The impact of aerosols on stratiform clouds over southern West Africa: a large-eddy-simulation study

Low-level stratiform clouds (LLSCs) covering a large area appear frequently during the wet monsoon season in southern West Africa. This region is also a place where different types of aerosols coexist, including biomass burning aerosols coming from central and southern Africa and aerosols emitted by local anthropogenic activities. We investigate the indirect and semi-direct effects of these aerosols on the life cycle of LLSCs by conducting a case study based on airborne and ground-based observations from the field campaign of Dynamic-Aerosol-Chemistry-Cloud-Interaction in West Africa (DACCIWA). This case is modeled using a large-eddy-simulation (LES) model with fine resolution and in situ aerosol measurements, including size distribution and chemical composition. The model has successfully reproduced the observed life cycle of the LLSC, from stratus formation to stabilization during the night and to upward development after sunrise until break-up of the cloud deck in the late afternoon. Additional sensitivity simulations using different measured aerosol profiles also suggest that aerosols can affect the cloud life cycle through both the indirect and semi-direct effects. As expected, modeled cloud microphysical features, including cloud droplet number concentration, mean radius, and thus cloud reflectivity, are all controlled by aerosol concentration. However, it is found that the variation in cloud reflectivity induced by different aerosol profiles is not always the only factor in determining the incoming solar radiation at the ground and thus for the cloud life cycle after sunrise. Instead, the difference in cloud fraction brought by dry-air entrainment from above and thus the speed of consequent evaporation – also influenced by aerosol concentration – is another important factor to consider. Clouds influenced by higher aerosol concentrations and thus with a higher number concentration and smaller sizes of cloud droplets are found to evaporate more easily and thus impose a lower cloud fraction. In addition, our sensitivity runs including versus excluding aerosol direct radiative effects have also demonstrated the impacts specifically of solar absorption by black carbon on the cloud life cycle. The semi-direct effect resulting from an excessive atmospheric heating of up to 12 K d−1 by black carbon in our modeled cases is found to lower the cloud top as well as the liquid water path, reducing surface incoming solar radiation and dry entrainment and increasing the cloud fraction.</p

DEVELOPMENT AND VALIDATION OF A METHOD FOR THE LC DETERMINATION p-[18F]MPPF IN PLASMA USING A MISPE

Peer reviewe

Assessing the role of anthropogenic and biogenic sources on PM₁ over southern West Africa using aircraft measurements

As part of the Dynamics-Aerosol-Chemistry-Cloud Interactions in West Africa (DACCIWA) project, an airborne campaign was designed to measure a large range of atmospheric constituents, focusing on the effect of anthropogenic emissions on regional climate. The presented study details results of the French ATR42 research aircraft, which aimed to characterize gas-phase, aerosol and cloud properties in the region during the field campaign carried out in June/July 2016 in combination with the German Falcon 20 and the British Twin Otter aircraft. The aircraft flight paths covered large areas of Benin, Togo, Ghana and Côte d\u27Ivoire, focusing on emissions from large urban conurbations such as Abidjan, Accra and Lomé, as well as remote continental areas and the Gulf of Guinea. This paper focuses on aerosol particle measurements within the boundary layer (<  2000 m), in particular their sources and chemical composition in view of the complex mix of both biogenic and anthropogenic emissions, based on measurements from a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS) and ancillary instrumentation. Background concentrations (i.e. outside urban plumes) observed from the ATR42 indicate a fairly polluted region during the time of the campaign, with average concentrations of carbon monoxide of 131 ppb, ozone of 32 ppb, and aerosol particle number concentration ( >  15 nm) of 735 cm−3 stp. Regarding submicron aerosol composition (considering non-refractory species and black carbon, BC), organic aerosol (OA) is the most abundant species contributing 53 %, followed by SO4 (27 %), NH4 (11 %), BC (6 %), NO3 (2 %) and minor contribution of Cl (<  0.5 %). Average background PM1 in the region was 5.9 µg m−3 stp. During measurements of urban pollution plumes, mainly focusing on the outflow of Abidjan, Accra and Lomé, pollutants are significantly enhanced (e.g. average concentration of CO of 176 ppb, and aerosol particle number concentration of 6500 cm−3 stp), as well as PM1 concentration (11.9 µg m−3 stp). Two classes of organic aerosols were estimated based on C-ToF-AMS: particulate organic nitrates (pONs) and isoprene epoxydiols secondary organic aerosols (IEPOX–SOA). Both classes are usually associated with the formation of particulate matter through complex interactions of anthropogenic and biogenic sources. During DACCIWA, pONs have a fairly small contribution to OA (around 5 %) and are more associated with long-range transport from central Africa than local formation. Conversely, IEPOX–SOA provides a significant contribution to OA (around 24 and 28 % under background and in-plume conditions). Furthermore, the fractional contribution of IEPOX–SOA is largely unaffected by changes in the aerosol composition (particularly the SO4 concentration), which suggests that IEPOX–SOA concentration is mainly driven by pre-existing aerosol surface, instead of aerosol chemical properties. At times of large in-plume SO4 enhancements (above 5 µg m−3), the fractional contribution of IEPOX–SOA to OA increases above 50 %, suggesting only then a change in the IEPOX–SOA-controlling mechanism. It is important to note that IEPOX–SOA constitutes a lower limit to the contribution of biogenic OA, given that other processes (e.g. non-IEPOX isoprene, monoterpene SOA) are likely in the region. Given the significant contribution to aerosol concentration, it is crucial that such complex biogenic–anthropogenic interactions are taken into account in both present-day and future scenario models of this fast-changing, highly sensitive region

Aerosol influences on low-level clouds in the West African monsoon

Low-level clouds (LLC) cover a wide area of southern West Africa (SWA) during the summer monsoon months, and have an important cooling effect on the regional climate. Previous studies of these clouds have focused on modelling and remote sensing via satellite. We present the first comprehensive set of regional, in situ measurements of cloud microphysics, taken during June – July 2016, as part of the DACCIWA (Dynamics-Aerosol-Chemistry-Clouds Interactions in West Africa) campaign, assessing spatial and temporal variation in the properties of these clouds. LLC developed overnight and mean cloud cover peaked a few hundred kilometres inland around 10:00 local solar time (LST), before clouds began to dissipate and convection intensified in the afternoon. Additional sea breeze clouds developed near the coast in the late morning, reaching a maximum extent around 12:00 LST. Regional variation in LLC cover was largely determined by the modulation of the cool maritime inflow by the local orography, with peaks on the upwind side of hills and minima on the leeward sides. In the broad-scale cloud field, no lasting impacts related to anthropogenic aerosol were observed downwind of major population centres. The boundary layer cloud drop number concentration (CDNC) was locally variable inland, ranging from 200 to 840 cm−3 (10th and 90th percentiles at standard temperature and pressure), but showed no systematic regional variations. Enhancements were seen in pollution plumes from the coastal cities, but were not statistically significant across the region. The majority of accumulation mode aerosols, and therefore cloud condensation nuclei, were from ubiquitous biomass burning smoke transported from the southern hemisphere. Consequently, all clouds measured (inland and offshore) had significantly higher CDNC and lower effective radius than clouds over the remote south Atlantic from literature. A parcel model sensitivity analysis showed that doubling or halving local emissions only changed the calculated CDNC by 13–22 %, as the high background meant local emissions were a small fraction of total aerosol. As the population of SWA grows, local emissions are expected to rise. Biomass burning smoke transported from the southern hemisphere is likely to dampen any effect of these increased local emissions on cloud-aerosol interactions. An integrative analysis between local pollution and Central African biomass burning emissions must be considered when predicting anthropogenic impacts on the regional cloud field during the West African monsoon

Aerosol Hygroscopicity

International audienceThe hygroscopic and ice nucleation properties play a vital role for the direct and indirect effects of aerosols on climate by determining the interactions of aerosol particles with atmospheric water vapour, ice and cloud microphysical processes. This chapter reviews the existing published results on the aerosol hygroscopic properties at subsaturated (relative humidity below 100%) and supersaturated (relative humidity above 100%) conditions, and on the ice nucleation properties of aerosols from measurements at multiple sites in the Mediterranean. Rapid progress has been made in the last 20 years in understanding how different chemical and physical properties affect the aerosol hygroscopic growth. Some early investigations have yielded comprehensive information regarding the main sources and chemical composition of the atmospheric cloud condensation nuclei (CCN) and ice-nucleating particles (INP) in the Mediterranean region. Despite these advances, process-level understanding of aerosol hygroscopic properties and related ice nucleation remains insufficient, causing unacceptably large uncertainties when simulating aerosol radiative effects in future climate projections

Optical and hygroscopic properties of secondary organic aerosols produced from ozonolysis of α-pinène in a smog chamber

La connaissance de l'impact des aérosols sur le climat, au cours de leur cycle de vie, est aujourd'hui un enjeu majeur de la communauté scientifique. En particulier, les aérosols organiques secondaires (AOS) constituent une part importante de la fraction fine des aérosols et pourtant leurs propriétés optiques et hygroscopiques présentent encore des fortes incertitudes. Cette étude avait pour objectif de comprendre et d'évaluer l'évolution des propriétés optiques et hygroscopiques de l'AOS produit dans la chambre de simulation atmosphérique CESAM à partir de l'ozonolyse de l'α-pinène au cours de sa formation et de son vieillissement dans l'atmosphère. Afin de mener à bien ce projet, un HTDMA a été développé et validé. Cette approche a été complétée en mesurant les propriétés hygroscopiques de l'ensemble de la population polydispersé d'aérosols par humidification au sein de la chambre de simulation. Afin de mettre en évidence des modifications de propriétés optiques, l'évolution temporelle de l'indice complexe de réfraction a été déterminée. La méthodologie a été validée et l'effet du temps de contact des particules avec la vapeur d'eau a été investigué. Cette méthodologie a ensuite été appliquée à l'étude des propriétés optiques et hygroscopiques de l'AOS généré par ozonolyse de l'α-pinène au cours de sa formation et du vieillissement par différents processus: dans le noir, en présence d'un excès d'ozone et par photolyse. Les liens avec des modifications possibles de la composition chimique ont été investigués par des observations et par modélisationThe impact of aerosols on climate represents a major challenge in atmospheric science. This is particularly true for secondary organic aerosols, representing a major fraction of the fine aerosols. However, their optical and hygroscopic properties are poorly understood. The present work investigates the optical and hygroscopic properties of SOA generated from the ozonolysis of α-pinene at first and after having undergone atmospheric ageing reactions using the laboratory smog chamber CESAM. For that purpose, an HTDMA has been built and a new approach has been developed to measure hygroscopic properties of polydispersed aerosols by humidifying them directly in the smog chamber. The refractive index has been calculated to investigate the optical properties changes. The methodology has been validated and the residence time of particles with water vapor has been investigated. Then, it has been applied to study the optical and hygroscopic properties of α-pinene SOA during its formation and during ageing by various processes: reaction in the dark, with ozone, and photolysis. The link with changes in the composition has been investigated by measurements and modelin

Experimental study on the evolution of droplet size distribution during the fog life cycle

International audienceThe evolution of the droplet size distribution (DSD) during the fog life cycle remains poorly understood and progress is required to reduce the uncertainty of fog forecasts. To gain insights into the physical processes driving the microphysical properties, intensive field campaigns were conducted during the winters of 2010-2013 at the Instrumented Site for Atmospheric Remote Sensing Research (SIRTA) in a semi-urban environment southwest of Paris city center to monitor the simultaneous variations in droplet microphysical properties and their potential interactions at the different evolutionary stages of the fog events. Liquid water content (LWC), fog droplet number concentration (N d) and effective diameter (D eff) show large variations among the 42 fog events observed during the campaign and for individual events. Our findings indicate that the variability of these parameters results from the interaction between microphysical, dynamical and radiative processes. During the formation and development phases, activation of aerosols into fog droplets and condensational growth were the dominant processes. When vertical development of radiation fog occurred under the influence of increasing wind speed and subsequent turbulent motion, additional condensational growth of fog droplets was observed. The DSDs with single mode (around 11 µm) and double mode (around 11 and 22 µm) were observed during the field campaign. During the development phase of fog with two droplet size modes, a mass transfer occurred from the smaller droplets into the larger ones through collision-coalescence or Ostwald ripening processes. During the mature phase, evaporation due to surface warming induced by infrared radiation emitted by fog was the dominant process. Additional droplet removal through sedimentation is observed during this phase for fog with two droplet size modes. Because of differences in the physical processes involved, the relationship between LWC and N d is largely driven by the DSD. Although a positive relationship is found in most of the events due to continuous activation of aerosol into fog droplets, LWC varies at a constant N d in fog with large D eff (> 17 µm) due to additional collision-coalescence and Ostwald ripening processes. This work illustrates the need to accurately estimate the supersaturation for simulating the continuous activation of aerosols into droplets during the fog life cycle and to include advanced parameterizations of relevant microphysical processes such as collision-coalescence and Ostwald ripening processes, among others, in numerical models

Aerosol-cloud interactions and impact on regional climate

International audienceAerosols interact with clouds through radiative and microphysical mechanisms in addition to their direct radiative effects of scattering and absorbing of solar and thermal radiation. Aerosol indirect effects consist of the modification of cloud droplet number concentrations, cloud albedo, and ice nucleating particle concentrations with ensuing effects on precipitation through aerosol perturbations. Different aerosol types present over the basin, notably dust, sea-salt and anthropogenic contribute to the formation of cloud condensation and ice nucleating particles, thus modifying cloud parameters. These processes notably occur during the frequent dust outbreaks over the Mediterranean Sea. Besides, the semi-direct aerosol effect, namely changes in cloud cover and atmospheric dynamics due to aerosol absorption, is another impact on regional climate. Regional climate simulations including aerosol-cloud interactions highlight the importance of considering aerosols, even if uncertainties are still important notably with regards to effects on cloud microphysics. To date, the direct and semi-direct effects seem to have larger impacts on the average radiative budget over the Mediterranean than the cloud-albedo indirect effect, but the question remains open concerning other indirect effects. Therefore, more observations of these interactions coupled with numerical simulations considering all these processes are needed to reduce uncertainties