Since the 1980s several spaceborne sensors have been used to retrieve the aerosol optical depth (AOD) over the Mediterranean region. In parallel, AOD climatologies coming from different numerical model simulations are now also available, permitting to distinguish the contribution of several aerosol types to the total AOD. In this work, we perform a comparative analysis of this unique multi-year database in terms of total AOD and of its apportionment by the five main aerosol types (soil dust, sea-salt, sulfate, black and organic carbon). We use 9 different satellite-derived monthly AOD products: NOAA/AVHRR, SeaWiFS (2 products), TERRA/MISR, TERRA/MODIS, AQUA/MODIS, ENVISAT/MERIS, PARASOL/POLDER and MSG/SEVIRI, as well as 3 more historical datasets: NIMBUS7/CZCS, TOMS (onboard NIMBUS7 and Earth-Probe) and METEOSAT/MVIRI. Monthly model datasets include the aerosol climatology from Tegen et al. (1997), the climate-chemistry models LMDz-OR-INCA and RegCM-4, the multi-model mean coming from the ACCMIP exercise, and the reanalyses GEMS and MACC. Ground-based Level-2 AERONET AOD observations from 47 stations around the basin are used here to evaluate the model and satellite data. The sensor MODIS (on AQUA and TERRA) has the best average AOD scores over this region, showing a relevant spatio-temporal variability and highlighting high dust loads over Northern Africa and the sea (spring and summer), and sulfate aerosols over continental Europe (summer). The comparison also shows limitations of certain datasets (especially MERIS and SeaWiFS standard products). Models reproduce the main patterns of the AOD variability over the basin. The MACC reanalysis is the closest to AERONET data, but appears to underestimate dust over Northern Africa, where RegCM-4 is found closer to MODIS thanks to its interactive scheme for dust emissions. The vertical dimension is also investigated using the CALIOP instrument. This study confirms differences of vertical distribution between dust aerosols showing a large vertical spread, and other continental and marine aerosols which are confined in the boundary layer. From this compilation, we propose a 4-D blended product from model and satellite data, consisting in monthly time series of 3-D aerosol distribution at a 50 km horizontal resolution over the Euro-Mediterranean marine and continental region for the 2003–2009 period. The product is based on the total AOD from AQUA/MODIS, apportioned into sulfates, black and organic carbon from the MACC reanalysis, and into dust and sea-salt aerosols from RegCM-4 simulations, which are distributed vertically based on CALIOP climatology. We extend the 2003–2009 reconstruction to the past up to 1979 using the 2003–2009 average and applying the decreasing trend in sulfate aerosols from LMDz-OR-INCA, whose AOD trends over Europe and the Mediterranean are median among the ACCMIP models. Finally optical properties of the different aerosol types in this region are proposed from Mie calculations so that this reconstruction can be included in regional climate models for aerosol radiative forcing and aerosol-climate studies.

The Chemistry-Aerosol Mediterranean Experiment (ChArMEx; http://charmex.lsce.ipsl.fr) is a collaborative research program federating international activities to investigate Mediterranean regional chemistry-climate interactions. A special observing period (SOP-1a) including intensive airborne measurements was performed in the framework of the Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region (ADRIMED) project during the Mediterranean dry season over the western and central Mediterranean basins, with a focus on aerosol-radiation measurements and their modeling. The SOP-1a took place from 11 June to 5 July 2013. Airborne measurements were made by both the ATR-42 and F-20 French research aircraft operated from Sardinia (Italy) and instrumented for in situ and remote-sensing measurements, respectively, and by sounding and drifting balloons, launched in Minorca. The experimental setup also involved several ground-based measurement sites on islands including two ground-based reference stations in Corsica and Lampedusa and secondary monitoring sites in Minorca and Sicily. Additional measurements including lidar profiling were also performed on alert during aircraft operations at EARLINET/ACTRIS stations at Granada and Barcelona in Spain, and in southern Italy. Remote-sensing aerosol products from satellites (MSG/SEVIRI, MODIS) and from the AERONET/PHOTONS network were also used. Dedicated meso-scale and regional modeling experiments were performed in relation to this observational effort. We provide here an overview of the different surface and aircraft observations deployed during the ChArMEx/ADRIMED period and of associated modeling studies together with an analysis of the synoptic conditions that determined the aerosol emission and transport. Meteorological conditions observed during this campaign (moderate temperatures and southern flows) were not favorable to producing high levels of atmospheric pollutants or intense biomass burning events in the region. However, numerous mineral dust plumes were observed during the campaign, with the main sources located in Morocco, Algeria and Tunisia, leading to aerosol optical depth (AOD) values ranging between 0.2 and 0.6 (at 440 nm) over the western and central Mediterranean basins. One important point of this experiment concerns the direct observations of aerosol extinction onboard the ATR-42, using the CAPS system, showing local maxima reaching up to 150 M m⁻¹ within the dust plume. Non-negligible aerosol extinction (about 50 M m⁻¹) has also been observed within the marine boundary layer (MBL). By combining the ATR-42 extinction coefficient observations with absorption and scattering measurements, we performed a complete optical closure revealing excellent agreement with estimated optical properties. This additional information on extinction properties has allowed calculation of the dust single scattering albedo (SSA) with a high level of confidence over the western Mediterranean. Our results show a moderate variability from 0.90 to 1.00 (at 530 nm) for all flights studied compared to that reported in the literature on this optical parameter. Our results underline also a relatively low difference in SSA with values derived near dust sources. In parallel, active remote-sensing observations from the surface and onboard the F-20 aircraft suggest a complex vertical structure of particles and distinct aerosol layers with sea spray and pollution located within the MBL, and mineral dust and/or aged North American smoke particles located above (up to 6–7 km in altitude). Aircraft and balloon-borne observations allow one to investigate the vertical structure of the aerosol size distribution showing particles characterized by a large size (> 10 µm in diameter) within dust plumes. In most of cases, a coarse mode characterized by an effective diameter ranging between 5 and 10 µm, has been detected above the MBL. In terms of shortwave (SW) direct forcing, in situ surface and aircraft observations have been merged and used as inputs in 1-D radiative transfer codes for calculating the aerosol direct radiative forcing (DRF). Results show significant surface SW instantaneous forcing (up to −90 W m⁻² at noon). Aircraft observations provide also original estimates of the vertical structure of SW and LW radiative heating revealing significant instantaneous values of about 5° K per day in the solar spectrum (for a solar angle of 30°) within the dust layer. Associated 3-D modeling studies from regional climate (RCM) and chemistry transport (CTM) models indicate a relatively good agreement for simulated AOD compared with observations from the AERONET/PHOTONS network and satellite data, especially for long-range dust transport. Calculations of the 3-D SW (clear-sky) surface DRF indicate an average of about −10 to −20 W m⁻² (for the whole period) over the Mediterranean Sea together with maxima (−50 W m⁻²) over northern Africa. The top of the atmosphere (TOA) DRF is shown to be highly variable within the domain, due to moderate absorbing properties of dust and changes in the surface albedo. Indeed, 3-D simulations indicate negative forcing over the Mediterranean Sea and Europe and positive forcing over northern Africa. Finally, a multi-year simulation, performed for the 2003 to 2009 period and including an ocean–atmosphere (O–A) coupling, underlines the impact of the aerosol direct radiative forcing on the sea surface temperature, O–A fluxes and the hydrological cycle over the Mediterranean.

Aerosol absorption properties are of high importance to assess aerosol impact on regional climate. This study presents an analysis of aerosol absorption products obtained over the Mediterranean basin or land stations in the region from multi-year ground-based AERONET observations with a focus on the Absorbing Aerosol Optical Depth (AAOD), Single Scattering Albedo (SSA) and their spectral dependence. The AAOD and Absorption Angström Exponent (AAE) dataset is composed of daily averaged AERONET level 2 data from a total of 22 Mediterranean stations having long time series, mainly under the influence of urban-industrial aerosols and/or soil dust. This dataset covers the 17-yr period 1996–2012 with most data being from 2003–2011 (~89% of level-2 AAOD data). Since AERONET level-2 absorption products require a high aerosol load (AOD at 440 nm > 0.4), which is most often related to the presence of desert dust, we also consider level-1.5 SSA data, despite their higher uncertainty, and filter out data with an Angström exponent < 1.0 in order to study absorption by carbonaceous aerosols. The SSA dataset includes AERONET level-2 products. Sun-photometer observations show that values of AAOD at 440 nm vary between 0.024 ± 0.01 (resp. 0.040 ± 0.01) and 0.050 ± 0.01 (0.055 ± 0.01) for urban (dusty) sites. Analysis shows that the Mediterranean urban-industrial aerosols appear "moderately" absorbing with values of SSA close to ~0.94–0.95 ± 0.04 (at 440 nm) in most cases except over the large cities of Rome and Athens, where aerosol appears more absorbing (SSA ~0.89–0.90 ± 0.04). The aerosol Absorption Angström Exponent (AAE, estimated using 440 and 870 nm) is found to be larger than 1 for most sites over the Mediterranean, a manifestation of mineral dust (iron) and/or brown carbon producing the observed absorption. AERONET level-2 sun-photometer data indicate a possible East-West gradient, with higher values over the eastern basin (AAE_East = 1.39/AAE_West = 1.33). The North-South AAE gradient is more pronounced, especially over the western basin. Our additional analysis of AERONET level-1.5 data also shows that organic absorbing aerosols significantly affect some Mediterranean sites. These results indicate that current climate models treating organics as nonabsorbing over the Mediterranean certainly underestimate the warming effect due to carbonaceous aerosols.

The study of aerosols in the troposphere and in the stratosphere is of major importance both for climate and air quality studies. Among the numerous instruments available, optical aerosol particles counters (OPCs) provide the size distribution in diameter range from about 100 nm to a few tens of µm. Most of them are very sensitive to the nature of aerosols, and this can result in significant biases in the retrieved size distribution. We describe here a new versatile optical particle/sizer counter named LOAC (Light Optical Aerosol Counter), which is light and compact enough to perform measurements not only at the surface but under all kinds of balloons in the troposphere and in the stratosphere. LOAC is an original OPC performing observations at two scattering angles. The first one is around 12°, and is almost insensitive to the refractive index of the particles; the second one is around 60° and is strongly sensitive to the refractive index of the particles. By combining measurement at the two angles, it is possible to retrieve the size distribution between 0.2 and 100 µm and to estimate the nature of the dominant particles (droplets, carbonaceous, salts and mineral particles) when the aerosol is relatively homogeneous. This typology is based on calibration charts obtained in the laboratory. The uncertainty for total concentrations measurements is ±20 % when concentrations are higher than 1 particle cm⁻³ (for a 10 min integration time). For lower concentrations, the uncertainty is up to about ±60 % for concentrations smaller than 10⁻² particle cm⁻³. Also, the uncertainties in size calibration are ±0.025 µm for particles smaller than 0.6 µm, 5 % for particles in the 0.7–2 µm range, and 10 % for particles greater than 2 µm. The measurement accuracy of submicronic particles could be reduced in a strongly turbid case when concentration of particles > 3 µm exceeds a few particles cm⁻³. Several campaigns of cross-comparison of LOAC with other particle counting instruments and remote sensing photometers have been conducted to validate both the size distribution derived by LOAC and the retrieved particle number density. The typology of the aerosols has been validated in well-defined conditions including urban pollution, desert dust episodes, sea spray, fog, and cloud. Comparison with reference aerosol mass monitoring instruments also shows that the LOAC measurements can be successfully converted to mass concentrations.

Daily modeled fields of phosphate deposition to the Mediterranean from natural dust, anthropogenic combustion and wildfires were used to assess the effect of this external nutrient on marine biogeochemistry. The ocean model used is a high-resolution (1∕12°) regional coupled dynamical–biogeochemical model of the Mediterranean Sea (NEMO-MED12/PISCES). The input fields of phosphorus are for 2005, which are the only available daily resolved deposition fields from the global atmospheric chemical transport model LMDz-INCA. Traditionally, dust has been suggested to be the main atmospheric source of phosphorus, but the LMDz-INCA model suggests that combustion is dominant over natural dust as an atmospheric source of phosphate (PO₄, the bioavailable form of phosphorus in seawater) for the Mediterranean Sea. According to the atmospheric transport model, phosphate deposition from combustion (Pcomb) brings on average 40.5×10⁻⁶ mol PO₄ m⁻² yr⁻¹ over the entire Mediterranean Sea for the year 2005 and is the primary source over the northern part (e.g., 101×10⁻⁶ mol PO₄ m⁻² yr⁻¹ from combustion deposited in 2005 over the north Adriatic against 12.4×10⁻⁶ from dust). Lithogenic dust brings 17.2×10⁻⁶ mol PO₄ m⁻² yr⁻¹ on average over the Mediterranean Sea in 2005 and is the primary source of atmospheric phosphate to the southern Mediterranean Basin in our simulations (e.g., 31.8×10⁻⁶ mol PO₄ m⁻² yr⁻¹ from dust deposited in 2005 on average over the south Ionian basin against 12.4×10⁻⁶ from combustion). The evaluation of monthly averaged deposition flux variability of Pdust and Pcomb for the 1997–2012 period indicates that these conclusions may hold true for different years. We examine separately the two atmospheric phosphate sources and their respective flux variability and evaluate their impacts on marine surface biogeochemistry (phosphate concentration, chlorophyll a, primary production). The impacts of the different phosphate deposition sources on the biogeochemistry of the Mediterranean are found localized, seasonally varying and small, but yet statistically significant. Differences in the geographical deposition patterns between phosphate from dust and from combustion will cause contrasted and significant changes in the biogeochemistry of the basin. We contrast the effects of combustion in the northern basin (Pcomb deposition effects are found to be 10 times more important in the northern Adriatic, close to the main source region) to the effects of dust in the southern basin. These different phosphorus sources should therefore be accounted for in modeling studies.

Previous studies have provided some insight into the Saharan dust deposition at a few specific locations from observations over long time periods or intensive field campaigns. However, no assessment of the dust deposition temporal variability in connection with its regional spatial distribution has been achieved so far from network observations over more than 1 year. To investigate dust deposition dynamics at the regional scale, five automatic deposition collectors named CARAGA (Collecteur Automatique de Retombées Atmosphériques insolubles à Grande Autonomie in French) have been deployed in the western Mediterranean region during 1 to 3 years depending on the station. The sites include, from south to north, Lampedusa, Majorca, Corsica, Frioul and Le Casset (southern French Alps). Deposition measurements are performed on a common weekly period at the five sites. The mean dust deposition fluxes are higher close to the northern African coasts and decrease following a south–north gradient, with values from 7.4 g m⁻² year⁻¹ in Lampedusa (35°31′ N, 12°37′ E) to 1 g m⁻² year⁻¹ in Le Casset (44°59′ N, 6°28′ E). The maximum deposition flux recorded is of 3.2 g m⁻² wk⁻¹ in Majorca with only two other events showing more than 1 g m⁻² wk⁻¹ in Lampedusa, and a maximum of 0.5 g m⁻² wk⁻¹ in Corsica. The maximum value of 2.1 g m⁻² year⁻¹ observed in Corsica in 2013 is much lower than existing records in the area over the 3 previous decades (11–14 g m⁻² year⁻¹). From the 537 available samples, 98 major Saharan dust deposition events have been identified in the records between 2011 and 2013. Complementary observations provided by both satellite and air mass trajectories are used to identify the dust provenance areas and the transport pathways from the Sahara to the stations for the studied period. Despite the large size of African dust plumes detected by satellites, more than 80 % of the major dust deposition events are recorded at only one station, suggesting that the dust provenance, transport and deposition processes (i.e. wet vs. dry) of dust are different and specific for the different deposition sites in the Mediterranean studied area. The results tend to indicate that wet deposition is the main form of deposition for mineral dust in the western Mediterranean basin, but the contribution of dry deposition (in the sense that no precipitation was detected at the surface) is far from being negligible, and contributes 10 to 46 % to the major dust deposition events, depending on the sampling site.