scholarly journals Variability of aerosol, gaseous pollutants and meteorological characteristics associated with changes in air mass origin at the SW Atlantic coast of Iberia

2012 ◽  
Vol 12 (8) ◽  
pp. 3761-3782 ◽  
Author(s):  
J.-M. Diesch ◽  
F. Drewnick ◽  
S. R. Zorn ◽  
S.-L. von der Weiden-Reinmüller ◽  
M. Martinez ◽  
...  

Abstract. Measurements of the ambient aerosol were performed at the Southern coast of Spain, within the framework of the DOMINO (Diel Oxidant Mechanisms In relation to Nitrogen Oxides) project. The field campaign took place from 20 November until 9 December 2008 at the atmospheric research station "El Arenosillo" (37°5'47.76" N, 6°44'6.94" W). As the monitoring station is located at the interface between a natural park, industrial cities (Huelva, Seville) and the Atlantic Ocean, a variety of physical and chemical parameters of aerosols and gas phase could be characterized in dependency on the origin of air masses. Backwards trajectories were examined and compared with local meteorology to classify characteristic air mass types for several source regions. Aerosol number and mass as well as polycyclic aromatic hydrocarbons and black carbon concentrations were measured in PM1 and size distributions were registered covering a size range from 7 nm up to 32 μm. The chemical composition of the non-refractory submicron aerosol (NR-PM1) was measured by means of an Aerosol Mass Spectrometer (Aerodyne HR-ToF-AMS). Gas phase analyzers monitored various trace gases (O3, SO2, NO, NO2, CO2) and a weather station provided meteorological parameters. Lowest average submicron particle mass and number concentrations were found in air masses arriving from the Atlantic Ocean with values around 2 μg m−3 and 1000 cm−3. These mass concentrations were about two to four times lower than the values recorded in air masses of continental and urban origins. For some species PM1-fractions in marine air were significantly larger than in air masses originating from Huelva, a closely located city with extensive industrial activities. The largest fraction of sulfate (54%) was detected in marine air masses and was to a high degree not neutralized. In addition, small concentrations of methanesulfonic acid (MSA), a product of biogenic dimethyl sulfate (DMS) emissions, could be identified in the particle phase. In all air masses passing the continent the organic aerosol fraction dominated the total NR-PM1. For this reason, using Positive Matrix Factorization (PMF) four organic aerosol (OA) classes that can be associated with various aerosol sources and components were identified: a highly-oxygenated OA is the major component (43% OA) while semi-volatile OA accounts for 23%. A hydrocarbon-like OA mainly resulting from industries, traffic and shipping emissions as well as particles from wood burning emissions also contribute to total OA and depend on the air mass origin. A significant variability of ozone was observed that depends on the impact of different air mass types and solar radiation.

2011 ◽  
Vol 11 (12) ◽  
pp. 31585-31642 ◽  
Author(s):  
J.-M. Diesch ◽  
F. Drewnick ◽  
S. R. Zorn ◽  
S.-L. von der Weiden-Reinmüller ◽  
M. Martinez ◽  
...  

Abstract. Measurements of the ambient aerosol were performed at the Southern coast of Spain, within the framework of the DOMINO (Diel Oxidant Mechanisms In relation to Nitrogen Oxides) project. The field campaign took place from 20 November until 9 December 2008 at the atmospheric research station "El Arenosillo" (37°5'47.76" N, 6&deg44'6.94" W). As the monitoring station is located at the interface between a natural park, industrial cities (Huelva, Seville) and the Atlantic Ocean a variety of physical and chemical parameters of aerosols and gas phase could be characterized in dependency on the origin of air masses. Backwards trajectories were examined and compared with local meteorology to classify characteristic air mass types for several source regions. Aerosol number and mass as well as polycyclic aromatic hydrocarbons and black carbon concentrations were measured in PM1 and size distributions were registered covering a size range from 7 nm up to 32 μm. The chemical composition of the non-refractory submicron aerosol was measured by means of an Aerosol Mass Spectrometer (Aerodyne HR-ToF-AMS). Gas phase analyzers monitored various trace gases (O3, SO2, NO, NO2, CO2) and a weather station provided meteorological parameters. Lowest average submicron particle mass and number concentrations were found in air masses arriving from the Atlantic Ocean with values around 2 μg m−3 and 1000 cm−3. These mass concentrations were about two to four times lower than the values recorded in air masses of continental and urban origins. For some species PM1-fractions in marine air were significantly larger than in air masses originating from Huelva, a closely located city with extensive industrial activities. The largest fraction of sulfate (54%) was detected in marine air masses and was to a high degree not neutralized. In addition small concentrations of methanesulfonic acid (MSA), a product of biogenic dimethyl sulfate (DMS) emissions could be identified in the particle phase. In all air masses passing the continent the organic aerosol fraction dominated the total NR-PM1. For this reason, using Positive Matrix Factorization (PMF) four organic aerosol (OA) classes that can be associated with various aerosol sources and components were identified: a highly-oxygenated OA is the major component contributing an average of 43% of the particulate organic mass while the semi-volatile OA accounts for 23%. A hydrocarbon-like OA mainly resulting from industries, traffic and shipping emissions as well as particles from wood burning emissions also contribute to total OA dependent on the air mass origin. The variability of ozone is not only affected by different types of air masses but also significantly by the diurnal variation as a consequence of the solar radiation as well as local meteorological parameters.


2013 ◽  
Vol 13 (2) ◽  
pp. 933-959 ◽  
Author(s):  
F. Freutel ◽  
J. Schneider ◽  
F. Drewnick ◽  
S.-L. von der Weiden-Reinmüller ◽  
M. Crippa ◽  
...  

Abstract. During July 2009, a one-month measurement campaign was performed in the megacity of Paris. Amongst other measurement platforms, three stationary sites distributed over an area of 40 km in diameter in the greater Paris region enabled a detailed characterization of the aerosol particle and gas phase. Simulation results from the FLEXPART dispersion model were used to distinguish between different types of air masses sampled. It was found that the origin of air masses had a large influence on measured mass concentrations of the secondary species particulate sulphate, nitrate, ammonium, and oxygenated organic aerosol measured with the Aerodyne aerosol mass spectrometer in the submicron particle size range: particularly high concentrations of these species (about 4 μg m−3, 2 μg m−3, 2 μg m−3, and 7 μg m−3, respectively) were measured when aged material was advected from continental Europe, while for air masses originating from the Atlantic, much lower mass concentrations of these species were observed (about 1 μg m−3, 0.2 μg m−3, 0.4 μg m−3, and 1–3 μg m−3, respectively). For the primary emission tracers hydrocarbon-like organic aerosol, black carbon, and NOx it was found that apart from diurnal source strength variations and proximity to emission sources, local meteorology had the largest influence on measured concentrations, with higher wind speeds leading to larger dilution and therefore smaller measured concentrations. Also the shape of particle size distributions was affected by wind speed and air mass origin. Quasi-Lagrangian measurements performed under connected flow conditions between the three stationary sites were used to estimate the influence of the Paris emission plume onto its surroundings, which was found to be rather small. Rough estimates for the impact of the Paris emission plume on the suburban areas can be inferred from these measurements: Volume mixing ratios of 1–14 ppb of NOx, and upper limits for mass concentrations of about 1.5 μg m−3 of black carbon and of about 3 μg m−3 of hydrocarbon-like organic aerosol can be deduced which originate from both, local emissions and the overall Paris emission plume. The secondary aerosol particle phase species were found to be not significantly influenced by the Paris megacity, indicating their regional origin. The submicron aerosol mass concentrations of particulate sulphate, nitrate, and ammonium measured during time periods when air masses were advected from eastern central Europe were found to be similar to what has been found from other measurement campaigns in Paris and south-central France for this type of air mass origin, indicating that the results presented here are also more generally valid.


2012 ◽  
Vol 12 (8) ◽  
pp. 22199-22268 ◽  
Author(s):  
F. Freutel ◽  
J. Schneider ◽  
F. Drewnick ◽  
S.-L. von der Weiden-Reinmüller ◽  
M. Crippa ◽  
...  

Abstract. During July 2009, a one-month measurement campaign was performed in the megacity of Paris. Amongst other measurement platforms, three stationary sites distributed over an area of 40 km in diameter in the greater Paris region enabled a detailed characterization of the aerosol particle and gas phase. Simulation results from the FLEXPART dispersion model were used to distinguish between different types of air masses sampled. It was found that the origin of air masses had a large influence on measured mass concentrations of the secondary species particulate sulphate, nitrate, ammonium, and oxygenated organic aerosol measured with the Aerodyne aerosol mass spectrometer in the submicron particle size range: particularly high concentrations of these species (about 4 μg m−3, 2 μg m−3, 2 μg m−3, and 7 μg m−3, respectively) were measured when aged material was advected from continental Europe, while for air masses originating from the Atlantic, much lower mass concentrations of these species were observed (about 1 μg m−3, 0.2 μg m−3, 0.4 μg m−3, and 1–3 μg m−3, respectively). For the primary emission tracers hydrocarbon-like organic aerosol, black carbon, and NOx it was found that apart from diurnal source strength variations and proximity to emission sources, local meteorology had the largest influence on measured concentrations, with higher wind speeds leading to larger dilution and therefore smaller measured concentrations. Also the shape of particle size distributions was affected by wind speed and air mass origin. Quasi-Lagrangian measurements performed under connected flow conditions between the three stationary sites were used to estimate the influence of the Paris emission plume onto its surroundings, which was found to be rather small. Rough estimates for the impact of the Paris emission plume on the suburban areas can be inferred from these measurements: Volume mixing ratios of 1–14 ppb of NOx, and upper limits for mass concentrations of about 1.5 μg m−3 of black carbon and of about 3 μg m−3 of hydrocarbon-like organic aerosol can be deduced which originate from both, local emissions and the overall Paris emission plume. The secondary aerosol particle phase species were found to be not significantly influenced by the Paris megacity, indicating their regional origin. The submicron aerosol mass concentrations of particulate sulphate, nitrate, and ammonium measured during time periods when air masses were advected from eastern central Europe were found to be similar to what has been found from other measurement campaigns in Paris and South-Central France for this type of air mass origin, indicating that the results presented here are also more generally valid.


2014 ◽  
Vol 14 (3) ◽  
pp. 1397-1412 ◽  
Author(s):  
E. J. Freney ◽  
K. Sellegri ◽  
F. Canonaco ◽  
A. Colomb ◽  
A. Borbon ◽  
...  

Abstract. The MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) experiment took place in July 2009. The aim of this campaign was to study the aging and reactions of aerosol and gas-phase emissions in the city of Paris. Three ground-based measurement sites and several mobile platforms including instrument equipped vehicles and the ATR-42 aircraft were involved. We present here the variations in particle- and gas-phase species over the city of Paris, using a combination of high-time resolution measurements aboard the ATR-42 aircraft. Particle chemical composition was measured using a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS), giving detailed information on the non-refractory submicron aerosol species. The mass concentration of black carbon (BC), measured by a particle absorption soot photometer (PSAP), was used as a marker to identify the urban pollution plume boundaries. Aerosol mass concentrations and composition were affected by air-mass history, with air masses that spent longest time over land having highest fractions of organic aerosol and higher total mass concentrations. The Paris plume is mainly composed of organic aerosol (OA), BC, and nitrate aerosol, as well as high concentrations of anthropogenic gas-phase species such as toluene, benzene, and NOx. Using BC and CO as tracers for air-mass dilution, we observe the ratio of ΔOA / ΔBC and ΔOA / ΔCO increase with increasing photochemical age (−log(NOx / NOy)). Plotting the equivalent ratios of different organic aerosol species (LV-OOA, SV-OOA, and HOA) illustrate that the increase in OA is a result of secondary organic aerosol (SOA) formation. Within Paris the changes in the ΔOA / ΔCO are similar to those observed during other studies in London, Mexico City, and in New England, USA. Using the measured SOA volatile organic compounds (VOCs) species together with organic aerosol formation yields, we were able to predict ~50% of the measured organics. These airborne measurements during the MEGAPOLI experiment show that urban emissions contribute to the formation of OA and have an impact on aerosol composition on a regional scale.


2013 ◽  
Vol 13 (9) ◽  
pp. 24885-24924
Author(s):  
E. J. Freney ◽  
K. Sellegri ◽  
F. Canonaco ◽  
A. Colomb ◽  
A. Borbon ◽  
...  

Abstract. The MEGAPOLI experiment took place in July 2009. The aim of this campaign was to study the aging and reactions of aerosol and gas-phase emissions in the city of Paris. Three ground-based measurement sites and several mobile platforms including instrument equipped vehicles and the ATR-42 aircraft were involved. We present here the variations in particle- and gas-phase species over the city of Paris using a combination of high-time resolution measurements aboard the ATR-42 aircraft. Particle chemical composition was measured using a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS) giving detailed information of the non-refractory submicron aerosol species. The mass concentration of BC, measured by a particle absorption soot photometer (PSAP), was used as a marker to identify the urban pollution plume boundaries. Aerosol mass concentrations and composition were affected by air-mass history, with air masses that spent longest time over land having highest fractions of organic aerosol and higher total mass concentrations. The Paris plume is mainly composed of organic aerosol (OA), black carbon and nitrate aerosol, as well as high concentrations of anthropogenic gas-phase species such as toluene, benzene, and NOx. Using BC and CO as tracers for air-mass dilution, we observe the ratio of ΔOA / ΔBC and ΔOA / ΔCO increase with increasing photochemical age (−log(NOx / NOy). Plotting the equivalent ratios for the Positive Matrix Factorization (PMF) resolved species (LV-OOA, SV-OOA, and HOA) illustrate that the increase in OA is a result of secondary organic aerosol (SOA). Within Paris the changes in the ΔOA / ΔCO are similar to those observed during other studies in Mexico city, Mexico and in New England, USA. Using the measured VOCs species together with recent organic aerosol formation yields we predicted ~ 50% of the measured organics. These airborne measurements during the MEGAPOLI experiment show that urban emissions contribute to the formation of OA, and have an impact on aerosol composition on a regional scale. They provide a quantitative measure of this impact in terms of urban plume composition and evolution relative to background aerosol composition.


2015 ◽  
Vol 15 (1) ◽  
pp. 37-53 ◽  
Author(s):  
Y. J. Li ◽  
B. P. Lee ◽  
L. Su ◽  
J. C. H. Fung ◽  
C.K. Chan

Abstract. Atmospheric particulate matter (PM) remains poorly understood due to the lack of comprehensive measurements at high time resolution for tracking its dynamic features and the lack of long-term observation for tracking its seasonal variability. Here, we present highly time-resolved and seasonal compositions and characteristics of non-refractory components in PM with a diameter less than 1 μm (NR-PM1) at a suburban site in Hong Kong. The measurements were made with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) at the Hong Kong University of Science and Technology (HKUST) Air Quality Research Supersite for 4 months, with one in each season of the year. The average NR-PM1 concentration of ~ 15 μg m−3 is higher than those AMS measurements made in South Korea and Japan, but lower than those in North China, the Yangtze River Delta and the nearby Pearl River Delta. The seasonal dependence of the total NR-PM1 monthly averaged concentrations was small, but that of the fractions of the species in NR-PM1 was significant. Site characteristic plays an important role in the relative fractions of species in NR-PM1 and our results are generally consistent with measurements at other non-urban sites in this regard. Detailed analyses were conducted on the AMS data in the aspects of (1) species concentrations, (2) size distributions, (3) degree of oxygenation of organics, and (4) positive matrix factorization (PMF)-resolved organic factors in a seasonal context, as well as with air mass origin from back-trajectory analysis. Sulfate had the highest fraction in NR-PM1 (> 40%), and the surrogates of secondary organic species – semi-volatile oxygenated organic aerosol (SVOOA) and low-volatility oxygenated organic aerosol (LVOOA) – prevailed (~ 80%) in the organic portion of NR-PM1. Local contributions to the organic portion of NR-PM1 at this suburban site was strongly dependent on season. The hydrocarbon-like organic aerosol (HOA) factor related to local traffic emissions contributed > 10% to organic aerosols in spring and summer but only 6–7% in autumn and winter. The cooking organic aerosol (COA) factor contributed > 10% to organic aerosols in winter. With the aid of highly time-resolved data, diurnal patterns of the degree of oxygenation of organic aerosols were used to determine the sources and formation processes of the least understood organic portion of PM. The oxygen-to-carbon atomic ratio (O : C) and average carbon oxidation state OS C) showed little variation in autumn and winter, when the long-range transport of oxidized organics dominated, whereas they peaked in the afternoon in spring and summer, when locally produced secondary organic aerosol prevailed. Air mass origin, in contrast, had a strong influence on both NR-PM1 concentrations and the fractions of species in NR-PM1. The findings of the current study provide a better understanding of the role of air mass origin in the seasonal characteristics of the PM composition and the relative importance of local vs. transported organic aerosols in this region.


2015 ◽  
Vol 15 (6) ◽  
pp. 2935-2951 ◽  
Author(s):  
A. Ripoll ◽  
M. C. Minguillón ◽  
J. Pey ◽  
J. L. Jimenez ◽  
D. A. Day ◽  
...  

Abstract. Real-time measurements of inorganic (sulfate, nitrate, ammonium, chloride and black carbon (BC)) and organic submicron aerosols (particles with an aerodynamic diameter of less than 1 μm) from a continental background site (Montsec, MSC, 1570 m a.s.l.) in the western Mediterranean Basin (WMB) were conducted for 10 months (July 2011–April 2012). An aerosol chemical speciation monitor (ACSM) was co-located with other online and offline PM1 measurements. Analyses of the hourly, diurnal, and seasonal variations are presented here, for the first time, for this region. Seasonal trends in PM1 components are attributed to variations in evolution of the planetary boundary layer (PBL) height, air mass origin, and meteorological conditions. In summer, the higher temperature and solar radiation increases convection, enhancing the growth of the PBL and the transport of anthropogenic pollutants towards high altitude sites. Furthermore, the regional recirculation of air masses over the WMB creates a continuous increase in the background concentrations of PM1 components and causes the formation of reservoir layers at relatively high altitudes. The combination of all these atmospheric processes results in a high variability of PM1 components, with poorly defined daily patterns, except for the organic aerosols (OA). OA was mostly composed (up to 90%) of oxygenated organic aerosol (OOA), split in two types: semivolatile (SV-OOA) and low-volatility (LV-OOA), the rest being hydrocarbon-like OA (HOA). The marked diurnal cycles of OA components regardless of the air mass origin indicates that they are not only associated with anthropogenic and long-range-transported secondary OA (SOA) but also with recently produced biogenic SOA. Very different conditions drive the aerosol phenomenology in winter at MSC. The thermal inversions and the lower vertical development of the PBL leave MSC in the free troposphere most of the day, being affected by PBL air masses only after midday, when the mountain breezes transport emissions from the adjacent valleys and plains to the top of the mountain. This results in clear diurnal patterns of both organic and inorganic concentrations. OA was also mainly composed (71%) of OOA, with contributions from HOA (5%) and biomass burning OA (BBOA; 24%). Moreover, in winter sporadic long-range transport from mainland Europe is observed. The results obtained in the present study highlight the importance of SOA formation processes at a remote site such as MSC, especially in summer. Additional research is needed to characterize the sources and processes of SOA formation at remote sites.


2018 ◽  
Vol 18 (4) ◽  
pp. 2973-2983 ◽  
Author(s):  
Christian Rolf ◽  
Bärbel Vogel ◽  
Peter Hoor ◽  
Armin Afchine ◽  
Gebhard Günther ◽  
...  

Abstract. The impact of air masses originating in Asia and influenced by the Asian monsoon anticyclone on the Northern Hemisphere stratosphere is investigated based on in situ measurements. A statistically significant increase in water vapor (H2O) of about 0.5 ppmv (11 %) and methane (CH4) of up to 20 ppbv (1.2 %) in the extratropical stratosphere above a potential temperature of 380 K was detected between August and September 2012 during the HALO aircraft missions Transport and Composition in the UT/LMS (TACTS) and Earth System Model Validation (ESMVal). We investigate the origin of the increased water vapor and methane using the three-dimensional Chemical Lagrangian Model of the Stratosphere (CLaMS). We assign the source of the moist air masses in the Asian region (northern and southern India, eastern China, southeast Asia, and the tropical Pacific) based on tracers of air mass origin used in CLaMS. The water vapor increase is correlated with an increase of the simulated Asian monsoon air mass contribution from about 10 % in August to about 20 % in September, which corresponds to a doubling of the influence from the Asian monsoon region. Additionally, back trajectories starting at the aircraft flight paths are used to differentiate transport from the Asian monsoon anticyclone and other source regions by calculating the Lagrangian cold point (LCP). The geographic location of the LCPs, which indicates the region where the set point of water vapor mixing ratio along these trajectories occurs, can be predominantly attributed to the Asian monsoon region.


2017 ◽  
Vol 74 (4) ◽  
pp. 1201-1210
Author(s):  
Tobias Selz ◽  
Lucas Fischer ◽  
George C. Craig

Abstract The spatial scale dependence of midlatitude water vapor variability in the high-resolution limited-area model COSMO is evaluated using diagnostics of scaling behavior. Past analysis of airborne lidar measurements showed that structure function scaling exponents depend on the corresponding airmass characteristics, and that a classification of the troposphere into convective and nonconvective layers led to significantly different power-law behaviors for each of these two regimes. In particular, scaling properties in the convective air mass were characterized by rough and highly intermittent data series, whereas the nonconvective regime was dominated by smoother structures with weaker small-scale variability. This study finds similar results in a model simulation with an even more pronounced distinction between the two air masses. Quantitative scaling diagnostics agree well with measurements in the nonconvective air mass, whereas in the convective air mass the simulation shows a much higher intermittency. Sensitivity analyses were performed using the model data to assess the impact of limitations of the observational dataset, which indicate that analyses of lidar data most likely underestimated the intermittency in convective air masses due to the small samples from single flight tracks, which led to a bias when data with poor fits were rejected. Though the quantitative estimation of intermittency remains uncertain for convective air masses, the ability of the model to capture the dominant weather regime dependence of water vapor scaling properties is encouraging.


2008 ◽  
Vol 8 (7) ◽  
pp. 1881-1896 ◽  
Author(s):  
M. Santese ◽  
F. De Tomasi ◽  
M. R. Perrone

Abstract. Aerosol products by AERONET sun-sky radiometer measurements combined with air-mass backtrajectories were analyzed to identify source regions and pathways of air masses carrying aerosols to south-east Italy, and to determine the dependence of aerosol mean optical properties on advection patterns. Aerosol optical depth (AOD), fine mode fraction (η ), single scattering albedo (SSA), asymmetry factor (g), and lidar ratio (Lr) at 440 nm were used to characterize aerosol properties. The analysis of 5-day-backtrajectories ending in Lecce on south-east Italy and referring to 240 measurement days of the 2003–2004 years revealed that 32% of the measurement days were characterized by air masses coming from all continental European sources with the exception of Spain. 3% of the measurement days were characterized by air masses coming from both the Southern Mediterranean Sea and the Africa continent, and the Western Mediterranean, the Iberian Peninsula, and the Atlantic Ocean. 62% of the measurement days were characterized by mixed advection patterns. We found that AOD, SSA and g average values were not significantly dependent on air mass source regions. In contrast, η and Lr average values were quite affected by the air mass source region. AOD, &eta, SSA, g, and Lr average values, which were equal to 0.29±0.15, 0.93±0.03, 0.93±0.03, 0.67±0.03, and 72±20 sr, respectively indicated that the aerosol advected from all continental European sources with the exception of Spain, could be considered representative of "continental average aerosol", mostly made of water soluble and a small amount of soot and insoluble components. Polluted-desert dust particles characterized by AOD=0.29±0.05, η=0.72±0.05, SSA=0.94±0.03, g=0.69±0.02, Lr=56±13 sr, were advected over south-east Italy from the Southern Mediterranean Sea and the Africa continent. The Western Mediterranean, the Iberian Peninsula, and the Atlantic Ocean were instead responsible of the advection of maritime-polluted particles, which were characterized by AOD=0.27±0.17, η=0.8±0.1, SSA=0.94±0.03, g=0.67±0.03, Lr=58±24 sr. Hence, we found that the aerosol load over south-east Italy was dominated by moderately-absorbing, fine-mode particles even if it was also affected by the minor contribution of desert and maritime type aerosol. The application of an aerosol mask to the data points retrieved on measurement days characterized by mixed advection patterns, supported last comment


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