The BLLAST field experiment: Boundary-Layer late afternoon and sunset turbulence

Due to the major role of the sun in heating the earth's surface, the atmospheric planetary boundary layer over land is inherently marked by a diurnal cycle. The afternoon transition, the period of the day that connects the daytime dry convective boundary layer to the night-time stable boundary layer, still has a number of unanswered scientific questions. This phase of the diurnal cycle is challenging from both modelling and observational perspectives: it is transitory, most of the forcings are small or null and the turbulence regime changes from fully convective, close to homogeneous and isotropic, toward a more heterogeneous and intermittent state. These issues motivated the BLLAST (Boundary-Layer Late Afternoon and Sunset Turbulence) field campaign that was conducted from 14 June to 8 July 2011 in southern France, in an area of complex and heterogeneous terrain. A wide range of instrumented platforms including full-size aircraft, remotely piloted aircraft systems, remote-sensing instruments, radiosoundings, tethered balloons, surface flux stations and various meteorological towers were deployed over different surface types. The boundary layer, from the earth's surface to the free troposphere, was probed during the entire day, with a focus and intense observation periods that were conducted from midday until sunset. The BLLAST field campaign also provided an opportunity to test innovative measurement systems, such as new miniaturized sensors, and a new technique for frequent radiosoundings of the low troposphere. Twelve fair weather days displaying various meteorological conditions were extensively documented during the field experiment. The boundary-layer growth varied from one day to another depending on many contributions including stability, advection, subsidence, the state of the previous day's residual layer, as well as local, meso- or synoptic scale conditions. Ground-based measurements combined with tethered-balloon and airborne observations captured the turbulence decay from the surface throughout the whole boundary layer and documented the evolution of the turbulence characteristic length scales during the transition period. Closely integrated with the field experiment, numerical studies are now underway with a complete hierarchy of models to support the data interpretation and improve the model representations.publishedVersio

Mixing state of aerosols and direct observation of carbonaceous and marine coatings on African dust by individual particle analysis

The mixing state of aerosols collected at M'Bour, Senegal, during the Special Observing Period conducted in January–February 2006 (SOP-0) of the African Monsoon Multidisciplinary Analysis project (AMMA), was studied by individual particle analysis. The sampling location on the Atlantic coast is particularly adapted for studying the mixing state of tropospheric aerosols since it is (1) located on the path of Saharan dust plumes transported westward over the northern tropical Atlantic, (2) influenced by biomass burning events particularly frequent from December to March, and (3) strongly influenced by anthropogenic emissions from polluted African cities. Particle size, morphology, and chemical composition were determined for 12,672 particles using scanning electron microscopy (automated SEM-EDX). Complementary analyses were performed using transmission electron microscopy combined with electron energy loss spectrometry (TEM-EELS) and Raman microspectrometry. Mineral dust and carbonaceous and marine compounds were predominantly found externally mixed, i.e., not present together in the same particles. Binary internally mixed particles, i.e., dust/carbonaceous, carbonaceous/marine, and dust/marine mixtures, accounted for a significant fraction of analyzed particles (from 10.5% to 46.5%). Western Sahara was identified as the main source of mineral dust. Two major types of carbonaceous particles were identified: “tar balls” probably coming from biomass burning emissions and soot from anthropogenic emissions. Regarding binary internally mixed particles, marine and carbonaceous compounds generally formed a coating on mineral dust particles. The carbonaceous coating observed at the particle scale on African dust was evidenced by the combined use of elemental and molecular microanalysis techniques, with the identification of an amorphous rather than crystallized carbon structure

Atmospheric reactivity of hydroxyl radicals with guaiacol (2-methoxyphenol), a biomass burning emitted compound: Secondary organic aerosol formation and gas-phase oxidation products

Methoxyphenols are low molecular weight semi-volatile polar aromatic compounds produced from the pyrolysis of wood lignin. The reaction of guaiacol (2-methoxyphenol) with hydroxyl radicals has been studied in the LPCA simulation chamber at (294±2) K, atmospheric pressure, low relative humidity (RHx conditions using CH3ONO as OH source. The aerosol production was monitored using a SMPS (Scanning Mobility Particle Sizer); the SOA yields were in the range from 0.003 to 0.87 and the organic aerosol formation can be expressed by a one-product gas/particle partitioning absorption model. Transmission (TEM) and Scanning (SEM) Electron Microscopy observations were performed to characterize the physical state of SOA produced from the OH reaction with guaiacol; they display both liquid and solid particles (in an amorphous state).GC-FID (Gas Chromatography - Flame Ionization Detection) and GC-MS (Gas Chromatography - Mass Spectrometry) analysis show the formation of nitroguaiacol isomers as main oxidation products in the gas- and aerosol-phases. In the gas-phase, the formation yields were (10±2) % for 4-nitroguaiacol (1-hydroxy-2-methoxy-4-nitrobenzene; 4-NG) and (6±2) % for 3- or 6-nitroguaiacol (1-hydroxy-2-methoxy-3-nitrobenzene or 1-hydroxy-2-methoxy-6-nitrobenzene; 3/6-NG; the standards are not commercially available so both isomers cannot be distinguished) whereas in SOA their yield were much lower (≤0.1%).To our knowledge, this work represents the first identification of nitroguaiacols as gaseous oxidation products of the OH reaction with guaiacol. As the reactivity of nitroguaiacols with atmospheric oxidants is probably low, we suggest using them as biomass burning emission gas tracers. The atmospheric implications of the guaiacol+OH reaction are also discussed

Laboratory study of iron isotope fractionation during dissolution of mineral dust and industrial ash in simulated cloud water

Atmospheric deposition is a key mode of iron (Fe) input to ocean regions where low concentrations of this micronutrient limit marine primary production. Various natural particles (e.g. mineral dust, volcanic ash) and anthropogenic particles (e.g. from industrial processes, biomass burning) can deliver Fe to the ocean, and assessment of their relative importance in supplying Fe to seawater requires knowledge of both their deposition flux and their Fe solubility (a proxy for Fe bioavailability). Iron isotope (54Fe, 56Fe, 57Fe, 58Fe) analysis is a potential tool for tracing natural and anthropogenic Fe inputs to the ocean. However, it remains uncertain how the distinct Fe isotopic signatures (δ56Fe) of these particles may be modified by physicochemical processes (e.g. acidification, photochemistry, condensation-evaporation cycles) that are known to enhance Fe solubility during atmospheric transport. In this experimental study, we measure changes over time in both Fe solubility and δ56Fe of a Tunisian soil dust and an Fe–Mn alloy factory industrial ash exposed under irradiation to a pH 2 solution containing oxalic acid, the most widespread organic complexing agent in cloud- and rainwater. The Fe released per unit surface area of the ash (∼1460 μg Fe m−2) is ∼40 times higher than that released by the dust after 60 min in solution. Isotopic fractionation is also observed, to a greater extent in the dust than the ash, in parallel with dissolution of the solid particles and driven by preferential release of 54Fe into solution. After the initial release of 54Fe, the re-adsorption of A-type Fe-oxalate ternary complexes on the most stable surface sites of the solid particles seems to impair the release of the heavier Fe isotopes, maintaining a relative enrichment in the light Fe isotope in solution over time. These findings provide new insights on Fe mobilisation and isotopic fractionation in mineral dust and industrial ash during atmospheric processing, with potential implications for ultimately improving the tracing of natural versus anthropogenic contributions of soluble Fe to the ocean.SCOPUS: ar.jinfo:eu-repo/semantics/publishe

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