The time series of total, fine and coarse POLAC/PARASOL aerosol optical depth (AOD) satellite products (2005–2013) processed by the POLAC algorithm are examined to investigate the transport of ...aerosols over the North Tropical Atlantic Ocean, a region that is characterized by significant dust aerosols events. First, the comparison of satellite observations with ground-based measurements acquired by AERONET ground-based measurements shows a satisfactory consistency for both total AOD and coarse mode AOD (i.e., correlation coefficients of 0.75 and bias ranging from −0.03 to 0.03), thus confirming the robustness and performance of POLAC/PARASOL data to investigate the spatio-temporal variability of the aerosols over the study area. Regarding fine mode aerosol, POLAC/PARASOL data present a lower performance with correlation coefficient ranging from 0.37 to 0.73. Second, the analysis of POLAC/PARASOL aerosol climatology reveals a high contribution of the coarse mode of aerosols ( AOD c between 0.1 and 0.4) at long distance from the African sources, confirming previous studies related to dust transport. The POLAC/PARASOL data were also compared with aerosol data obtained over the North Tropical Atlantic Ocean from MACC and MERRA-2 reanalyses. It is observed that the total AOD is underestimated in both reanalysis with a negative bias reaching −0.2. In summary, our results thus suggest that satellite POLAC/PARASOL observations of fine and coarse modes of aerosols could provide additional constraints useful to improve the quantification of the dust direct radiative forcing on a regional scale but also the biogeochemical processes such as nutrient supply to the surface waters.
Marine nitrogen fixation is co-limited by the supply of iron (Fe) and phosphorus in large regions of the global ocean. The deposition of soluble aerosol Fe can initiate nitrogen fixation and trigger ...toxic algal blooms in nitrate-poor tropical waters. We present dry season soluble Fe data from the Savannah Fires in the Early Dry Season (SAFIRED) campaign in northern Australia that reflects coincident dust and biomass burning sources of soluble aerosol Fe. The mean soluble and total aerosol Fe concentrations were 40 and 500 ng m−3 respectively. Our results show that while biomass burning species may not be a direct source of soluble Fe, biomass burning may substantially enhance the solubility of mineral dust. We observed fractional Fe solubility up to 12 % in mixed aerosols. Thus, Fe in dust may be more soluble in the tropics compared to higher latitudes due to higher concentrations of biomass-burning-derived reactive organic species in the atmosphere. In addition, biomass-burning-derived particles can act as a surface for aerosol Fe to bind during atmospheric transport and subsequently be released to the ocean upon deposition. As the aerosol loading is dominated by biomass burning emissions over the tropical waters in the dry season, additions of biomass-burning-derived soluble Fe could have harmful consequences for initiating nitrogen-fixing toxic algal blooms. Future research is required to quantify biomass-burning-derived particle sources of soluble Fe over tropical waters.
Savanna fires contribute significantly to global aerosol loading and hence to the Earth's radiative budget. Modeling of the climatic impact of these aerosols is made difficult due to a lack of ...knowledge of their size distribution. Australia is the third largest source of global carbon emissions from biomass burning, with emissions dominated by tropical savanna fires. Despite this, only a few previous studies have reported emission factors of trace gases from this important ecosystem and there are no previous published emission factors for the aerosol properties reported here for Australian savanna fires. In June 2014, the SAFIRED campaign (Savanna Fires in the Early Dry season) took place in the Northern Territory of Australia, with the purpose of investigating emissions and aging of aerosols from Australian savanna fires. This paper presents observed enhancement ratios and inferred emission factors of trace gases (CO2, CO, CH4, N2O, and gaseous elemental mercury), particles over different size modes (Aitken and accumulation), and speciated aerosols components (organics, sulfate, nitrate, ammonium, and chloride). Nine smoke events were identified from the data using large enhancements in CO and/or aerosol data to indicate biomass burning event. The results reported in this paper include the first emission factors for Aitken and accumulation mode aerosols from savanna fires, providing useful size information to enable better modeling of the climatic impact of this important source of global aerosols.
Key Points
First emission factors for Aitken and accumulation mode particles from savanna fires
First emission factors for speciated aerosols from Australian savanna fires
First emission factors for gaseous elemental mercury from Australian savanna fires
The evaluation and quantification of Southern Ocean cloud-radiation interactions simulated by climate models are essential in understanding the sources and magnitude of the radiative bias that ...persists in climate models for this region. To date, most evaluation methods focus on specific synoptic or cloud-type conditions that do not consider the entirety of the Southern Ocean's cloud regimes at once. Furthermore, it is difficult to directly quantify the complex and non-linear role that different cloud properties have on modulating cloud radiative effect. In this study, we present a new method of model evaluation, using machine learning that can at once identify complexities within a system and individual contributions.
Measurements of aerosol composition and size distributions were taken during the summer of 2013 at the remote island of Lampedusa in the southern central Mediterranean Sea. These measurements were ...part of the ChArMEx/ADRIMED (Chemistry and Aerosol Mediterranean Experiment/Aerosol Direct Radiative Forcing on the Mediterranean Climate) framework and took place during Special Observation Period 1a (SOP-1a) from 11 June to 5 July 2013. From compact time-of-flight aerosol mass spectrometer (cToF-AMS) measurements in the size range below 1 µm in aerodynamic diameter (PM1), particles were predominately comprised of ammonium and sulfate. On average, ammonium sulfate contributed 63 % to the non-refractory PM1 mass, followed by organics (33 %). The organic aerosol was generally very highly oxidized (f44 values were typically between 0.25 and 0.26). The contribution of ammonium sulfate was generally higher than organic aerosol in comparison to measurements taken in the western Mediterranean but is consistent with studies undertaken in the eastern basin. Source apportionment of organics using a statistical (positive matrix factorization) model revealed four factors: a hydrocarbon-like organic aerosol (HOA), a methanesulfonic-acid-related oxygenated organic aerosol (MSA-OOA), a more oxidized oxygenated organic aerosol (MO-OOA) and a less oxidized oxygenated organic aerosol (LO-OOA). The MO-OOA was the dominant factor for most of the campaign (53 % of the PM1 OA mass). It was well correlated with SO42-, highly oxidized and generally more dominant during easterly air masses originating from the eastern Mediterranean and central Europe. The LO-OOA factor had a very similar composition to the MO-OOA factor but was more prevalent during westerly winds, with air masses originating from the Atlantic Ocean, the western Mediterranean and at high altitudes over France and Spain from mistral winds. The MSA-OOA factor contributed an average 12 % to the PM1 OA and was more dominant during the mistral winds. The HOA, representing observed primary organic aerosol, only contributed 8 % of the average PM1 OA during the campaign. Even though Lampedusa is one of the most remote sites in the Mediterranean, PM1 concentrations (10 ± 5 µg m−3) were comparable to those observed in coastal cities and sites closer to continental Europe. Cleaner conditions corresponded to higher wind speeds. Nucleation and growth of new aerosol particles was observed during periods of north-westerly winds. From a climatology analysis from 1999 to 2012, these periods were much more prevalent during the measurement campaign than during the preceding 13 years. These results support previous findings that highlight the importance of different large-scale synoptic conditions in determining the regional and local aerosol composition and oxidation and also suggest that a non-polluted surface atmosphere over the Mediterranean is rare.
The Aerosol, Radiation and Clouds in southern Africa (AEROCLO-sA) project investigates the role of aerosols on the regional climate of southern Africa. This is a unique environment where natural and ...anthropogenic aerosols and a semipermanent and widespread stratocumulus (Sc) cloud deck are found. The project aims to understand the dynamical, chemical, and radiative processes involved in aerosol–cloud–radiation interactions over land and ocean and under various meteorological conditions. The AEROCLO-sA field campaign was conducted in August and September of 2017 over Namibia. An aircraft equipped with active and passive remote sensors and aerosol in situ probes performed a total of 30 research flight hours. In parallel, a ground-based mobile station with state-of-the-art in situ aerosol probes and remote sensing instrumentation was implemented over coastal Namibia, and complemented by ground-based and balloonborne observations of the dynamical, thermodynamical, and physical properties of the lower troposphere. The focus laid on mineral dust emitted from salty pans and ephemeral riverbeds in northern Namibia, the advection of biomass-burning aerosol plumes from Angola subsequently transported over the Atlantic Ocean, and aerosols in the marine boundary layer at the ocean-atmosphere interface. This article presents an overview of the AEROCLO-sA field campaign with results from the airborne and surface measurements. These observations provide new knowledge of the interactions of aerosols and radiation in cloudy and clear skies in connection with the atmospheric dynamics over southern Africa. They will foster new advanced climate simulations and enhance the capability of spaceborne sensors, ultimately allowing a better prediction of future climate and weather in southern Africa.
The vast majority of Australia's fires occur in the tropical north of the continent during the dry season. These fires are a significant source of aerosol and cloud condensation nuclei (CCN) in the ...region, providing a unique opportunity to investigate the biomass burning aerosol (BBA) in the absence of other sources. CCN concentrations at 0.5 % supersaturation and aerosol size and chemical properties were measured at the Australian Tropical Atmospheric Research Station (ATARS) during June 2014. CCN concentrations reached over 104 cm−3 when frequent and close fires were burning – up to 45 times higher than periods with no fires. Both the size distribution and composition of BBA appeared to significantly influence CCN concentrations. A distinct diurnal trend in the proportion of BBA activating to cloud droplets was observed, with an activation ratio of 40 ± 20 % during the night and 60 ± 20 % during the day. BBA was, on average, less hygroscopic during the night (κ = 0. 04 ± 0.03) than during the day (κ = 0.07 ± 0.05), with a maximum typically observed just before midday. Size-resolved composition of BBA showed that organics comprised a constant 90 % of the aerosol volume for aerodynamic diameters between 100 and 200 nm. While this suggests that the photochemical oxidation of organics led to an increase in the hygroscopic growth and an increase in daytime activation ratios, it does not explain the decrease in hygroscopicity after midday. Modelled CCN concentrations assuming typical continental hygroscopicities produced very large overestimations of up to 200 %. Smaller, but still significant, overpredictions up to ∼ 100 % were observed using aerosol mass spectrometer (AMS)- and hygroscopicity tandem differential mobility analyser (H-TDMA)-derived hygroscopicities as well as campaign night and day averages. The largest estimations in every case occurred during the night, when the small variations in very weakly hygroscopic species corresponded to large variations in the activation diameters. Trade winds carry the smoke generated from these fires over the Timor Sea, where aerosol–cloud interactions are likely to be sensitive to changes in CCN concentrations, perturbing cloud albedo and lifetime. Dry season fires in northern Australia are therefore potentially very important in cloud processes in this region.
There is a lack of knowledge of how biomass burning aerosols in the tropics age, including those in the fire-prone Northern Territory in Australia. This paper reports chemical characterization of ...fresh and aged aerosols monitored during the 1-month-long SAFIRED (Savannah Fires in the Early Dry Season) field study, with an emphasis on the chemical signature and aging of organic aerosols. The campaign took place in June 2014 during the early dry season when the surface measurement site, the Australian Tropical Atmospheric Research Station (ATARS), located in the Northern Territory, was heavily influenced by thousands of wild and prescribed bushfires. ATARS was equipped with a wide suite of instrumentation for gaseous and aerosol characterization. A compact time-of-flight aerosol mass spectrometer was deployed to monitor aerosol chemical composition. Approximately 90 % of submicron non-refractory mass was composed of organic material. Ozone enhancement in biomass burning plumes indicated increased air mass photochemistry. The diversity in biomass burning emissions was illustrated through variability in chemical signature (e.g. wide range in f44, from 0.06 to 0.18) for five intense fire events. The background particulate loading was characterized using positive matrix factorization (PMF). A PMF-resolved BBOA (biomass burning organic aerosol) factor comprised 24 % of the submicron non-refractory organic aerosol mass, confirming the significance of fire sources. A dominant PMF factor, OOA (oxygenated organic aerosol), made up 47 % of the sampled aerosol, illustrating the importance of aerosol aging in the Northern Territory. Biogenic isoprene-derived organic aerosol factor was the third significant fraction of the background aerosol (28 %).
Several studies have shown the importance of desert dust aerosols in weather forecast models. Nevertheless, desert dust has been poorly represented in such models and is the source of some prediction ...errors, in particular for tropical and subtropical regions. The purpose of this paper is to illustrate the formation and the three‐dimensional transport of a severe dust storm which occurred in March 2006 over West Africa. An intense dust haze was transported southward over the Gulf of Guinea thereby generating an aerosol optical thickness (AOT) greater than 4 over Nigeria. The MesoNH mesoscale atmospheric model coupled with new dust parameterization schemes has been used to illustrate the three‐dimensional transport of the dust plume and the vertical layering of this desert air mass above the lower atmosphere monsoon flux layer. It is modeled that more than 50 g m−2 of dust was emitted during this event from the surface by a strong Harmattan wind over the Sahel region. It is also shown that when the dust layer is located over the boundary layer, it can modify the atmospheric stability by as much as 9.5 K in terms of potential temperature in the lowest 2000 m of the atmosphere.
Using the regional climate model (RegCM4), optical depth and shortwave (SW) direct radiative forcing (DRF) of secondary organic aerosol (SOA) are investigated over China during the summer period. The ...biogenic emission and gas phase chemistry modules are updated to investigate α-pinene and limonene emissions and their reactions with atmosphere oxidants. The VBS (volatility basis set) model is implemented into RegCM4 to illustrate gas-particle partition process. During the study period (July 2006), the mean surface concentration and column burden of anthropogenic SOA (ASOA) over China are 1.90 µg m
−3
and 4.50 mg m
−3
, respectively. The ones of biogenic SOA (BSOA) are 2.00 and 3.35 mg m
−3
, respectively. Monthly mean calculated optical depths (at 550 nm) are 0.020 and 0.013 for ASOA and BSOA. The domain averaged simulated ASOA direct SW radiative forcing at surface and at the top of atmosphere (TOA) are −1.21 and −0.66 W m
−2
. For BSOA, the surface and TOA SW DRF are −0.75 and −0.46 W m
−2
. The errors induced by applying optical parameters of primary organic aerosol for SOA DRF modelling are also accessed. For DRF at TOA, it will increase by 156 and 161% for ASOA and BSOA. Though the optical parameters applied in this study are still rough, especially for intermediate SOA, this is a first step to apply explicit optical parameters for both ASOA and BSOA in DRF estimation.
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