[1] Ground-based and airborne volatile organic compound (VOC) measurements in Los Angeles, California, and Paris, France, during the Research at the Nexus of Air Quality and Climate Change (CalNex) and Megacities: Emissions, Urban, Regional and Global Atmospheric Pollution and Climate Effects, and Integrated Tools for Assessment and Mitigation (MEGAPOLI) campaigns, respectively, are used to examine the spatial variability of the composition of anthropogenic VOC urban emissions and to evaluate regional emission inventories. Two independent methods that take into account the effect of chemistry were used to determine the emission ratios of anthropogenic VOCs (including anthropogenic isoprene and oxygenated VOCs) over carbon monoxide (CO) and acetylene. Emission ratios from both methods agree within AE20%, showing the reliability of our approach. Emission ratios for alkenes, alkanes, and benzene are fairly similar between Los Angeles and Paris, whereas the emission ratios for C7-C9 aromatics in Paris are higher than in Los Angeles and other French and European Union urban areas by a factor of 2-3. The results suggest that the emissions of gasoline-powered vehicles still dominate the hydrocarbon distribution in northern mid-latitude urban areas, which disagrees with emission inventories. However, regional characteristics like the gasoline composition could affect the composition of hydrocarbon emissions. The observed emission ratios show large discrepancies by a factor of 2-4 (alkanes and oxygenated VOC) with the ones derived from four reference emission databases. A bias in CO emissions was also evident for both megacities. Nevertheless, the difference between measurements and inventory in terms of the overall OH reactivity is, in general, lower than 40%, and the potential to form secondary organic aerosols (SOA) agrees within 30% when considering volatile organic emissions as the main SOA precursors.Citation: Borbon, A., et al. (2013), Emission ratios of anthropogenic volatile organic compounds in northern mid-latitude megacities: Observations versus emission inventories in Los Angeles and Paris,

This paper presents data on elemental and mineralogical composition of mineral dust from various source regions of Africa collected during the African Monsoon Multidisciplinary Analyses (AMMA) SOP0/DABEX and Dust Ouflow and Deposition to the Ocean (DODO) DODO1 experiments (January–February 2006), and the DODO2 campaign (August 2006). Bulk filter samples were collected at the AMMA supersite of Banizoumbou, Niger, as well as on board the Facility for Airborne Atmospheric Measurements (FAAM) BAe‐146 aircraft. Both mineral dust and biomass burning in external mixing occurred in surface and elevated layers during the winter field phase of the campaign. However, mineral dust was overwhelming, accounting for 72% of the estimated aerosol mass in aged elevated biomass burning layers and up to 93% in plumes of mineral dust, which generally occurred in the boundary layer. A number of well‐defined episodes of advection of mineral dust could be identified both at the ground and on the aircraft. The elemental and mineralogical composition varied depending on source region. This variability could be well traced by the calcium content, which is enhanced in dust from North Africa but depleted in dust from the Sahel. Iron oxides in the form of hematite and goethite are enriched in dust emitted within Sahel and in Mauritania, whereas dust from the Bodélé depression is iron‐oxide depleted. Iron oxides represented between 2.4% and 4.5% of the total estimated dust oxide mass. This regional variability will have to be taken into account in estimating the optical properties of absorption of mineral dust from western Africa.

Abstract. This study presents in situ aircraft measurements of Saharan mineral dust transported over the western Mediterranean basin in June–July 2013 during the ChArMEx/ADRIMED (the Chemistry-Aerosol Mediterranean Experiment/Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region) airborne campaign. Dust events differing in terms of source region (Algeria, Tunisia and Morocco), time of transport (1–5 days) and height of transport were sampled. Mineral dust were transported above the marine boundary layer, which conversely was dominated by pollution and marine aerosols. The dust vertical structure was extremely variable and characterized by either a single layer or a more complex and stratified structure with layers originating from different source regions. Mixing of mineral dust with pollution particles was observed depending on the height of transport of the dust layers. Dust layers carried a higher concentration of pollution particles below 3 km above sea level (a.s.l.) than above 3 km a.s.l., resulting in a scattering Ångström exponent up to 2.2 below 3 km a.s.l. However, the optical properties of the dust plumes remained practically unchanged with respect to values previously measured over source regions, regardless of the altitude. Moderate absorption of light by the dust plumes was observed with values of aerosol single scattering albedo at 530 nm ranging from 0.90 to 1.00. Concurrent calculations from the aerosol chemical composition revealed a negligible contribution of pollution particles to the absorption properties of the dust plumes that was due to a low contribution of refractory black carbon in regards to the fraction of dust and sulfate particles. This suggests that, even in the presence of moderate pollution, likely a persistent feature in the Mediterranean, the optical properties of the dust plumes could be assumed similar to those of native dust in radiative transfer simulations, modelling studies and satellite retrievals over the Mediterranean. Measurements also showed that the coarse mode of mineral dust was conserved even after 5 days of transport in the Mediterranean, which contrasts with the gravitational depletion of large particles observed during the transport of dust plumes over the Atlantic. Simulations with the WRF mesoscale meteorological model highlighted a strong vertical turbulence within the dust layers that could prevent deposition of large particles during their atmospheric transport. This has important implications for the dust radiative effects due to surface dimming, atmospheric heating and cloud formation. The results presented here add to the observational data set necessary for evaluating the role of mineral dust on the regional climate and rainfall patterns in the western Mediterranean basin and understanding their atmospheric transport at global scale.

Abstract. In the last few years, several ground-based and airborne field campaigns have allowed the exploration of the properties and impacts of mineral dust in western Africa, one of the major emission and transport areas worldwide. In this paper, we explore the synthesis of these observations to provide a large-scale quantitative view of the mineralogical composition and its variability according to source region and time after transport.This work reveals that mineral dust in western Africa is a mixture of clays, quartz, iron and titanium oxides, representing at least 92 % of the dust mass. Calcite ranged between 0.3 and 8.4 % of the dust mass, depending on the origin. Our data do not show a systematic dependence of the dust mineralogical composition on origin; this is to be the case as, in most of the instances, the data represent the composition of the atmospheric burden after 1-2 days after emission, when air masses mix and give rise to a more uniform dust load. This has implications for the representation of the mineral dust composition in regional and global circulation models and in satellite retrievals.Iron oxides account for 58 ± 7 % of the mass of elemental Fe and for between 2 and 5 % of the dust mass. Most of them are composed of goethite, representing between 52 and 78 % of the iron oxide mass. We estimate that titanium oxides account for 1-2 % of the dust mass, depending on whether the dust is of Saharan or Sahelian origin.The mineralogical composition is a critical parameter for estimating the radiative and biogeochemical impact of mineral dust. The results regarding dust composition have been used to estimate the optical properties as well as the iron fractional solubility of Saharan and Sahelian dust.Data presented in this paper are provided in numerical form upon email request while they are being turned into a public database, the Dust-Mapped Archived Properties (DUST-MAP), which is an open repository for compositional data from other source regions in Africa and worldwide.

In the frame of the African Monsoon Multidisciplinary Analysis–Special Observation Period 0 (AMMA SOP0) field campaign, a sophisticated instrumental setup specially designed for documenting the characteristics of aerosols in the surface boundary layer has been operated for 1 month (13 January to 13 February 2006) at the Banizoumbou supersite in Niger. The analysis of the long‐term routine sunphotometer measurements shows that the intensive measurements were performed during a transition phase between a period when biomass burning aerosols are present in the atmospheric column and another when mineral dust is clearly predominant. On the basis of ground‐level observations, three types of events can be defined. (1) Type B events are those corresponding to advection of Biomass burning plumes from southern Sahel. They represent only 3% of the measurement period. (2) Type D events are those during which mineral dust concentrations are larger than 200 μg m−3. They represent 35% of the measuring time, and coincide with advection of mineral dust from distant sources to the measurement site. The composition of the dust differs significantly from one episode to the other, depending on the trajectory of air mass that transported it. (3) Type L events are those that can be explained by occurrence of local erosion and that are of short duration. During them, the aerosol size distribution is dominated by a coarser mode (9 μm) than during the events of the D type dominated by a finer mode (4.5 μm). Elemental analysis also shows that mineral dust is relatively rich in Fe and poor in Ca, which is typical of the Sahelian aerosols.

This paper reports on the X-ray absorption analysis of samples of mineral dust emitted from or transported to Western Africa. We found that iron oxides account, by mass, for 38% to 72% of the total elemental iron. They are composed of minerals in the Fe(III) oxidation state: goethite (FeO·OH) and hematite (Fe 2 O 3 ). The apparent fraction of iron oxide attributed to goethite is higher than hematite regardless of the source region from which the dust originated. The goethite percent content of iron oxides is in the range 52-78% (by mass), the highest values being measured for dust originating in the Sahel. The limited number of samples analyzed and the sample-to-sample variability prevent us from concluding firmly on the regional variability of the goethite-to-hematite ratio. Based on the experimental data on mineralogical composition and on concurrent measurements of the number size distribution, the optical properties of mineral dust have been calculated in a Mie approximation for homogeneous spherical particles. At 550 nm, the single-scattering albedo ω 0 ranges between 0.89 and 0.93, the asymmetry factor g ranges between 0.76 and 0.8 and the mass extinction efficiency k ext varies between 0.5 and 1.1 m 2 g À1 ; these values are all in the range of those from independent direct measurements. Neglecting the partitioning between hematite and goethite and the assimilation of iron oxides by hematite, as it is often done with models, lowers the single-scattering albedo and increases the asymmetry factor in the UV-visible spectral region below 550 nm. The mass extinction efficiency is insensitive to the nature of the iron oxides but rather responds to variations in the number size distribution. The mineralogy of iron oxides should therefore be taken into account when assessing the effect of mineral dust on climate and atmospheric chemistry, in particular via interactions involving photolysis.

Abstract. This paper presents new laboratory measurements of the mass absorption efficiency (MAE) between 375 and 850 nm for 12 individual samples of mineral dust from different source areas worldwide and in two size classes: PM 10.6 (mass fraction of particles of aerodynamic diameter lower than 10.6 µm) and PM 2.5 (mass fraction of particles of aerodynamic diameter lower than 2.5 µm). The experiments were performed in the CESAM simulation chamber using mineral dust generated from natural parent soils and included optical and gravimetric analyses.The results show that the MAE values are lower for the PM 10.6 mass fraction (range 37-135 × 10 −3 m 2 g −1 at 375 nm) than for the PM 2.5 (range 95-711 × 10 −3 m 2 g −1 at 375 nm) and decrease with increasing wavelength as λ −AAE , where the Ångström absorption exponent (AAE) averages between 3.3 and 3.5, regardless of size. The size independence of AAE suggests that, for a given size distribution, the dust composition did not vary with size for this set of samples. Because of its high atmospheric concentration, light absorption by mineral dust can be competitive with black and brown carbon even during atmospheric transport over heavy polluted regions, when dust concentrations are significantly lower than at emission. The AAE values of mineral dust are higher than for black carbon (∼ 1) but in the same range as light-absorbing organic (brown) carbon. As a result, depending on the environment, there can be some ambiguity in apportioning the aerosol absorption optical depth (AAOD) based on spectral dependence, which is relevant to the development of remote sensing of light-absorbing aerosols and their assimilation in climate models. We suggest that the sample-to-sample variability in our dataset of MAE values is related to regional differences in the mineralogical composition of the parent soils. Particularly in the PM 2.5 fraction, we found a strong linear correlation between the dust lightPublished by Copernicus Publications on behalf of the European Geosciences Union. 7176 L. Caponi et al.: Spectral-and size-resolved mass absorption efficiency of mineral dust aerosols absorption properties and elemental iron rather than the iron oxide fraction, which could ease the application and the validation of climate models that now start to include the representation of the dust composition, as well as for remote sensing of dust absorption in the UV-vis spectral region.

Abstract. 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....