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Land–atmosphere interactions govern the process of dust emission and transport. An accurate depiction of these physical processes within numerical weather prediction models allows for better estimating the spatial and temporal distribution of the dust burden and the characterisation of source and recipient areas. In the presented study, the ECMWF-IFS (European Centre for Medium-Range Weather Forecast – Integrated Forecasting System) outputs, produced with and without the assimilation of Aeolus quality-assured Rayleigh–clear and Mie–cloudy horizontal line-of-sight wind profiles, are used as initial or boundary conditions in the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) to simulate 2-month periods in the spring and autumn of 2020, focusing on a case study in October. The experiments have been performed over the broader eastern Mediterranean and Middle East (EMME) region, which is frequently subjected to dust transport, as it encompasses some of the most active erodible dust sources. Aerosol- and dust-related model outputs (extinction coefficient, optical depth and concentrations) are qualitatively and quantitatively evaluated against ground- and satellite-based observations. Ground-based columnar and vertically resolved aerosol optical properties are acquired through AERONET sun photometers and PollyXT lidar, while near-surface concentrations are taken from EMEP. Satellite-derived vertical dust and columnar aerosol optical properties are acquired through LIVAS (LIdar climatology of Vertical Aerosol Structure) and MIDAS (ModIs Dust AeroSol), respectively. Overall, in cases of either high or low aerosol loadings, the model predictive skill is improved when WRF-Chem simulations are initialised with the meteorological fields of Aeolus wind profiles assimilated by the IFS. The improvement varies in space and time, with the most significant impact observed during the autumn months in the study region. Comparison with observation datasets saw a remarkable improvement in columnar aerosol optical depths, vertically resolved dust mass concentrations and near-surface particulate concentrations in the assimilated run against the control run. Reductions in model biases, either positive or negative, and an increase in the correlation between simulated and observed values was achieved for October 2020.

Mineral dust and sea spray aerosol represent important sources of ice-nucleating particles (INPs), the minor fraction of aerosol particles able to trigger cloud ice crystal formation and, consequently, influence multiple climate-relevant cloud properties including lifetime, radiative properties and precipitation initiation efficiency. Mineral dust is considered the dominant INP source in many parts of the world due to its ice nucleation efficiency and its sheer abundance, with global emission rates of up to 4700 Tg a−1. However, INPs emitted from the ocean surface in sea spray aerosol frequently dominate INP populations in remote marine environments, including parts of the Southern Ocean where cloud-resolving model simulations have demonstrated that cloud radiative properties are likely strongly controlled by INPs. Here we report INP concentrations measured in aerosol and seawater samples during Air Quality and Climate Change in the Arabian Basin (AQABA), a shipborne campaign that spanned the Red Sea, Gulf of Aden, Arabian Sea, Arabian Gulf and part of the Mediterranean. In aerosol samples collected within a few hundred kilometers of the first and second ranked sources of dust globally, the Sahara and Arabian Peninsula, INP concentrations ranged from 0.2 to 11 L−1 at −20 ∘C with observed ice-active surface site densities (ns) 1–3 orders of magnitude below levels predicted by mineral dust INP parameterizations. Over half of the samples (at least 14 of 26) were collected during dust storms with average dust mass concentrations between 150 and 490 µg m−3 (PM10), as simulated by the Modern-Era Retrospective analysis for Research and Application, version 2 (MERRA-2). The impacts of heat and peroxide treatments indicate that organics dominated the observed ice nucleation (IN) activity at temperatures ≥ −15 ∘C with proteinaceous (heat-labile) INPs frequently observed at high freezing temperatures >−10 ∘C. INP concentrations in seawater samples ranged between 3 and 46 mL−1 at −19 ∘C, demonstrating the relatively low INP source potential of seawater in the region as compared to seawater from multiple other regions reported previously. Overall, our results demonstrate that despite proximity to the Sahara and the Arabian Peninsula and the dominance of mineral dust in the aerosol sampled, existing mineral dust parameterizations alone would not skillfully represent the near-surface ns in the observed temperature regime (−6 to −25 ∘C). Future efforts to develop or improve representations of dust INPs at modest supercooling (≥-15 ∘C) would benefit from a characterization of the specific organic species associated with dust INPs. More generally, an improved understanding of the organic species associated with increased IN activity and their variability across dust source regions would directly inform efforts to determine whether ns-based parameterizations are appropriate for faithful representation of dust INPs in this sensitive temperature regime, whether region-specific parameterizations are required, or whether an alternative to the ns approach is necessary.

Urban areas and industrial facilities, which concentrate the majority of human activity and industrial production, are major sources of air pollutants, with serious implications for human health and global climate. For most of these pollutants, emission inventories are often highly uncertain, especially in developing countries. Spaceborne measurements from the TROPOMI instrument, on board the Sentinel-5 Precursor satellite, are used to retrieve nitrogen dioxide (NO2) column densities at high spatial resolution. Here, we use 2 years of TROPOMI retrievals to map nitrogen oxide (NOx = NO + NO2) emissions in Egypt with a top-down approach using the continuity equation in steady state. Emissions are expressed as the sum of a transport term and a sink term representing the three-body reaction comprising NO2 and hydroxyl radical (OH). This sink term requires information on the lifetime of NO2, which is calculated with the use of the CAMS near-real-time temperature and OH concentration fields. We compare this derived lifetime with the lifetime inferred from the fitting of NO2 line density profiles in large plumes with an exponentially modified Gaussian function. This comparison, which is conducted for different samples of NO2 patterns above the city of Riyadh, provides information on the reliability of the CAMS near-real-time OH concentration fields; it also provides some hint on the vertical levels that best represent typical pollution sources in industrial areas and megacities in the Middle East region. In Egypt, total emissions of NOx are dominated by the sink term, but they can be locally dominated by wind transport, especially along the Nile where human activities are concentrated. Megacities and industrial regions clearly appear as the largest sources of NOx emissions in the country. Our top-down model infers emissions with a marked annual variability. By looking at the spatial distribution of emissions at the scale of different cities with different industrial characteristics, it appears that this variability is consistent with national electricity consumption. We detect lower emissions on Fridays, which are inherent to the social norm of the country, and quantify the drop in emissions in 2020 due to the COVID-19 pandemic. Overall, our estimations of NOx emissions for Egypt are 7.0 % higher than the CAMS-GLOB-ANT_v4.2 inventory and significantly differ in terms of seasonality.

With the growing evidence that high particle number concentrations may impact health, modelling their emissions and understanding formation processes is necessary, especially in cities where many people are exposed. As emission inventories of particle numbers and size distribution over cities are usually not available, a methodology is defined to estimate them from PM2.5 emissions and ratios of PM1 / PM2.5 and PM0.1 / PM2.5 by activity sector. In this methodology, a fitting parameter αem is used to redistribute the number concentrations in the lowest emission diameter range. This parameter is chosen by comparing measured and simulated number concentrations during non-nucleation days. The emission size distribution is then finely discretised by conserving both mass and number in each of the size ranges where emissions are specified. The methodology is applied over Greater Paris during the MEGAPOLI campaign (July 2009). Three-dimensional simulations are performed using the chemistry transport model Polair3D/Polyphemus coupled to the aerosol module SSH-aerosol to represent the evolution of particles by condensation, evaporation, coagulation, and nucleation, with a sectional approach for the size distribution. The model is first compared to measurements during non-nucleation days, and the influence over the month of July 2009 of three different nucleation parameterisations is assessed, i.e. binary (sulfuric acid, water), ternary (sulfuric acid, ammonia, water), and heteromolecular (extremely low-volatility organic compounds (ELVOCs) from monoterpenes and sulfuric acid). The modelled number concentrations compare very well to measurements, with an average normalised mean error of 42 % for the daily number concentrations of particles larger than 10 nm and 37 % for the number concentrations of particles larger than 100 nm. The influence of the binary nucleation is low, and the ternary nucleation scheme leads to better simulated number concentrations (in terms of bias and error) at only one site out of three, but it systematically reduces the model to measurement correlation, suggesting that ternary nucleation may not be the dominant process in new particle formation. However, the relative bias and error, as well as the correlation at suburban sites, are systematically improved using the heteromolecular nucleation scheme involving sulfuric acid and ELVOCs from monoterpenes. This suggests that heteromolecular nucleation may be important in cities, especially at suburban sites in summer, and that a better characterisation of the emissions of ELVOC precursors from traffic is needed.

Shipborne measurements of nitryl chloride (ClNO2), hydrogen chloride (HCl) and sulphur dioxide (SO2) were made during the AQABA (Air Quality and climate change in the Arabian BAsin) ship campaign in summer 2017. The dataset includes measurements over the Mediterranean Sea, the Suez Canal, the Red Sea, the Gulf of Aden, the Arabian Sea, the Gulf of Oman and the Arabian Gulf (also known as Persian Gulf) with observed ClNO2 mixing ratios ranging from the limit of detection to ≈ 600 pptv. We examined the regional variability in the generation of ClNO2 via the uptake of dinitrogen pentoxide (N2O5) to Cl-containing aerosol and its importance for Cl-atom generation in a marine boundary layer under the (variable) influence of emissions from shipping and oil industry. The yield of ClNO2 formation per NO3 radical generated was generally low (median of ≈ 1–5 % depending on the region), mainly as a result of gas-phase loss of NO3 dominating over heterogeneous loss of N2O5, the latter being disfavoured by the high temperatures found throughout the campaign. The contributions of ClNO2 photolysis and OH-induced HCl oxidation to Cl-radical formation were derived and their relative contributions over the diel cycle compared. The results indicate that over the northern Red Sea, the Gulf of Suez and the Gulf of Oman the formation of Cl-atoms will enhance the oxidation rates of some VOCs, especially in the early morning.

A PM2.5-capable aerosol chemical speciation monitor (ACSM) was deployed in urban Nanjing, China for the first time to measure in-situ non-refractory fine particle (NR-PM2.5) composition from October 20 to November 19, 2015 along with parallel measurements of submicron aerosol (PM1) species by a standard ACSM. Our results show that the NR-PM2.5 species (organics, sulfate, nitrate, and ammonium) measured by the PM2.5-ACSM are highly correlated (r2 > 0.9) with those measured by a Sunset Lab OC/EC Analyzer and a Monitor for AeRosols and GAses (MARGA). The comparisons between the two ACSMs illustrated similar temporal variations in all NR species between PM1 and PM2.5, yet substantial mass fractions of aerosol species were observed in the size range of 1–2.5 μm. On average, NR-PM1–2.5 contributed 53 % of the total NR-PM2.5 with sulfate and secondary organic aerosols (SOA) being the two largest contributors (26 % and 27 %, respectively). Rapid formation and thereafter growth of secondary inorganic aerosols (SIA) were observed under fog processing in NH3-rich environments. Positive matrix factorization of organic aerosol showed similar temporal variations in both primary and secondary OA between PM1 and PM2.5 although the mass spectra were slightly different due to more thermal decomposition on the capture vaporizer of PM2.5-ACSM. We observed an enhancement of SOA under high relative humidity conditions, which is associated with simultaneous increases in particle surface area, gas-phase species (NO2, SO2, and NH3) concentrations and aerosol water content driven by anthropogenic SIA. These results likely indicate an enhanced reactive uptake of SOA precursors upon aqueous particles. Therefore, reducing anthropogenic NOx, SO2, and NH3 emissions might not only reduce SIA but also SOA burden during haze episodes in China.

Ambient particle number size distributions were measured in Paris, France, during summer (1–31 July 2009) and winter (15 January to 15 February 2010) at three fixed ground sites and using two mobile laboratories and one airplane. The campaigns were part of the Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation (MEGAPOLI) project. New particle formation (NPF) was observed only during summer on approximately 50 % of the campaign days, assisted by the low condensation sink (about 10.7 ± 5.9 × 10−3 s−1). NPF events inside the Paris plume were also observed at 600 m altitude onboard an aircraft simultaneously with regional events identified on the ground. Increased particle number concentrations were measured aloft also outside of the Paris plume at the same altitude, and were attributed to NPF. The Paris plume was identified, based on increased particle number and black carbon concentration, up to 200 km away from the Paris center during summer. The number concentration of particles with diameters exceeding 2.5 nm measured on the surface at the Paris center was on average 6.9 ± 8.7 × 104 and 12.1 ± 8.6 × 104 cm−3 during summer and winter, respectively, and was found to decrease exponentially with distance from Paris. However, further than 30 km from the city center, the particle number concentration at the surface was similar during both campaigns. During summer, one suburban site in the NE was not significantly affected by Paris emissions due to higher background number concentrations, while the particle number concentration at the second suburban site in the SW increased by a factor of 3 when it was downwind of Paris.

High uncertainties affect black carbon (BC) emissions, and, despite its important impact on air pollution and climate, very few BC emissions evaluations are found in the literature. This paper presents a novel approach, based on airborne measurements across the Paris, France, plume, developed in order to evaluate BC and NOx emissions at the scale of a whole agglomeration. The methodology consists in integrating, for each transect, across the plume observed and simulated concentrations above background. This allows for several error sources (e.g., representativeness, chemistry, plume lateral dispersion) to be minimized in the model used. The procedure is applied with the CHIMERE chemistry-transport model to three inventories – the EMEP inventory and the so-called TNO and TNO-MP inventories – over the month of July 2009. Various systematic uncertainty sources both in the model (e.g., boundary layer height, vertical mixing, deposition) and in observations (e.g., BC nature) are discussed and quantified, notably through sensitivity tests. Large uncertainty values are determined in our results, which limits the usefulness of the method to rather strongly erroneous emission inventories. A statistically significant (but moderate) overestimation is obtained for the TNO BC emissions and the EMEP and TNO-MP NOx emissions, as well as for the BC / NOx emission ratio in TNO-MP. The benefit of the airborne approach is discussed through a comparison with the BC / NOx ratio at a ground site in Paris, which additionally suggests a spatially heterogeneous error in BC emissions over the agglomeration.

Online non-refractory submicron aerosol mass spectrometer (AMS) measurements in urban areas have successfully allowed the apportionment of specific sources and/or physical and chemical properties of the organic fraction. However, in order to be fully representative of PM pollution, a comprehensive source apportionment analysis is needed by taking into account all major components of submicron aerosols, creating strengthened bonds between the organic components and pollution sources. We present here a novel two-step methodology to perform such an analysis, by taking advantage of high time resolution of monitoring instruments: the aerosol chemical speciation monitor (ACSM) and the multi-wavelength absorption measurements (Aethalometer AE31) in Paris, France. As a first step, organic aerosols (OA) were deconvolved to hydrocarbon-like OA (HOA), biomass burning OA (BBOA) and oxygenated OA (OOA) with positive matrix factorization (PMF), and black carbon was deconvolved into its wood burning and fossil fuel combustion fractions. A second PMF analysis was then carried out with organic factors, BC fractions and inorganic species (nitrate, sulfate, ammonium, chloride), leading to a four-factor solution allowing highly time-resolved characterization of the major sources of PM1. Outputs of this PMF2 include two dominant combustion sources (wood burning and traffic) as well as semi-volatile and low-volatile secondary aerosols. While HOA is found to be emitted by both wood burning and traffic, the latter sources occurred to significantly contribute also to OOA.

During an intensive field campaign on aerosol, clouds, and ice nucleation in the Eastern Mediterranean in April 2016, we measured the abundance of ice nucleating particles (INPs) in the lower troposphere from unmanned aircraft systems (UASs). Aerosol samples were collected by miniaturized electrostatic precipitators onboard the UASs at altitudes up to 2.5 km. The number of INPs in these samples, which are active in the deposition and condensation modes at temperatures from −20 to −30 °C, were analyzed immediately after collection on site using the ice nucleus counter FRIDGE (FRankfurt Ice nucleation Deposition freezinG Experiment). During the 1-month campaign, we encountered a series of Saharan dust plumes that traveled at several kilometers' altitude. Here we present INP data from 42 individual flights, together with aerosol number concentrations, observations of lidar backscattering, dust concentrations derived by the dust transport model DREAM (Dust Regional Atmospheric Model), and results from scanning electron microscopy. The effect of the dust plumes is reflected by the coincidence of INPs with the particulate matter (PM), the lidar signal, and the predicted dust mass of the model. This suggests that mineral dust or a constituent related to dust was a major contributor to the ice nucleating properties of the aerosol. Peak concentrations of above 100 INPs std L−1 were measured at −30 °C. The INP concentration in elevated plumes was on average a factor of 10 higher than at ground level. Since desert dust is transported for long distances over wide areas of the globe predominantly at several kilometers' altitude, we conclude that INP measurements at ground level may be of limited significance for the situation at the level of cloud formation.

Hourly concentrations of inorganic salts (ions) and carbonaceous material in fine aerosols (aerodynamic diameter, A.D. 2.5). This time-resolved dataset allowed investigating the factors controlling the levels of PM2.5 in Paris and showed that polluted periods with PM2.5 > 15 μg m−3 were characterized by air masses of continental (North-Western Europe) origin and chemical composition made by 75% of ions. By contrast, periods with clean marine air masses have shown the lowest PM2.5 concentrations (typically of about 10 μg m−3); carbonaceous aerosols contributing for most of this mass (typically 75%). In order to better discriminate between local and continental contributions to the observed chemical composition and concentrations of PM2.5 over Paris, a comparative study was performed between this time-resolved dataset and the outputs of a chemistry transport model (CHIMERE), showing a relatively good capability of the model to reproduce the time-limited intense maxima observed in the field for PM2.5 and ion species. Different model scenarios were then investigated switching off local and European (North-Western and Central) emissions. Results of these scenarios have clearly shown that most of the ions observed over Paris during polluted periods, were either transported or formed in-situ from gas precursors transported from Northern Europe. On the opposite, long-range transport from Europe appeared to weakly contribute to the levels of carbonaceous aerosols observed over Paris. The model failed to properly account for the concentration levels and variability of secondary organic aerosols (SOA) determined experimentally by the EC-tracer method. The abundance of SOA (relatively to organic aerosol, OA) was as much as 75%, showing a weak dependence on air masses origin. Elevated SOA/OA ratios were also observed for air masses having residence time above ground of less than 10 h, suggesting intense emissions and/or photochemical processes leading to rapid formation of secondary organic aerosols.

PAR00002853; International audience; The global sulphur cycle has been simulated using a general circulation model with a focus on the source and oxidation of atmospheric dimethylsulphide (DMS). The sensitivity of atmospheric DMS to the oceanic DMS climatology, the parameterisation of the sea-air transfer and to the oxidant fields have been studied. The importance of additional oxidation pathways (by O3 in the gas- and aqueous-phases and by BrO in the gas phase) not incorporated in global models has also been evaluated. While three different climatologies of the oceanic DMS concentration produce rather similar global DMS fluxes to the atmosphere at 24-27 Tg S yr -1, there are large differences in the spatial and seasonal distribution. The relative contributions of OH and NO3 radicals to DMS oxidation depends critically on which oxidant fields are prescribed in the model. Oxidation by O3 appears to be significant at high latitudes in both hemispheres. Oxidation by BrO could be significant even for BrO concentrations at sub-pptv levels in the marine boundary layer. The impact of such refinements on the DMS chemistry onto the indirect radiative forcing by anthropogenic sulphate aerosols is also discussed.