An off‐line global three‐dimensional tracer model based on analyzed wind fields was augmented to simulate the atmospheric transport of mineral dust. The model describes the evolution of the aerosol size distribution and hence allows to compute aerosol number and mass concentrations. In this study we describe the parameterization of the sedimentation process and include a preliminary source formulation but exclude wet deposition. Validation of the model is done during a 16‐day period in June‐July 1988 with very scarce precipitation. It is based on a comparison of every model grid box with daily satellite‐derived optical thickness observations of Saharan dust plumes over the North Atlantic and the Mediterranean. The model reproduces accurately the daily position of the dust plumes over the ocean, with the exception of Atlantic regions remote from the African coast. By systematic analysis of transport and aerosol components we show that the largest uncertainty in reproducing the position of the dust clouds is the correct localization of the source regions. The model simulation is also very sensitive to the inclusion of convection and to an accurate treatment of the sedimentation process. Only the combination of source activation, rapid transport of dust to higher altitudes by convective updraft and long‐range transport allows the simulation of the dust plumes position. This study shows that a mineral dust transport model is only constrained if both the source strength and the aerosol size distribution are known. The satellite observation of optical thickness over the Mediterranean and assumptions about the size distribution indicate that the dust emission flux was of the order of 17×10 6 t for the 16‐day period under investigation. The simulations suggest that a major aerosol mode initially around 2.5 μm with a standard deviation of 2.0 plays the dominant role in long‐range transport of mineral dust.
Abstract. Since the 1970s, the French space agency CNES has developed boundary-layer pressurized balloons (BLPBs) with the capability to transport lightweight scientific payloads at isopycnic level and offer a quasi-Lagrangian sampling of the lower atmosphere over very long distances and durations (up to several weeks). Electrochemical concentration cell (ECC) ozonesondes are widely used under small sounding balloons. However, their autonomy is limited to few hours owing to power consumption and electrolyte evaporation. An adaptation of the ECC sonde has been developed specifically for long-duration BLPB flights. Compared to conventional ECC sondes, the main feature is the possibility of programming periodic measurement sequences (with possible remote control during the flight). To increase the ozonesonde autonomy, the strategy has been adopted of short measurement sequences (2–3 min) regularly spaced in time (e.g., every 15 min). The rest of the time, the sonde pump is turned off. Results of preliminary ground-based tests are first presented. In particular, the sonde was able to provide correct ozone concentrations against a reference UV-absorption ozone analyzer for 4 days on a 15-min time base. Then we illustrate results from 16 BLBP flights launched over the western Mediterranean during three summer field cam- paigns of the ChArMEx project ( http://charmex.lsce.ipsl.fr): TRAQA in 2012 and ADRIMED and SAFMED in 2013. BLPB drifting altitudes were in the range 0.25–3.2 km. The longest flight lasted more than 32 hours and covered more than 1000 km. Satisfactory data were obtained when compared to independent ozone measurements close in space and time. The quasiLagrangian measurements allowed a first look at ozone diurnal evolution in the marine boundary layer as well as in the lower free troposphere. During some flight segments, there was indication of photochemical ozone production in the marine boundary layer or even in the free troposphere, at rates ranging from 1 to 2 ppbv h−1.
Abstract. This study reports the only recent characterization of two contrasted wet deposition events collected during the PEACETIME (ProcEss studies at the Air–sEa Interface after dust deposition in the MEditerranean Sea) cruise in the open Mediterranean Sea (Med Sea) and their impact on trace metal (TM) marine stocks. Rain samples were analysed for Al, 12 TMs (Co, Cd, Cr, Cu, Fe, Mn, Mo, Ni, Pb, Ti, V and Zn) and nutrient (N, P, dissolved organic carbon) concentrations. The first rain sample collected in the Ionian Sea (Rain ION) was a typical regional background wet deposition event, whereas the second rain sample collected in the Algerian Basin (Rain FAST) was a Saharan dust wet deposition event. Even in the remote Med Sea, all background TM inputs presented an anthropogenic signature, except for Fe, Mn and Ti. The concentrations of TMs in the two rain samples were significantly lower compared to concentrations in rains collected at coastal sites reported in the literature, due to the decrease in anthropogenic emissions during the preceding decades. The atmospheric TM inputs were mainly dissolved forms, even in dusty Rain FAST. The TM stocks in the mixed layer (ML, 0–20 m) at the FAST station before and after the event showed that the atmospheric inputs were a significant supply of particulate TMs and dissolved Fe and Co for surface seawater. Even if the wet deposition delivers TMs mainly in soluble form, the post-deposition aerosol dissolution could to be a key additional pathway in the supply of dissolved TMs. At the scale of the western and central Mediterranean, the atmospheric inputs were of the same order of magnitude as ML stocks for dissolved Fe, Co and Zn, highlighting the role of the atmosphere in their biogeochemical cycles in the stratified Med Sea. In case of intense dust-rich wet deposition events, the role of atmospheric inputs as an external source was extended to dissolved Co, Fe, Mn, Pb and Zn. Our results suggest that the wet deposition constitutes only a source of some of dissolved TMs for Med Sea surface waters. The contribution of dry deposition to the atmospheric TM inputs needs to be investigated.
The mass of African dust present over the western Mediterranean during a transport episode from northwestern Africa, which occurred in early July 1985, is estimated using a desert aerosol model, an Earth‐atmosphere radiative transfer model and Meteosat visible channel data from 4 days running. Dust pixels are selected from Meteosat images, and their aerosol optical thickness is retrieved. A proportionality factor between aerosol optical thickness and atmospheric columnar aerosol loading is computed and applied to the dust pixels. The total mass of atmospheric particles over the basin is obtained by interpolation and spatial integration. The maximum aerosol optical thickness is 1.8. The maximum aerosol columnar loading is evaluated to be 2.3 g m −2 . The integrated mass of particles present at a given time is estimated to raise up to about 0.6 × 10 12 g at the maximum and the total mass of dust exported from Africa to be of the order of 10 12 g. The method is carefully evaluated and uncertainties are discussed, with particular emphasis on the relationship between atmospheric dust mass and aerosol optical depth. The overall uncertainty on the total mass is roughly a factor ±3. In the absence of clouds it appears that the major uncertainty results from the lack of knowledge of the actual mass‐size distribution of suspended dust particles, pointing out the lack of relevant data on particles larger than 10 μm in diameter. A simple calculation based on results from both computations and simultaneous field measurements yields a net transfer velocity of particles from the dust layer of approximately 1 cm s −1 .
Abstract. We used phosphate deposition from natural dust, anthropogenic combustion and wildfires simulated for the year 2005 by a global atmospheric chemical transport model (LMDz–INCA) as additional sources of external nutrient for a high resolution regional coupled dynamical–biogeochemical model of the Mediterranean Sea. In general, dust is considered as 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 (the bioavailable form of phosphorus in seawater) for the Mediterranean Sea. According to the atmospheric transport model, anthropogenic phosphate deposition from combustion (Pcomb) brings on average 40.5 10−6 mol PO4 m−2 year−1 over the entire Mediterranean Sea for the year 2005 and is the primary source over the northern part (101 10−6 mol PO4 m−2 year−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 year−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 (31.8 10−6 mol PO4 m−2 year−1 from dust deposited in 2005 on average over the South Ionian basin against 12.4 10−6 from combustion). We examine separately the different soluble phosphorus (PO4) sources and their respective fluxes variability and evaluate their impacts on marine surface biogeochemistry (phosphate concentrations, Chl 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. The impact of the different sources of phosphate on the biogeochemical cycles is remarkably different and should be accounted for in modeling studies.
Abstract. Organic aerosols are measured at a remote site (Ersa) on Corsica Cape in the northwestern Mediterranean basin during the Chemistry-Aerosol Mediterranean Experiment (CharMEx) winter campaign of 2014, when high organic concentrations from anthropogenic origin are observed. This work aims at representing the observed organic aerosol concentrations and properties (oxidation state) using the air-quality model Polyphemus with a surrogate approach for secondary organic aerosol (SOA) formation. Because intermediate/semi-volatile organic compounds (I/S-VOC) are the main precursors of SOA at Ersa during the winter 2014, different parameterizations to represent the emission and ageing of I/S-VOC were implemented in the chemistry-transport model of the air-quality platform Polyphemus (different volatility distribution emissions, single-step oxidation vs multi-step oxidation within a Volatility Basis Set framework, inclusion of non-traditional volatile organic compounds NTVOC). Simulations using the different parameterizations are compared to each other and to the measurements (concentration and oxidation state). The high observed organic concentrations are well reproduced whatever the parameterizations. They are slightly under-estimated with most parameterizations, but they are slightly over-estimated when the ageing of NTVOC is taken into account. The volatility distribution at emissions influences more strongly the concentrations than the choice of the parameterization that may be used for ageing (single-step oxidation vs multi-step oxidation), stressing the importance of an accurate characterization of emissions. Assuming the volatility distribution of sectors other than residential heating to be the same as residential heating may lead to a strong under-estimation of organic concentrations. The observed organic oxidation and oxygenation states are strongly under-estimated in all simulations, even when a recently developed parameterization for modeling the ageing of I/S-VOC from residential heating is used. This suggests that uncertainties in the ageing of I/S-VOC emissions remain to be elucidated, with a potential role of organic nitrate from anthropogenic precursors and highly oxygenated organic molecules.
Abstract. In the framework of ChArMEx (the Chemistry-Aerosol Mediterranean Experiment), the air quality model Polyphemus is used to understand the sources of inorganic and organic particles in the western Mediterranean and evaluate the uncertainties linked to the model parameters (meteorological fields, anthropogenic and sea-salt emissions and hypotheses related to the model representation of condensation/evaporation). The model is evaluated by comparisons to in situ aerosol measurements performed during three consecutive summers (2012, 2013 and 2014). The model-to-measurement comparisons concern the concentrations of PM10, PM1, organic matter in PM1 (OM1) and inorganic aerosol concentrations monitored at a remote site (Ersa) on Corsica Island, as well as airborne measurements performed above the western Mediterranean Sea. Organic particles are mostly from biogenic origin. The model parameterization of sea-salt emissions has been shown to strongly influence the concentrations of all particulate species (PM10, PM1, OM1 and inorganic concentrations). Although the emission of organic matter by the sea has been shown to be low, organic concentrations are influenced by sea-salt emissions; this is owing to the fact that they provide a mass onto which gaseous hydrophilic organic compounds can condense. PM10, PM1, OM1 are also very sensitive to meteorology, which affects not only the transport of pollutants but also natural emissions (biogenic and sea salt). To avoid large and unrealistic sea-salt concentrations, a parameterization with an adequate wind speed power law is chosen. Sulfate is shown to be strongly influenced by anthropogenic (ship) emissions. PM10, PM1, OM1 and sulfate concentrations are better described using the emission inventory with the best spatial description of ship emissions (EDGAR-HTAP). However, this is not true for nitrate, ammonium and chloride concentrations, which are very dependent on the hypotheses used in the model regarding condensation/evaporation. Model simulations show that sea-salt aerosols above the sea are not mixed with background transported aerosols. Taking the mixing state of particles with a dynamic approach to condensation/evaporation into account may be necessary to accurately represent inorganic aerosol concentrations.
