scholarly journals Summertime Aerosol over the West of Ireland Dominated by Secondary Aerosol during Long-Range Transport

Atmosphere ◽  
2019 ◽  
Vol 10 (2) ◽  
pp. 59 ◽  
Author(s):  
Chunshui Lin ◽  
Darius Ceburnis ◽  
Ru-Jin Huang ◽  
Francesco Canonaco ◽  
André Prévôt ◽  
...  
Keyword(s):  
Long Range ◽  
Chemical Speciation ◽  
Organic Aerosol ◽  
Long Range Transport ◽  
Secondary Formation ◽  
Range Transport ◽  
Secondary Aerosols ◽  
Inorganic Aerosol ◽  
The Uk ◽  
Inorganic Sulfate

The chemical composition and sources of non-refractory submicron aerosol (NR-PM1) on Galway, a west coast city of Ireland, were characterized using an aerosol chemical speciation monitor during summertime in June 2016. Organic aerosol (OA) was found to be the major part of NR-PM1 (54%), followed by secondary inorganic sulfate (25%), ammonium (11%), and nitrate (10%). Factor analysis revealed that oxygenated OA (OOA) was the dominant OA factor, on average accounting for 84% of the total OA. The remaining 16% of OA was attributed to primary peat burning associated with domestic heating activities. As a result, secondary organic and inorganic aerosol together accounted for 91% of the total NR-PM1, pointing to an aged aerosol population originating from secondary formation during long-range transport. Concentration-weighted trajectory analysis indicated that these secondary aerosols were mainly associated with easterly long-range transport from the UK and/or France.

scholarly journals The role of long-range transport and domestic emissions in determining atmospheric secondary inorganic particle concentrations across the UK

2014 ◽  
Vol 14 (16) ◽  
pp. 8435-8447 ◽  
Author(s):  
M. Vieno ◽  
M. R. Heal ◽  
S. Hallsworth ◽  
D. Famulari ◽  
R. M. Doherty ◽  
...  
Keyword(s):  
Long Range ◽  
Long Range Transport ◽  
Limit Values ◽  
Substantial Impact ◽  
Inorganic Particle ◽  
Model Simulations ◽  
Range Transport ◽  
Inorganic Aerosol ◽  
The Uk

Abstract. Surface concentrations of secondary inorganic particle components over the UK have been analysed for 2001–2010 using the EMEP4UK regional atmospheric chemistry transport model and evaluated against measurements. Gas/particle partitioning in the EMEP4UK model simulations used a bulk approach, which may lead to uncertainties in simulated secondary inorganic aerosol. However, model simulations were able to accurately represent both the long-term decadal surface concentrations of particle sulfate and nitrate and an episode in early 2003 of substantially elevated nitrate measured across the UK by the AGANet network. The latter was identified as consisting of three separate episodes, each of less than 1 month duration, in February, March and April. The primary cause of the elevated nitrate levels across the UK was meteorological: a persistent high-pressure system, whose varying location impacted the relative importance of transboundary versus domestic emissions. Whilst long-range transport dominated the elevated nitrate in February, in contrast it was domestic emissions that mainly contributed to the March episode, and for the April episode both domestic emissions and long-range transport contributed. A prolonged episode such as the one in early 2003 can have substantial impact on annual average concentrations. The episode led to annual concentration differences at the regional scale of similar magnitude to those driven by long-term changes in precursor emissions over the full decade investigated here. The results demonstrate that a substantial part of the UK, particularly the south and southeast, may be close to or exceeding annual mean limit values because of import of inorganic aerosol components from continental Europe under specific conditions. The results reinforce the importance of employing multiple year simulations in the assessment of emissions reduction scenarios on particulate matter concentrations and the need for international agreements to address the transboundary component of air pollution.

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.

scholarly journals Effect of long-range transport on local PM 10 concentrations in the UK

2000 ◽  
Vol 10 (3) ◽  
pp. 229-238 ◽  
Author(s):  
Iain J. Beverland ◽  
Trygve Tunes ◽  
Malgorzata Sozanska ◽  
Robert A. Elton ◽  
Raymond M. Agius ◽  
...  
Keyword(s):  
Long Range ◽  
Long Range Transport ◽  
Range Transport ◽  
The Uk ◽  
Pm 10

scholarly journals Parametrisation of the orographic enhancement of precipitation and deposition in a long-term, long-range transport model

2000 ◽  
Vol 18 (11) ◽  
pp. 1447-1466 ◽  
Author(s):  
D. S. Lee ◽  
R. D. Kingdon ◽  
J. A. Garland ◽  
B. M. R. Jones
Keyword(s):  
Sulfur Dioxide ◽  
Long Range ◽  
Wet Deposition ◽  
Enhancement Factor ◽  
Long Range Transport ◽  
Orographic Precipitation ◽  
Range Transport ◽  
Orographic Enhancement ◽  
The Uk

Abstract. Orographic enhancement of wet deposition arising from the 'seeder-feeder' effect is, by necessity, highly parametrised in long-range transport models of acid deposition that are long-term (i.e. annual average) and spatially resolved at tens of kilometres. Here, we describe a mechanistic approach to the incorporation of these mechanisms into such a model. The model formulation required the following: precipitation rate by direction and quantification of the fractions that are orographic and non-orographic; treatment of the fast oxidation of sulfur dioxide in clouds; the directionality of the seeder-feeder process; and a quantitative basis for increasing wet deposition factors to account for the seeder-feeder process. The directionality of non-orographic precipitation was determined from meteorological data at 47 sites across the UK. Orographic precipitation varies on a much finer scale than can be interpolated from measurements, and thus a modelling approach was adopted. The directionality of the seeder-feeder effect was taken from measurements. The enhancement factor of the orographic component of precipitation, assumed to represent feeder-rain, was determined from a review of measurements. Fast oxidation of sulfur dioxide is an observed phenomenon in cap-cloud, but limited in duration. An adjustment was made to the sulfur dioxide oxidation rate in the model in locations where cap-cloud was assumed to be present. The results from the model were compared with UK deposition budgets and enhanced wet deposition maps. The revised parametrisation underestimated the UK wet deposition budgets of oxidised N and S, but spatial patterns of deposition were improved for much of the UK. It was concluded that this was a satisfactory outcome given the constraints of the statistical approach of weighting of deposition at receptors utilising straight line trajectories. The sensitivity of the model to directional constraints of seeder-feeder enhancement was tested and it was concluded that a fairly narrow constraint resulted in similar estimations to a broader one, and the broader constraint was thus adopted as frontal conditions which result in the process arrive from a fairly broad band of directions. When enhancement was allowed to occur from all directions, UK wet deposition of oxidised N and S was increased by 10%. The sensitivity to the enhancement factor on wet deposition was tested and found to be relatively robust. An increase in the enhancement factor from 2 to 6 resulted in increases in UK wet deposition of oxidised N and S of 9 and 6%, respectively.Key words: Atmospheric composition and structure (pollution – urban and regional) – Meteorology and atmospheric dynamics (precipitation)

Modelling the long-range transport of secondary PM10 to the UK

2000 ◽  
Vol 34 (6) ◽  
pp. 881-894 ◽  
Author(s):  
A.L. Malcolm ◽  
R.G. Derwent ◽  
R.H. Maryon
Keyword(s):  
Long Range ◽  
Long Range Transport ◽  
Range Transport ◽  
The Uk

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 Modeling regional aerosol variability over California and its sensitivity to emissions and long-range transport during the 2010 CalNex and CARES campaigns

2014 ◽  
Vol 14 (6) ◽  
pp. 7187-7303 ◽  
Author(s):  
J. D. Fast ◽  
J. Allan ◽  
R. Bahreini ◽  
J. Craven ◽  
L. Emmons ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Aerosol Optical Depth ◽  
Long Range ◽  
Optical Depth ◽  
Trace Gases ◽  
Organic Aerosol ◽  
Global Model ◽  
Long Range Transport ◽  
Anthropogenic Emissions ◽  
Range Transport

Abstract. The performance of the Weather Research and Forecasting regional model with chemistry (WRF-Chem) in simulating the spatial and temporal variations in aerosol mass, composition, and size over California is quantified using measurements collected during the California Nexus of Air Quality and Climate Experiment (CalNex) and the Carbonaceous Aerosol and Radiative Effects Study (CARES) conducted during May and June of 2010. The extensive meteorological, trace gas, and aerosol measurements collected at surface sites and along aircraft and ship transects during CalNex and CARES were combined with operational monitoring network measurements to create a single dataset that was used to evaluate the one configuration of the model. Simulations were performed that examined the sensitivity of regional variations in aerosol concentrations to anthropogenic emissions and to long-range transport of aerosols into the domain obtained from a global model. The configuration of WRF-Chem used in this study is shown to reproduce the overall synoptic conditions, thermally-driven circulations, and boundary layer structure observed in region that controls the transport and mixing of trace gases and aerosols. However, sub-grid scale variability in the meteorology and emissions as well as uncertainties in the treatment of secondary organic aerosol chemistry likely contribute to errors at a primary surface sampling site located at the edge of the Los Angeles basin. Differences among the sensitivity simulations demonstrate that the aerosol layers over the central valley detected by lidar measurements likely resulted from lofting and recirculation of local anthropogenic emissions along the Sierra Nevada. Reducing the default emissions inventory by 50% led to an overall improvement in many simulated trace gases and black carbon aerosol at most sites and along most aircraft flight paths; however, simulated organic aerosol was closer to observed when there were no adjustments to the primary organic aerosol emissions. The model performance for some aerosol species was not uniform over the region, and we found that sulfate was better simulated over northern California whereas nitrate was better simulated over southern California. While the overall spatial and temporal variability of aerosols and their precursors were simulated reasonably well, we show cases where the local transport of some aerosol plumes were either too slow or too fast, which adversely affects the statistics regarding the differences between observed and simulated quantities. Comparisons with lidar and in-situ measurements indicate that long-range transport of aerosols from the global model was likely too high in the free troposphere even though their concentrations were relatively low. This bias led to an over-prediction in aerosol optical depth by as much as a factor of two that offset the under-predictions of boundary-layer extinction resulting primarily from local emissions. Lowering the boundary conditions of aerosol concentrations by 50% greatly reduced the bias in simulated aerosol optical depth for all regions of California. This study shows that quantifying regional-scale variations in aerosol radiative forcing and determining the relative role of emissions from local and distant sources is challenging during "clean" conditions and that a wide array of measurements are needed to ensure model predictions are correct for the right reasons. In this regard, the combined CalNex and CARES datasets are an ideal testbed that can be used to evaluate aerosol models in great detail and develop improved treatments for aerosol processes.

scholarly journals The role of long-range transport and domestic emissions in determining atmospheric secondary inorganic particle concentrations across the UK

2013 ◽  
Vol 13 (12) ◽  
pp. 33433-33462
Author(s):  
M. Vieno ◽  
M. R. Heal ◽  
S. Hallsworth ◽  
D. Famulari ◽  
R. M. Doherty ◽  
...  
Keyword(s):  
Long Range ◽  
Regional Scale ◽  
Long Range Transport ◽  
Substantial Part ◽  
Limit Values ◽  
Substantial Impact ◽  
Inorganic Particle ◽  
Range Transport ◽  
The Uk

Abstract. Surface concentrations of secondary inorganic particle components over the UK have been analysed for 2001–2010 using the EMEP4UK regional atmospheric chemistry transport model. In early 2003 an episode of substantially elevated surface concentrations of ammonium nitrate was measured across the UK by the AGANET network. The EMEP4UK model was able accurately to represent both the long-term decadal surface concentrations and the episode in 2003. The latter was identified as consisting of three separate episodes, each of less than 1 month duration, in February, March and April. The primary cause of the elevated nitrate levels across the UK was meteorological, a persistent high pressure system, but whose varying location impacted the relative importance of transboundary vs. domestic emissions. Whilst long-range transport dominated the elevated nitrate in February, in contrast it was domestic emissions that mainly contributed to the March episode, and for the April episode both domestic emissions and long-range transport contributed. A prolonged episode such as the one in early 2003 can have substantial impact on annual average concentrations. The episode led to annual concentration differences at the regional scale of similar magnitude to those driven by long-term changes in precursor emissions over the full decade investigated here. The results demonstrate that a substantial part of the UK, particularly the south and south-east, may be close to or actually exceeding annual mean limit values because of import of inorganic aerosol components from continental Europe under specific conditions. The results reinforce the importance of employing multiple year simulations in the assessment of emissions reduction scenarios on PM concentrations and the need for international agreements to address the transboundary component of air pollution.

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