[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,

Abstract. Long-term monitoring of the chemical composition of clouds (73 cloud events representing 199 individual samples) sampled at the puy de Dôme (pdD) station (France) was performed between 2001 and 2011. Physicochemical parameters, as well as the concentrations of the major organic and inorganic constituents, were measured and analyzed by multicomponent statistical analysis. Along with the corresponding back-trajectory plots, this allowed for distinguishing four different categories of air masses reaching the summit of the pdD: polluted, continental, marine and highly marine. The statistical analysis led to the determination of criteria (concentrations of inorganic compounds, pH) that differentiate each category of air masses. Highly marine clouds exhibited high concentrations of Na+ and Cl−; the marine category presented lower concentration of ions but more elevated pH. Finally, the two remaining clusters were classified as "continental" and "polluted"; these clusters had the second-highest and highest levels of NH4+, NO3−, and SO24−, respectively. This unique data set of cloud chemical composition is then discussed as a function of this classification. Total organic carbon (TOC) is significantly higher in polluted air masses than in the other categories, which suggests additional anthropogenic sources. Concentrations of carboxylic acids and carbonyls represent around 10% of the organic matter in all categories of air masses and are studied for their relative importance. Iron concentrations are significantly higher for polluted air masses and iron is mainly present in its oxidation state (+II) in all categories of air masses. Finally, H2O2 concentrations are much more varied in marine and highly marine clouds than in polluted clouds, which are characterized by the lowest average concentration of H2O2. This data set provides concentration ranges of main inorganic and organic compounds for modeling purposes on multiphase cloud chemistry.

During July 2009, a one-month measurement campaign was performed in the megacity of Paris. Amongst other measurement platforms, three stationary sites distributed over an area of 40 km in diameter in the greater Paris region enabled a detailed characterization of the aerosol particle and gas phase. Simulation results from the FLEXPART dispersion model were used to distinguish between different types of air masses sampled. It was found that the origin of air masses had a large influence on measured mass concentrations of the secondary species particulate sulphate, nitrate, ammonium, and oxygenated organic aerosol measured with the Aerodyne aerosol mass spectrometer in the submicron particle size range: particularly high concentrations of these species (about 4 μg m^−3, 2 μg m^−3, 2 μg m^−3, and 7 μg m^−3, respectively) were measured when aged material was advected from continental Europe, while for air masses originating from the Atlantic, much lower mass concentrations of these species were observed (about 1 μg m^−3, 0.2 μg m^−3, 0.4 μg m^−3, and 1–3 μg m^−3, respectively). For the primary emission tracers hydrocarbon-like organic aerosol, black carbon, and NO_x it was found that apart from diurnal source strength variations and proximity to emission sources, local meteorology had the largest influence on measured concentrations, with higher wind speeds leading to larger dilution and therefore smaller measured concentrations. Also the shape of particle size distributions was affected by wind speed and air mass origin. Quasi-Lagrangian measurements performed under connected flow conditions between the three stationary sites were used to estimate the influence of the Paris emission plume onto its surroundings, which was found to be rather small. Rough estimates for the impact of the Paris emission plume on the suburban areas can be inferred from these measurements: Volume mixing ratios of 1–14 ppb of NO_x, and upper limits for mass concentrations of about 1.5 μg m^−3 of black carbon and of about 3 μg m^−3 of hydrocarbon-like organic aerosol can be deduced which originate from both, local emissions and the overall Paris emission plume. The secondary aerosol particle phase species were found to be not significantly influenced by the Paris megacity, indicating their regional origin. The submicron aerosol mass concentrations of particulate sulphate, nitrate, and ammonium measured during time periods when air masses were advected from eastern central Europe were found to be similar to what has been found from other measurement campaigns in Paris and south-central France for this type of air mass origin, indicating that the results presented here are also more gen...

The European Union (EU)-funded project Dynamics–Aerosol–Chemistry–Cloud Interactions in West Africa (DACCIWA) investigates the relationship between weather, climate, and air pollution in southern West Africa—an area with rapid population growth, urbanization, and an increase in anthropogenic aerosol emissions. The air over this region contains a unique mixture of natural and anthropogenic gases, liquid droplets, and particles, emitted in an environment in which multilayer clouds frequently form. These exert a large influence on the local weather and climate, mainly owing to their impact on radiation, the surface energy balance, and thus the diurnal cycle of the atmospheric boundary layer. In June and July 2016, DACCIWA organized a major international field campaign in Ivory Coast, Ghana, Togo, Benin, and Nigeria. Three supersites in Kumasi, Savè, and Ile-Ife conducted permanent measurements and 15 intensive observation periods. Three European aircraft together flew 50 research flights between 27 June and 16 July 2016, for a total of 155 h. DACCIWA scientists launched weather balloons several times a day across the region (772 in total), measured urban emissions, and evaluated health data. The main objective was to build robust statistics of atmospheric composition, dynamics, and low-level cloud properties in various chemical landscapes to investigate their mutual interactions. This article presents an overview of the DACCIWA field campaign activities as well as some first research highlights. The rich data obtained during the campaign will be made available to the scientific community and help to advance scientific understanding, modeling, and monitoring of the atmosphere over southern West Africa.

A detailed characterization of air quality in the megacity of Paris (France) during two 1-month intensive campaigns and from additional 1-year observations revealed that about 70% of the urban background fine particulate matter (PM) is transported on average into the megacity from upwind regions. This dominant influence of regional sources was confirmed by in situ measurements during short intensive and longer-term campaigns, aerosol optical depth (AOD) measurements from ENVISAT, and modeling results from PMCAMx and CHIMERE chemistry transport models. While advection of sulfate is well documented for other megacities, there was surprisingly high contribution from long-range transport for both nitrate and organic aerosol. The origin of organic PM was investigated by comprehensive analysis of aerosol mass spectrometer (AMS), radiocarbon and tracer measurements during two intensive campaigns. Primary fossil fuel combustion emissions constituted less than 20% in winter and 40% in summer of carbonaceous fine PM, unexpectedly small for a megacity. Cooking activities and, during winter, residential wood burning are the major primary organic PM sources. This analysis suggests that the major part of secondary organic aerosol is of modern origin, i.e., from biogenic precursors and from wood burning. Black carbon concentrations are on the lower end of values encountered in megacities worldwide, but still represent an issue for air quality. These comparatively low air pollution levels are due to a combination of low emissions per inhabitant, flat terrain, and a meteorology that is in general not conducive to local pollution build-up. This revised picture of a megacity only being partially responsible for its own average and peak PM levels has important implications for air pollution regulation policies

Detailed investigations of the chemical and microphysical properties of atmospheric aerosol particles were performed at the puy-de-Dôme (pdD) research station (1465 m) in autumn (September and October 2008), winter (February and March 2009), and summer (June 2010) using a compact Time-of-Flight Aerosol Mass Spectrometer (cToF-AMS). Over the three campaigns, the average mass concentrations of the non-refractory submicron particles ranged from 10 μg m^&minus;3 up to 27 μg m^&minus;3. Highest nitrate and ammonium mass concentrations were measured during the winter and during periods when marine modified airmasses were arriving at the site, whereas highest concentrations of organic particles were measured during the summer and during periods when continental airmasses arrived at the site. The measurements reported in this paper show that atmospheric particle composition is strongly influenced by both the season and the origin of the airmass. The total organic mass spectra were analysed using positive matrix factorisation to separate individual organic components contributing to the overall organic particle mass concentrations. These organic components include a low volatility oxygenated organic aerosol particle (LV-OOA) and a semi-volatile organic aerosol particle (SV-OOA). Correlations of the LV-OOA components with fragments of <i>m/z</i> 60 and <i>m/z</i> 73 (mass spectral markers of wood burning) during the winter campaign suggest that wintertime LV-OOA are related to aged biomass burning emissions, whereas organic aerosol particles measured during the summer are likely linked to biogenic sources. Equivalent potential temperature calculations, gas-phase, and LIDAR measurements define whether the research site is in the planetary boundary layer (PBL) or in the free troposphere (FT)/residual layer (RL). We observe that SV-OOA and nitrate particles are associated with air masses arriving from the PBL where as particle composition measured from RL/FT airmasses contain high mass fractions of sulphate and LV-OOA. This study provides unique insights into the effects of season and airmass variability on regional aerosol particles measured at an elevated site

Abstract. Since the nineties, atmospheric measurement systems have been deployed at Reunion Island, mainly for monitoring the atmospheric composition in the framework of NDSC/NDACC (Network for the Detection of Stratospheric

Environmental context. Oceans represent 70% of the blue planet, and surprisingly, ocean emission in term of volatile organic compounds is poorly understood. The potential climate impacts on a global scale of various trace organic gases have been established, and the terrestrial inputs are well studied, but little is known about which of these can be emitted from oceanic sources. In the present study, atmospheric samples were taken over the Southern Indian Ocean, while crossing some oceanic fronts and different phytoplankton species. Such a study should aid in understanding oceanic emission, especially from phytoplankton, and will help modellers to determine concentrations of organic traces in the remote marine troposphere. Abstract. Considering its size and potential importance, the ocean is poorly characterised in terms of volatile organic compounds (VOC) that play important roles in global atmospheric chemistry. In order to better understand their potential sources and sinks over the Southern Indian Austral Ocean, shipborne measurements of selected species were made during the MANCHOT campaign during December 2004, on board the research vessel Marion Dufresne. Along the transect La Réunion to Kerguelen Island, air measurements of selected VOC (including dimethylsulfide (DMS) isoprene, carbonyls and organohalogens), carbon monoxide and ozone were performed, crossing subtropical, temperate and sub-Antarctic waters as well as pronounced subtropical and sub-Antarctic oceanic fronts. The remote marine boundary layer was characterised at latitudes 45–50°S. Oceanic fronts were associated with enhanced chlorophyll and biological activity in the seawater and elevated DMS and organohalogens in the atmosphere. These were compared with a satellite-derived phytoplankton distribution (PHYSAT). Diurnal variation for isoprene, terpenes, acetone and acetaldehyde was observed, analogously to recent results observed in mesocosm experiments.