Data Set (GADS). The model SSR fluxes have been successfully validated against measurements from 80 surface stations of the Global Energy Balance Archive (GEBA) covering the period 2000–2007. A planetary cooling is found above the Mediterranean on an annual basis (regional mean DRETOA = −2.4 W m−2). Although a planetary cooling is found over most of the region, of up to −7 W m−2, large positive DRETOA values (up to +25 W m−2) are found over North Africa, indicating a strong planetary warming, and a weaker warming over the Alps (+0.5 W m−2). Aerosols are found to increase the absorption of solar radiation in the atmospheric column over the region (DREatm = +11.1 W m−2) and to decrease SSR (DREsurf = −16.5 W m−2 and DREnetsurf−13.5 W m−2) inducing thus significant atmospheric warming and surface radiative cooling. The calculated seasonal and monthly DREs are even larger, reaching −25.4 W m−2 (for DREsurf). Within the range of observed natural or anthropogenic variability of aerosol optical properties, AOD seems to be the main responsible parameter for modifications of regional aerosol radiative effects, which are found to be quasi-linearly dependent on AOD, ωaer and gaer.

Description: Changes in temperature due to variability in meteorology and climate change are expected to significantly impact atmospheric composition. The Mediterranean is a climate sensitive region and includes megacities like Istanbul and large urban agglomerations such as Athens. The effect of temperature changes on gaseous air pollutant levels and the atmospheric processes that are controlling them in the Eastern Mediterranean are here investigated. The WRF/CMAQ mesoscale modeling system is used, coupled with the MEGAN model for the processing of biogenic volatile organic compound emissions. A set of temperature perturbations (spanning from 1 to 5 K) is applied on a base case simulation corresponding to July 2004. The results indicate that the Eastern Mediterranean basin acts as a reservoir of pollutants and their precursor emissions from large urban agglomerations. During summer, chemistry is a major sink at these urban areas near the surface, and a minor contributor at downwind areas. On average, the atmospheric processes are more effective within the first 1000 m. The response rate of biogenic emissions to temperature changes is calculated to be 9±3% K−1. Ozone concentrations respond almost linearly to the changes in the ambient temperature with rates of 1±0.1 ppb O3 K−1 for all studied urban and receptor stations except for Istanbul, where a 0.4±0.1 ppb O3 K−1 change rate is calculated, which is almost half of the domain-averaged increase of 0.9±0.1 ppb O3 K−1. The computed changes in atmospheric processes are also linearly related with temperature changes.

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 Istanbul and Athens on local and regional air quality in the Eastern Mediterranean are quantified and the responses to hypothetical decentralization scenarios applied to the extended areas of these densely populated regions are evaluated. This study focuses on summertime impacts on air quality. The results show that Athens emissions have larger regional (0.8%) and downwind (2.7% at Finokalia) impacts on O3 than Istanbul emissions that contribute to surface O3 by 0.6% to the domain-mean and 2.1% to the levels at Finokalia. On the opposite, regarding fine particle (PM2.5) levels, Istanbul emissions have larger contribution both inside the megacity itself (75%) and regionally (2.4%) compared to Athens emissions, which have a local contribution of 65% and domain-wide contribution of 0.4%. Biogenic emissions are found to limit the production of secondary inorganic aerosol species due to their impact on oxidant levels. Hypothetical decentralization plans for these urban agglomerations, maintaining the total amount of their anthropogenic emissions constant but homogeneously distributing it over larger "new" extended areas, would result in higher O3 mixing ratios inside the urban core (215% and 26% in Istanbul and Athens, respectively). On the opposite, PM2.5 concentrations would decrease by 67% and 60% in Istanbul and Athens, respectively, whereas they would increase by 10% and 11% in the rural areas of Istanbul and Athens, respectively. Concerning the "new" extended areas, Athens would experience a reduction in O3 mixing ratios by ~2% whereas Istanbul would experience an increase by ~15%. Overall decreases of PM2.5 levels by 32% and 9% are calculated over the Istanbul and Athens "new" extended areas.

Description: We model the Penman potential evaporation (PE) over all land areas of the globe for the 25-year period 1983–2008, relying on radiation transfer models (RTMs) for the shortwave and longwave fluxes. Penman's PE is determined by two factors: available energy for evaporation and ground to atmosphere vapour transfer. Input to the PE model and RTMs comprises satellite cloud and aerosol data, as well as data from reanalyses. PE is closely linked to pan evaporation, whose trends have sparked controversy in the community, since the factors responsible for the observed pan evaporation trends are not determined with consensus. Our particular interest is the temporal evolution of PE, and the provided insight to the observed trends of pan evaporation. We examine the interannual trends of PE and various related physical quantities, such as net solar flux, net longwave flux, water vapour saturation deficit and wind speed. Our findings are the following: Global warming has led to a larger water vapour saturation deficit. Global dimming/brightening cycles in the last 25 years slightly increased the available energy for evaporation. PE trends seem to follow closely the trends of energy availability and not the trends of the atmospheric capability for vapour transfer, almost everywhere on the globe, with trends in the Northern hemisphere significantly larger than in the Southern. These results support the hypothesis that secular changes in the radiation fluxes, and not vapour transfer considerations, are responsible for potential evaporation trends.