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Arndt, J, Sciare J, Mallet M, Roberts GC, Marchand N, Sartelet K, Sellegri K, Dulac F, Healy RM, Wenger JC.  2017.  Sources and mixing state of summertime background aerosol in the north-western Mediterranean basin. Atmospheric Chemistry and Physics. 17:6975-7001.   10.5194/acp-17-6975-2017   AbstractWebsite

An aerosol time-of-flight mass spectrometer (ATOFMS) was employed to provide real-time single particle mixing state and thereby source information for aerosols impacting the western Mediterranean basin during the ChArMEx-ADRIMED and SAF-MED campaigns in summer 2013. The ATOFMS measurements were made at a ground-based remote site on the northern tip of Corsica. Twenty-seven distinct ATOFMS particle classes were identified and subsequently grouped into eight general categories: EC-rich (elemental carbon), K-rich, Na-rich, amines, OC-rich (organic carbon), V-rich, Fe-rich and Ca-rich particles. Mass concentrations were reconstructed for the ATOFMS particle classes and found to be in good agreement with other co-located quantitative measurements (PM1, black carbon (BC), organic carbon, sulfate mass and ammonium mass). Total ATOFMS reconstructed mass (PM2.5) accounted for 70-90% of measured PM10 mass and was comprised of regionally transported fossil fuel (EC-rich) and biomass burning (K-rich) particles. The accumulation of these transported particles was favoured by repeated and extended periods of air mass stagnation over the western Mediterranean during the sampling campaigns. The single particle mass spectra proved to be valuable source markers, allowing the identification of fossil fuel and biomass burning combustion sources, and was therefore highly complementary to quantitative measurements made by Particle into Liquid Sampler ion chromatography (PILS-IC) and an aerosol chemical speciation monitor (ACSM), which have demonstrated that PM1 and PM10 were comprised predominantly of sulfate, ammonium and OC. Good temporal agreement was observed between ATOFMS EC-rich and K-rich particle mass concentrations and combined mass concentrations of BC, sulfate, ammonium and low volatility oxygenated organic aerosol (LV-OOA). This combined information suggests that combustion of fossil fuels and biomass produced primary EC- and OC-containing particles, which then accumulated ammonium, sulfate and alkylamines during regional transport. Three other sources were also identified: local biomass burning, marine and shipping. Local combustion particles

Roberts, GC, Ramana MV, Corrigan C, Kim D, Ramanathan V.  2008.  Simultaneous observations of aerosol-cloud-albedo interactions with three stacked unmanned aerial vehicles. Proceedings of the National Academy of Sciences of the United States of America. 105:7370-7375.   10.1073/pnas.0710308105   AbstractWebsite

Aerosol impacts on climate change are still poorly understood, in part, because the few observations and methods for detecting their effects are not well established. For the first time, the enhancement in cloud albedo is directly measured on a cloud-by-cloud basis and linked to increasing aerosol concentrations by using multiple autonomous unmanned aerial vehicles to simultaneously observe the cloud microphysics, vertical aerosol distribution, and associated solar radiative fluxes. In the presence of long-range transport of dust and anthropogenic pollution, the trade cumuli have higher droplet concentrations and are on average brighter. Our observations suggest a higher sensitivity of radiative forcing by trade cumuli to increases in cloud droplet concentrations. than previously reported owing to a constrained droplet radius such that increases in droplet concentrations also increase cloud liquid water content. This aerosol-cloud forcing efficiency is as much as -60 W m(-2) per 100% percent cloud fraction for a doubling of droplet concentrations and associated increase of liquid water content. Finally, we develop a strategy for detecting aerosol-cloud interactions based on a nondimensional scaling analysis that relates the contribution of single clouds to albedo measurements and illustrates the significance of characterizing cloud morphology in resolving radiometric measurements. This study demonstrates that aerosol-cloud-albedo interactions can be directly observed by simultaneous observations below, in, and above the clouds.

Guyon, P, Graham B, Roberts GC, Mayol-Bracero OL, Maenhaut W, Artaxo P, Andreae MO.  2004.  Sources of optically active aerosol particles over the Amazon forest. Atmospheric Environment. 38:1039-1051.   10.1016/j.atmosenv.2003.10.051   AbstractWebsite

Size-fractionated ambient aerosol samples were collected at a pasture site and a primary rainforest site in the Brazilian Amazon Basin during two field campaigns (April-May and September-October 1999), as part of the European contribution to the Large-Scale Biosphere-Atmosphere Experiment in Amazonia (LBA-EUSTACH). The samples were analyzed for up to 19 trace elements by particle-induced X-ray emission analysis (PIXE), for equivalent black carbon (BCe) by a light reflectance technique and for mass concentration by gravimetric analysis. Additionally, we made continuous measurements of absorption and light scattering by aerosol particles. The vertical chemical composition gradients at the forest site have been discussed in a companion article (Journal of Geophysical Research-Atmospheres 108 (1318), 4591 (doi:4510.1029/2003JD003465)). In this article, we present the results of a source identification and quantitative apportionment study of the wet and dry season aerosols, including an apportionment of the measured scattering and absorption properties of the total aerosol in terms of the identified aerosol sources. Source apportionments (obtained from absolute principal component analysis) revealed that the wet and dry season aerosols contained the same three main components, but in different (absolute and relative) amounts: the wet season aerosol consisted mainly of a natural biogenic component, whereas pyrogenic aerosols dominated the dry season aerosol mass. The third component identified was soil dust, which was often internally mixed with the biomass-burning aerosol. All three components contributed significantly to light extinction during both seasons. At the pasture site, up to 47% of the light absorption was attributed to biogenic particles during the wet season, and up to 35% at the tower site during the wet-to-dry transition period. The results from the present study suggest that, in addition to pyrogenic particles, biogenic and soil dust aerosols must be taken into account when modeling the physical and optical properties of aerosols in forested regions such the Amazon Basin. (C) 2003 Published by Elsevier Ltd.

Guyon, P, Graham B, Roberts GC, Mayol-Bracero OL, Maenhaut W, Artaxo P, Andreae MO.  2003.  In-canopy gradients, composition, sources, and optical properties of aerosol over the Amazon forest. Journal of Geophysical Research-Atmospheres. 108   10.1029/2003jd003465   AbstractWebsite

[1] As part of the Large-Scale Biosphere-Atmosphere Experiment in Amazonia-European Studies on Trace Gases and Atmospheric Chemistry (LBA-EUSTACH), size-fractionated aerosol samples were collected at a primary rain forest in the Brazilian Amazon during two field campaigns in April - May and September - October 1999. These two periods encompassed parts of the wet and dry seasons, respectively. Daytime-nighttime-segregated sampling was carried out at three different heights ( above, within, and below canopy level) on a 54-m meteorological tower at the forest site in order to better characterize the aerosol sources. The samples were analyzed for up to 19 trace elements by particle-induced X-ray emission analysis and for carbonaceous components by thermal-optical analysis. Equivalent black carbon (BCe) and gravimetric analyses were also performed. The average mass concentrations for particles < 2 μm diameter were 2.2 and 33.5 μg m(-3) for the wet and the dry seasons, respectively. The elements related to biomass burning and soil dust generally exhibited highest concentrations above the canopy and during daytime, while forest-derived aerosol was more concentrated underneath the canopy and during nighttime. These variations can be largely attributed to daytime convective mixing and the formation of a shallow nocturnal boundary layer, along with the possibility of enhanced nighttime release of biogenic aerosol particles. Mass scattering (α(s)) and mass absorption efficiency (α(a)) data indicate that scattering was dominated by fine aerosol, while fine and coarse aerosol both contributed significantly to absorption during both seasons. The data also suggest that components other than elemental carbon were responsible for a substantial fraction of the absorption.

Graham, B, Mayol-Bracero OL, Guyon P, Roberts GC, Decesari S, Facchini MC, Artaxo P, Maenhaut W, Koll P, Andreae MO.  2002.  Water-soluble organic compounds in biomass burning aerosols over Amazonia - 1. Characterization by NMR and GC-MS. Journal of Geophysical Research-Atmospheres. 107   10.1029/2001jd000336   AbstractWebsite

[1] As part of the European contribution to the Large-Scale Atmosphere-Biosphere Experiment in Amazonia (LBA-EUSTACH), aerosols were sampled at representative pasture and primary rainforest sites in Rondonia, Brazil, during the 1999 "burning season" and dry-to-wet season transition (September-October). Water-soluble organic compounds (WSOCs) within the samples were characterized using a combination of H-1 Nuclear Magnetic Resonance (NMR) spectroscopy for chemical functional group analysis, and Gas Chromatography-Mass Spectrometry (GC-MS) for identification and quantification of individual low-molecular-weight compounds. The H-1 NMR analysis indicates that WSOCs are predominantly aliphatic or oxygenated aliphatic compounds (alcohols, carboxylic acids, etc.), with a minor content of aromatic rings carrying carboxylic and phenolic groups. Levoglucosan (1,6-anhydro-beta-D-glucose), a well-known cellulose combustion product, was the most abundant individual compound identified by GC-MS (0.04-6.90 mug m(-3)), accounting for 1-6% of the total carbon (TC) and 2-8% of the water-soluble organic carbon (WSOC). Other anhydrosugars, produced by hemicellulose breakdown, were detected in much smaller amounts, in addition to series of acids, hydroxyacids, oxoacids, and polyalcohols (altogether 2-5% of TC, 3-6% of WSOC). Most correlated well with organic carbon, black carbon, and potassium, indicating biomass burning to be the major source. A series of sugar alcohols (mannitol, arabitol, erythritol) and sugars (glucose, fructose, mannose, galactose, sucrose, trehalose) were identified as part of the natural background aerosol and are probably derived from airborne microbes and other biogenic material. The bulk of the WSOCs (86-91% WSOC) eluded analysis by GC-MS and may be predominantly high-molecular weight in nature.

Roberts, GC, Andreae MO, Maenhaut W, Fernandez-Jimenez MT.  2001.  Composition and sources of aerosol in a central African rain forest during the dry season. Journal of Geophysical Research-Atmospheres. 106:14423-14434.   10.1029/2000jd900774   AbstractWebsite

During the Experiment for Regional Sources and Sinks of Oxidants (EXPRESSO-96), size-fractionated aerosol samples were collected in November and December 1996 at a ground site in the tropical rain forest at the N'doki National Park (NNP) in the Republic of Congo. The samples were analyzed for up to 26 elements using particle-induced X-ray emission. Elements related to mineral dust and pyrogenic aerosol exhibited greater concentrations during the daytime, while aerosol produced by the rain forest exhibited higher concentrations at night. Samples were also collected at two levels on the tower, above and below the canopy, to characterize vegetation sources. Absolute principal component analysis (APCA) identified three major aerosol source types in each size fraction, which explained more than 90% of the data variance. The fine-size fraction contained mineral dust (Al, Si, Ca, Ti, and Fe), pyrogenic (black carbon, K, and Zn), and marine/anthropogenic sulfur components. The coarse-size fraction included a mineral dust (Al, Si, Ca, Ti, Mn, and Fe) and two primary biogenic components consisting of K, P, Zn, and S. Absolute principal component scores were calculated for the components of APCA, and temporal trends were compared to 7 day isopycnic backward trajectories. Consistent relationships between the temporal trends of the fine fraction aerosol components and meteorological patterns were observed. Trade wind air masses transported biomass burning and mineral dust aerosol to NNP during the first half of the experiment. The fine fraction sulfur component correlated well with the pyrogenic activity before the change in meteorological patterns halfway through the experiment. The fine and coarse sulfur concentrations nearly doubled in the latter part of the experiment as a monsoon circulation brought sulfur-enriched aerosol from the Atlantic Ocean. Various industrial activities on the coast of Cameroon and Gabon probably contributed to the high sulfur concentrations as well.

Formenti, P, Andreae MO, Lange L, Roberts G, Cafmeyer J, Rajta I, Maenhaut W, Holben BN, Artaxo P, Lelieveld J.  2001.  Saharan dust in Brazil and Suriname during the Large-Scale Biosphere-Atmosphere Experiment in Amazonia (LBA) - Cooperative LBA Regional Experiment (CLAIRE) in March 1998. Journal of Geophysical Research-Atmospheres. 106:14919-14934.   10.1029/2000jd900827   AbstractWebsite

Advection of Saharan dust was observed via chemical and optical measurements during March 1998 in Brazil and Suriname during the Large-Scale Biosphere-Atmosphere Experiment in Amazonia (LBA)-Cooperative LBA Airborne Regional Experiment (CLAIRE)-98 experiment. In Brazil the dust outbreak produced an increase of a factor of 3 in the daily mean mass concentration (up to 26 +/- 7 mug m(-3)) of particles smaller than 10 mum equivalent aerodynamic diameter (EAD), and in the daily mean aerosol particle scattering coefficient sigma (N) (up to 26 +/- 8 Mm(-1) STP, ambient humidity). Background levels of aerosol scattering (ambient) were sigma (s) similar to 10 Mm(-1). The effect of dust advection was evident for all major crustal elements (Al, Si, Ca, Ti, Mn, and Fe), as well as the sea-salt elements (Na, Cl, and S), as the dust layer was transported at low altitude (below 800 hPa). Coarse P and organic carbon (OC) concentrations were not influenced by the occurrence of dust, and were mainly emitted by the rain forest. The dry scattering mass efficiency of dust (particles smaller than 10 mum EAD) was estimated to be between 0.65 (+/- 0.06) and 0.89 (+/- 0.08) m(2) g(-1). Airborne profiles of aerosol scattering showed two distinct types of vertical structure in the dust layer over Suriname, either vertically uniform (15, 26 March), or plume-like (25 March). Dust layers extended generally up to 700 hPa, while scattering layers occasionally encountered at higher altitudes resulted from smoke emitted by biomass burning in Venezuela and Colombia, Observations in South America were supported by measurements in Israel and Tenerife (Canary Islands), where the dust outbreaks were also detected.