scholarly journals Source apportionment of the organic aerosol over the Atlantic Ocean from 53° N to 53° S: significant contributions from marine emissions and long-range transport

2018 ◽  
Vol 18 (24) ◽  
pp. 18043-18062 ◽  
Author(s):  
Shan Huang ◽  
Zhijun Wu ◽  
Laurent Poulain ◽  
Manuela van Pinxteren ◽  
Maik Merkel ◽  
...  
Keyword(s):  
Atlantic Ocean ◽  
Source Apportionment ◽  
Long Range ◽  
Aerosol Particles ◽  
Organic Aerosol ◽  
Long Range Transport ◽  
Data Set ◽  
Climate Effect ◽  
Dms Oxidation ◽  
Range Transport

Abstract. Marine aerosol particles are an important part of the natural aerosol systems and might have a significant impact on the global climate and biological cycle. It is widely accepted that truly pristine marine conditions are difficult to find over the ocean. However, the influence of continental and anthropogenic emissions on the marine boundary layer (MBL) aerosol is still less understood and non-quantitative, causing uncertainties in the estimation of the climate effect of marine aerosols. This study presents a detailed chemical characterization of the MBL aerosol as well as the source apportionment of the organic aerosol (OA) composition. The data set covers the Atlantic Ocean from 53∘ N to 53∘ S, based on four open-ocean cruises in 2011 and 2012. The aerosol particle composition was measured with a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), which indicated that sub-micrometer aerosol particles over the Atlantic Ocean are mainly composed of sulfates (50 % of the particle mass concentration), organics (21 %) and sea salt (12 %). OA has been apportioned into five factors, including three factors linked to marine sources and two with continental and/or anthropogenic origins. The marine oxygenated OA (MOOA, 16 % of the total OA mass) and marine nitrogen-containing OA (MNOA, 16 %) are identified as marine secondary products with gaseous biogenic precursors dimethyl sulfide (DMS) or amines. Marine hydrocarbon-like OA (MHOA, 19 %) was attributed to the primary emissions from the Atlantic Ocean. The factor for the anthropogenic oxygenated OA (Anth-OOA, 19 %) is related to continental long-range transport. Represented by the combustion oxygenated OA (Comb-OOA), aged combustion emissions from maritime traffic and wild fires in Africa contributed, on average, a large fraction to the total OA mass (30 %). This study provides the important finding that long-range transport was found to contribute averagely 49 % of the submicron OA mass over the Atlantic Ocean. This is almost equal to that from marine sources (51 %). Furthermore, a detailed latitudinal distribution of OA source contributions showed that DMS oxidation contributed markedly to the OA over the South Atlantic during spring, while continental-related long-range transport largely influenced the marine atmosphere near Europe and western and central Africa (15∘ N to 15∘ S). In addition, supported by a solid correlation between marine tracer methanesulfonic acid (MSA) and the DMS-oxidation OA (MOOA, R2>0.85), this study suggests that the DMS-related secondary organic aerosol (SOA) over the Atlantic Ocean could be estimated by MSA and a scaling factor of 1.79, especially in spring.

scholarly journals Formation of organic aerosol in the Paris region during the MEGAPOLI summer campaign: evaluation of the Volatility-Basis-Set approach within the CHIMERE model

2012 ◽  
Vol 12 (11) ◽  
pp. 29475-29533 ◽  
Author(s):  
Q. J. Zhang ◽  
M. Beekmann ◽  
F. Drewnick ◽  
F. Freutel ◽  
J. Schneider ◽  
...  
Keyword(s):  
Long Range ◽  
Organic Aerosol ◽  
Basis Set ◽  
Long Range Transport ◽  
Data Set ◽  
Campaign Evaluation ◽  
North East ◽  
Range Transport ◽  
Volatile Organic ◽  
Paris Region

Abstract. Results of the chemistry transport model CHIMERE are compared with the measurements performed during the MEGAPOLI summer campaign in the Greater Paris Region in July, 2009. The Volatility-Basis-Set approach (VBS) is implemented into this model, taking into account the volatility of primary organic aerosol (POA) and the chemical aging of semi-volatile organic species. Organic aerosol is the main focus and is simulated with three different configurations related to the volatility of POA and the scheme of secondary organic aerosol (SOA) formation. In addition, two types of emission inventories are used as model input in order to test the uncertainty related to the emissions. Predictions of basic meteorological parameters and primary and secondary pollutant concentrations are evaluated and four pollution regimes according to the air mass origin are defined. Primary pollutants are generally overestimated, while ozone is consistent with observations. Sulfate is generally overestimated, while ammonium and nitrate levels are well simulated with the refined emission data set. As expected, the simulation with non-volatile POA and a single-step SOA formation mechanism largely overestimates POA and underestimates SOA. Simulation of organic aerosol with the VBS approach taking into account the aging of semi-volatile organic compounds (SVOC) shows the best correlation with measurements. All observed high concentration events are reproduced by the model mostly after long range transport, indicating that long range transport of SOA to Paris is well reproduced. Depending on the emission inventory used, simulated POA levels are either reasonable or underestimated, while SOA levels tend to be overestimated. Several uncertainties related to the VBS scheme (POA volatility, SOA yields, the aging parameterization), to emission input data, and to simulated OH levels can be responsible for this behavior. Despite these uncertainties, the implementation of the VBS scheme into the CHIMERE model allowed for much more realistic organic aerosol simulations for Paris during summer time. The advection of SOA from outside Paris is mostly responsible for the highest OA concentration levels. During advection of polluted air masses from north-east (Benelux and Central Europe), simulations indicate high levels of both anthropogenic and biogenic SOA fractions, while biogenic SOA dominates during days with advection from Southern France and Spain.

scholarly journals Insights into the aging of biomass burning aerosol from satellite observations and 3D atmospheric modeling: evolution of the aerosol optical properties in Siberian wildfire plumes

2021 ◽  
Vol 21 (1) ◽  
pp. 357-392
Author(s):  
Igor B. Konovalov ◽  
Nikolai A. Golovushkin ◽  
Matthias Beekmann ◽  
Meinrat O. Andreae
Keyword(s):  
Optical Properties ◽  
Long Range ◽  
Biomass Burning ◽  
Organic Aerosol ◽  
Satellite Observations ◽  
Long Range Transport ◽  
Aerosol Optical Properties ◽  
Smoke Plumes ◽  
Range Transport ◽  
Aerosol Aging

Abstract. Long-range transport of biomass burning (BB) aerosol from regions affected by wildfires is known to have a significant impact on the radiative balance and air quality in receptor regions. However, the changes that occur in the optical properties of BB aerosol during long-range transport events are insufficiently understood, limiting the adequacy of representations of the aerosol processes in chemistry transport and climate models. Here we introduce a framework to infer and interpret changes in the optical properties of BB aerosol from satellite observations of multiple BB plumes. Our framework includes (1) a procedure for analysis of available satellite retrievals of the absorption and extinction aerosol optical depths (AAOD and AOD) and single-scattering albedo (SSA) as a function of the BB aerosol photochemical age and (2) a representation of the AAOD and AOD evolution with a chemistry transport model (CTM) involving a simplified volatility basis set (VBS) scheme with a few adjustable parameters. We apply this framework to analyze a large-scale outflow of BB smoke plumes from Siberia toward Europe that occurred in July 2016. We use AAOD and SSA data derived from OMI (Ozone Monitoring Instrument) satellite measurements in the near-UV range along with 550 nm AOD and carbon monoxide (CO) columns retrieved from MODIS (Moderate Resolution Imaging Spectroradiometer) and IASI (Infrared Atmospheric Sounding Interferometer) satellite observations, respectively, to infer changes in the optical properties of Siberian BB aerosol due to its atmospheric aging and to get insights into the processes underlying these changes. Using the satellite data in combination with simulated data from the CHIMERE CTM, we evaluate the enhancement ratios (EnRs) that allow isolating AAOD and AOD changes due to oxidation and gas–particle partitioning processes from those due to other processes, including transport, deposition, and wet scavenging. The behavior of EnRs for AAOD and AOD is then characterized using nonlinear trend analysis. It is found that the EnR for AOD strongly increases (by about a factor of 2) during the first 20–30 h of the analyzed evolution period, whereas the EnR for AAOD does not exhibit a statistically significant increase during this period. The increase in AOD is accompanied by a statistically significant enhancement of SSA. Further BB aerosol aging (up to several days) is associated with a strong decrease in EnRs for both AAOD and AOD. Our VBS simulations constrained by the observations are found to be more consistent with satellite observations of strongly aged BB plumes than “tracer” simulations in which atmospheric transformations of BB organic aerosol were disregarded. The simulation results indicate that the upward trends in EnR for AOD and in SSA are mainly due to atmospheric processing of secondary organic aerosol (SOA), leading to an increase in the mass scattering efficiency of BB aerosol. Evaporation and chemical fragmentation of the SOA species, part of which is assumed to be absorptive (to contain brown carbon), are identified as likely reasons for the subsequent decrease in the EnR for both AAOD and AOD. Hence, our analysis reveals that the long-range transport of smoke plumes from Siberian fires is associated with major changes in BB aerosol optical properties and chemical composition. Overall, this study demonstrates the feasibility of using available satellite observations for evaluating and improving representations in atmospheric models of the BB aerosol aging processes in different regions of the world at much larger temporal scales than those typically addressed in aerosol chamber experiments.

scholarly journals Long-Range Transport Mechanisms in East and Southeast Asia and Impacts on Size-Resolved Aerosol Composition: Contrasting High and Low Aerosol Loading Events

2019 ◽  
Author(s):  
Rachel A. Braun ◽  
Mojtaba Azadi Aghdam ◽  
Paola Angela Bañaga ◽  
Grace Betito ◽  
Maria Obiminda Cambaliza ◽  
...  
Keyword(s):  
Long Range ◽  
Biomass Burning ◽  
Dicarboxylic Acids ◽  
Organic Aerosol ◽  
Water Soluble ◽  
Long Range Transport ◽  
Aerosol Loading ◽  
Range Transport ◽  
Metro Manila ◽  
East And Southeast Asia

Abstract. This study analyzes mechanisms of long-range transport of aerosol and aerosol chemical characteristics in and around East and Southeast Asia. Ground-based size-resolved aerosol measurements collected at the Manila Observatory in Metro Manila, Philippines from July–October 2018 were used to identify and contrast high and low aerosol loading events. Multiple data sources, including models, remote-sensing, and in situ measurements, are used to analyze the impacts of long-range aerosol transport on Metro Manila and the conditions at the local and synoptic scales facilitating this transport. Evidence of long-range transport of biomass burning aerosol from the Maritime Continent was identified through model results and the presence of biomass burning tracers (e.g. K, Rb) in the ground-based measurements. The impacts of emissions transported from continental East Asia are also identified; for one of the events analyzed, this transport was facilitated by the nearby passage of a typhoon. Changes in the aerosol size distributions, water-soluble chemical composition, and contributions of various organic aerosol species to the total water-soluble organic aerosol were examined for the different cases. The events impacted by biomass burning transport had the overall highest concentration of water-soluble organic acids, while the events impacted by long-range transport from continental East Asia, showed high percent contributions from shorter chain dicarboxylic acids (i.e. oxalate) that are often representative of photochemical and aqueous processing in the atmosphere. The low aerosol loading event was subject to a larger precipitation accumulation than the high aerosol events, indicative of wet scavenging as an aerosol sink in the study region. This low aerosol event was characterized by a larger relative contribution from supermicrometer aerosols and had a higher percent contribution from longer-chain dicarboxylic acids (i.e. maleate) to the water-soluble organic aerosol fraction. Results of this study have implications for better understanding of the transport and chemical characteristics of aerosol in a highly-populated region that has thus far been difficult to measure through remote-sensing methods. Furthermore, findings associated with the effects of air mass mixing on aerosol physiochemical properties are applicable to other global regions impacted by both natural and anthropogenic sources.

Long-Range Transport of Anthropogenically and Naturally Produced Particulate Matter in the Mediterranean and North Atlantic: Current State of Knowledge

2007 ◽  
Vol 46 (8) ◽  
pp. 1230-1251 ◽  
Author(s):  
George Kallos ◽  
Marina Astitha ◽  
Petros Katsafados ◽  
Chris Spyrou
Keyword(s):  
Particulate Matter ◽  
Air Quality ◽  
North America ◽  
Atlantic Ocean ◽  
Long Range ◽  
Saharan Dust ◽  
Long Range Transport ◽  
Transport And Transformation ◽  
New Findings ◽  
Range Transport

Abstract During the past 20 years, organized experimental campaigns as well as continuous development and implementation of air-pollution modeling have led to significant gains in the understanding of the paths and scales of pollutant transport and transformation in the greater Mediterranean region (GMR). The work presented in this paper has two major objectives: 1) to summarize the existing knowledge on the transport paths of particulate matter (PM) in the GMR and 2) to illustrate some new findings related to the transport and transformation properties of PM in the GMR. Findings from previous studies indicate that anthropogenically produced air pollutants from European sources can be transported over long distances, reaching Africa, the Atlantic Ocean, and North America. The PM of natural origin, like Saharan dust, can be transported toward the Atlantic Ocean and North America mostly during the warm period of the year. Recent model simulations and studies in the area indicate that specific long-range transport patterns of aerosols, such as the transport from Asia and the Indian Ocean, central Africa, or America, have negligible or at best limited contribution to air-quality degradation in the GMR when compared with the other sources. Also, new findings from this work suggest that the imposed European Union limits on PM cannot be applicable for southern Europe unless the origin (natural or anthropogenic) of the PM is taken into account. The impacts of high PM levels in the GMR are not limited only to air quality, but also include serious implications for the water budget and the regional climate. These are issues that require extensive investigation because the processes involved are complex, and further model development is needed to include the relevant physicochemical processes properly.

Evidence for long range transport of biological and anthropogenic aerosol particles in the atmosphere

Grana ◽  
1984 ◽  
Vol 23 (1) ◽  
pp. 43-53 ◽  
Author(s):  
Paolo Mandrioli ◽  
Maria Grazia Negrini ◽  
Giulio Cesari ◽  
Griffith Morgan
Keyword(s):  
Long Range ◽  
Aerosol Particles ◽  
Long Range Transport ◽  
Anthropogenic Aerosol ◽  
Range Transport
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