scholarly journals First insights into Northern Africa high-altitude background aerosol chemical composition and source influences

2021 ◽  
Author(s):  
Nabil Deabji ◽  
Khanneh Wadinga Fomba ◽  
Souad El Hajjaji ◽  
Abdelwahid Mellouki ◽  
Hartmut Herrmann
Keyword(s):  
Organic Matter ◽  
Chemical Composition ◽  
High Altitude ◽  
Field Measurements ◽  
High Volume ◽  
Ionic Species ◽  
Atmospheric Composition ◽  
Chemical Compositions ◽  
Aerosol Composition ◽  
Aerosol Chemical Composition

Abstract. Field measurements were conducted to determine aerosol chemical composition in a newly established remote high-altitude site in North Africa to investigate the variations in aerosol composition useful in assessing global and regional changes in atmospheric composition. Particulate matter (PM10) filter samples (200) were collected at the Atlas Mohammed V atmospheric observatory (AM5) located in the Middle-Atlas Mountains in Morocco using a high-volume (HV) collector in a 12 h sampling interval from August to December 2017. The chemical composition of the samples was analyzed for trace metals, ions, elemental carbon, organic carbon, aliphatic hydrocarbons, and polycyclic aromatic hydrocarbon (PAHs) content. The results indicate that high-altitudes aerosol composition is influenced by both regional as well as trans-regional transport of emissions. However, local sources play an important role, especially during low wind speed periods, as observed for November and December. Despite the proximity of the site to the Sahara Desert, its influence on the atmospheric composition at this high-altitude site was mainly seasonal and accounted for only 14 % of the sampling duration. Background conditions at this remote site are characterized by low wind speeds (Av. 2.5 m/s) and mass concentrations in the range of 9.8 and 20 µg/m3. The chemical composition is found to be dominated by inorganic elements, mainly suspended dust (47 %) and ionic species (16 %), followed by organic matter (15 %), water content (12 %), and indeterminate mass (9 %). Biogenic organics contributed up to 7 % of the organic matter with high contributions from compounds such as Nonacosane, Heptacosane, and 2-Pentadecanone. The AM5 site is dominated by four main air mass inflow, which often leads to different aerosol chemical compositions. Mineral dust influenced was seasonal and ranged between 20 and 70 % of the PM mass with peaks observed during the summer and was accompanied by high concentrations of SO42− of up to 1.3 µg/m3. During winter, PM10 concentrations are low (

scholarly journals First insights into northern Africa high-altitude background aerosol chemical composition and source influences

2021 ◽  
Vol 21 (24) ◽  
pp. 18147-18174
Author(s):  
Nabil Deabji ◽  
Khanneh Wadinga Fomba ◽  
Souad El Hajjaji ◽  
Abdelwahid Mellouki ◽  
Laurent Poulain ◽  
...  
Keyword(s):  
Organic Matter ◽  
Chemical Composition ◽  
High Altitude ◽  
North Africa ◽  
Mineral Dust ◽  
Water Soluble ◽  
Atmospheric Composition ◽  
Chemical Compositions ◽  
Aerosol Composition ◽  
Aerosol Chemical Composition

Abstract. Field measurements were conducted to determine aerosol chemical composition at a newly established remote high-altitude site in North Africa at the Atlas Mohammed V (AMV) atmospheric observatory located in the Middle Atlas Mountains. The main objectives of the present work are to investigate the variations in the aerosol composition and better assess global and regional changes in atmospheric composition in North Africa. A total of 200 particulate matter (PM10) filter samples were collected at the site using a high-volume (HV) collector in a 12 h sampling interval from August to December 2017. The chemical composition of the samples was analyzed for trace metals, water-soluble ions, organic carbon (OC/EC), aliphatic hydrocarbons, and polycyclic aromatic hydrocarbon (PAH) contents. The results indicate that high-altitude aerosol composition is influenced by both regional and transregional transport of emissions. However, local sources play an important role, especially during low wind speed periods, as observed for November and December. During background conditions characterized by low wind speeds (avg. 3 m s-1) and mass concentrations in the range from 9.8 to 12 μg m-3, the chemical composition is found to be dominated by inorganic elements, mainly suspended dust (61 %) and ionic species (7 %), followed by organic matter (7 %), water content (12 %), and unidentified mass (11 %). Despite the proximity of the site to the Sahara, its influence on the atmospheric composition at this high-altitude site was mainly seasonal and accounted for only 22 % of the sampling duration. Biogenic organics contributed up to 7 % of the organic matter with high contributions from compounds such as heneicosane, hentriacontane, and nonacosane. The AMV site is dominated by four main air mass inflows, which often leads to different aerosol chemical compositions. Mineral dust influence was seasonal and ranged between 21 % and 74 % of the PM mass, with peaks observed during the summer, and was accompanied by high concentrations of SO42- of up to 3.0 μg m-3. During winter, PM10 concentrations are low (<30 μg m-3), the influence of the desert is weaker, and the marine air masses (64 %) are more dominant with a mixture of sea salt and polluted aerosol from the coastal regions (Rabat and Casablanca). During the daytime, mineral dust contribution to PM increased by about 42 % because of road dust resuspension. In contrast, during nighttime, an increase in the concentrations of alkanes, PAHs, alkane-2-ones, and anthropogenic metals such as Pb, Ni, and Cu was found due to variations in the boundary layer height. The results provide the first detailed seasonal and diurnal variation of the aerosol chemical composition, which is valuable for long-term assessment of climate and regional influence of air pollution in North Africa.

Aerosol chemical composition of the middle Atlas region of North Africa

2021 ◽  
Author(s):  
Nabil Deabji ◽  
Khanneh Wadinga Fomba ◽  
Souad El Hajjaji ◽  
Abdelwahid Mellouki ◽  
Hartmut Herrmann
Keyword(s):  
Boundary Layer ◽  
Organic Matter ◽  
Chemical Composition ◽  
High Altitude ◽  
North Africa ◽  
Atmospheric Composition ◽  
North African ◽  
Air Masses ◽  
Middle Atlas ◽  
Aerosol Chemical Composition

&lt;p&gt;Mountain and high-altitude sites provide representative data for the lower free troposphere and various pathways for aerosol interactions, changing boundary layer heights useful in understanding atmospheric composition. However, few studies exist in African regions despite its diversity in both natural and anthropogenic emissions. For this reason, the ATLAS Mohamed V (AM5) observatory in the Middle Atlas region was established to provide the necessary infrastructure for detailed atmospheric studies in the North African high-altitude region. Here, results of a field study conducted to determine the aerosol chemical composition in this region, understand its variations, and importance in assessing global and regional changes in the atmospheric composition is reported. Particulate matter (PM&lt;sub&gt;10&lt;/sub&gt;) filter samples (200) were collected using a high-volume (500l/min) collector in a 12h sampling interval from August to December 2017. The chemical composition of the samples was analyzed for trace metals, ions, elemental carbon, organic carbon, aliphatic hydrocarbons, and polycyclic aromatic hydrocarbon (PAHs) content. The results show that the high-altitude aerosol composition is influenced by regional and transregional transport of different pollutants. Local sources play an important role during periods when the wind speed is low, especially during autumn. Despite the proximity of the site to the Saharan Desert, its influence on the atmospheric composition was mainly seasonal and accounted for only 14% of the sampling duration. The chemical composition was dominated by inorganic elements, mainly suspended dust (47%) and ionic species (16%), and followed by organic matter (15%), water content (12%), and indeterminate mass (9%). Biogenic organics contributed up to 7% of the organic matter with high contributions from compounds such as Nonacosane, Heptacosane, and 2-Pentadecanone. Four main air masses characterized the inflow to the site, which often leads to different aerosol chemical compositions. Mineral dust influenced was seasonal and ranged between 20 and 70% of the PM mass with peaks observed during the summer and was accompanied by high concentrations of SO&lt;sub&gt;4&lt;/sub&gt;&lt;sup&gt;2-&lt;/sup&gt; of up to 1.3 &amp;#181;g/m&amp;#179;. PM&lt;sub&gt;10&lt;/sub&gt; concentrations during winter were low (&lt; 30 &amp;#181;g/m&amp;#179;), with a dominance of marine air masses (53%) carrying aerosols rich in sea salt and polluted anthropogenic aerosols from the coastal regions (Rabat and Casablanca). During the day-time, mineral dust contribution to PM increased by about 42% due to road dust resuspension. In contrast, during night-time, an increase in the concentrations of PAHs, ketones, and anthropogenic metals such as Pb, Ni, and Cu was found due to variations in the boundary layer height. The results provide first insights into typical North African high-altitude background aerosol chemical composition useful for long-term assessment of climate and regional influence of air pollution in North Africa.&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;

Source identification of aerosol chemical composition in the Atlas region of North Africa.

2021 ◽  
Author(s):  
Nabil Deabji ◽  
Khanneh Wadinga Fomba ◽  
Eduardo José dos Santos Souza ◽  
Hartmut Herrmann
Keyword(s):  
High Altitude ◽  
Complex Mixture ◽  
Saharan Dust ◽  
Atmospheric Composition ◽  
Urban Site ◽  
Chemical Components ◽  
Research Station ◽  
African Region ◽  
Aerosol Composition ◽  
The Impact

&lt;p&gt;Aerosol particles are important constituents of the atmosphere due to their role in controlling climate-related processes. In addition, their impacts on air quality and human health make it essential to study. However, the characterization and the identification of natural and anthropogenic atmospheric particles can be challenging due to the complex mixture occurring during atmospheric transport. Background locations such as high-altitude sites provide valuable infrastructure for obtaining representative data for understanding various pathways for aerosol interactions useful in assessing atmospheric composition. However, information about aerosol characteristics at high-altitude in the African regions and their relation to urban aerosol composition is still not well understood. In the present study, PM&lt;sub&gt;10&lt;/sub&gt; and PM&lt;sub&gt;2.5&lt;/sub&gt; particulate matter was characterized at two different sites in the North African region of Morocco. A background site located at the newly established AM5 research station in the Middle Atlas region at an altitude of 2100 m and an urban site situated in a polluted city, Fez. The goal was to determine chemical components, evaluate Saharan dust&amp;#8217;s role on the PM10 concentrations between the sites, and assess the impact of urban pollution on background aerosol composition. The results indicate that the background aerosol composition is influenced by both regional and trans-regional transport. Despite the site's proximity to the Sahara Desert, the deserts influence on the atmospheric composition was observed for only 22% of the time and this was mainly seasonal. Marine air masses were more dominant with a mixture of sea salt and polluted aerosol from the coastal regions especially during wintertime. Furthermore, high concentrations of mineral dust were observed during the daytime due to the resuspension of road dust. At the same time, an increase of PAHs and anthropogenic metals such as Pb, Ni, and Cu were found during the nighttime because of the boundary layer variation. The Fez's urban site is characterized by a high contribution of elemental carbon (6%) and organic biomass tracers (3%) such as Levoglucosane and 4-nitrophenol.&lt;/p&gt;

scholarly journals Using different assumptions of aerosol mixing state and chemical composition to predict CCN concentrations based on field measurements in urban Beijing

2018 ◽  
Vol 18 (9) ◽  
pp. 6907-6921 ◽  
Author(s):  
Jingye Ren ◽  
Fang Zhang ◽  
Yuying Wang ◽  
Don Collins ◽  
Xinxin Fan ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Black Carbon ◽  
Cloud Condensation Nuclei ◽  
Field Measurements ◽  
Minor Role ◽  
Mixing State ◽  
Mixing Processes ◽  
Size Dependent ◽  
Aerosol Mixing State ◽  
Aerosol Chemical Composition

Abstract. Understanding the impacts of aerosol chemical composition and mixing state on cloud condensation nuclei (CCN) activity in polluted areas is crucial for accurately predicting CCN number concentrations (NCCN). In this study, we predict NCCN under five assumed schemes of aerosol chemical composition and mixing state based on field measurements in Beijing during the winter of 2016. Our results show that the best closure is achieved with the assumption of size dependent chemical composition for which sulfate, nitrate, secondary organic aerosols, and aged black carbon are internally mixed with each other but externally mixed with primary organic aerosol and fresh black carbon (external–internal size-resolved, abbreviated as EI–SR scheme). The resulting ratios of predicted-to-measured NCCN (RCCN_p∕m) were 0.90 – 0.98 under both clean and polluted conditions. Assumption of an internal mixture and bulk chemical composition (INT–BK scheme) shows good closure with RCCN_p∕m of 1.0 –1.16 under clean conditions, implying that it is adequate for CCN prediction in continental clean regions. On polluted days, assuming the aerosol is internally mixed and has a chemical composition that is size dependent (INT–SR scheme) achieves better closure than the INT–BK scheme due to the heterogeneity and variation in particle composition at different sizes. The improved closure achieved using the EI–SR and INT–SR assumptions highlight the importance of measuring size-resolved chemical composition for CCN predictions in polluted regions. NCCN is significantly underestimated (with RCCN_p∕m of 0.66 – 0.75) when using the schemes of external mixtures with bulk (EXT–BK scheme) or size-resolved composition (EXT–SR scheme), implying that primary particles experience rapid aging and physical mixing processes in urban Beijing. However, our results show that the aerosol mixing state plays a minor role in CCN prediction when the κorg exceeds 0.1.

scholarly journals Characterization of aerosol chemical composition with aerosol mass spectrometry in Central Europe: an overview

2010 ◽  
Vol 10 (21) ◽  
pp. 10453-10471 ◽  
Author(s):  
V. A. Lanz ◽  
A. S. H. Prévôt ◽  
M. R. Alfarra ◽  
S. Weimer ◽  
C. Mohr ◽  
...  
Keyword(s):  
Mass Spectrometry ◽  
Chemical Composition ◽  
Organic Aerosol ◽  
Volatile Fraction ◽  
Aerosol Composition ◽  
Aerosol Mass ◽  
Aerosol Mass Spectrometry ◽  
Field Campaigns ◽  
Alpine Valleys ◽  
Aerosol Chemical Composition

Abstract. Real-time measurements of non-refractory submicron aerosols (NR-PM1) were conducted within the greater Alpine region (Switzerland, Germany, Austria, France and Liechtenstein) during several week-long field campaigns in 2002–2009. This region represents one of the most important economic and recreational spaces in Europe. A large variety of sites was covered including urban backgrounds, motorways, rural, remote, and high-alpine stations, and also mobile on-road measurements were performed. Inorganic and organic aerosol (OA) fractions were determined by means of aerosol mass spectrometry (AMS). The data originating from 13 different field campaigns and the combined data have been utilized for providing an improved temporal and spatial data coverage. The average mass concentration of NR-PM1 for the different campaigns typically ranged between 10 and 30 μg m−3. Overall, the organic portion was most abundant, ranging from 36% to 81% of NR-PM1. Other main constituents comprised ammonium (5–15%), nitrate (8–36%), sulfate (3–26%), and chloride (0–5%). These latter anions were, on average, fully neutralized by ammonium. As a major result, time of the year (winter vs. summer) and location of the site (Alpine valleys vs. Plateau) could largely explain the variability in aerosol chemical composition for the different campaigns and were found to be better descriptors for aerosol composition than the type of site (urban, rural etc.). Thus, a reassessment of classifications of measurements sites might be considered in the future, possibly also for other regions of the world. The OA data was further analyzed using positive matrix factorization (PMF) and the multi-linear engine ME (factor analysis) separating the total OA into its underlying components, such as oxygenated (mostly secondary) organic aerosol (OOA), hydrocarbon-like and freshly emitted organic aerosol (HOA), as well as OA from biomass burning (BBOA). OOA was ubiquitous, ranged between 36% and 94% of OA, and could be separated into a low-volatility and a semi-volatile fraction (LV-OOA and SV-OOA) for all summer campaigns at low altitude sites. Wood combustion (BBOA) accounted for a considerable fraction during wintertime (17–49% OA), particularly in narrow Alpine valleys BBOA was often the most abundant OA component. HOA/OA ratios were comparatively low for all campaigns (6–16%) with the exception of on-road, mobile measurements (23%) in the Rhine Valley. The abundance of the aerosol components and the retrievability of SV-OOA and LV-OOA are discussed in the light of atmospheric chemistry and physics.

scholarly journals Size-resolved aerosol composition and link to hygroscopicity at a forested site in Colorado

2013 ◽  
Vol 13 (9) ◽  
pp. 23817-23843 ◽  
Author(s):  
E. J. T. Levin ◽  
A. J. Prenni ◽  
B. Palm ◽  
D. Day ◽  
P. Campuzano-Jost ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Cloud Condensation Nuclei ◽  
Cloud Droplet ◽  
Large Mass ◽  
Aerosol Composition ◽  
Aerosol Mass Spectrometer ◽  
Aerosol Mass ◽  
Mass Fractions ◽  
Aerosol Hygroscopicity ◽  
Aerosol Chemical Composition

Abstract. Aerosol hygroscopicity describes the ability of a particle to take up water and form a cloud droplet. Modeling studies have shown sensitivity of precipitation-producing cloud systems to the availability of aerosol particles capable of serving as cloud condensation nuclei (CCN), and hygroscopicity is a key parameter controlling the number of available CCN. Continental aerosol is typically assumed to have a representative hygroscopicity parameter, κ, of 0.3; however, in remote locations this value can be lower due to relatively large mass fractions of organic components. To further our understanding of aerosol properties in remote areas, we measured size-resolved aerosol chemical composition and hygroscopicity in a forested, mountainous site in Colorado during the six-week BEACHON-RoMBAS campaign. This campaign followed a year-long measurement period at this site, and results from the intensive campaign shed light on the previously reported seasonal cycle in aerosol hygroscopicity. New particle formation events were observed routinely at this site and nucleation mode composition measurements indicated that the newly formed particles were predominantly organic. These events likely contribute to the dominance of organic species at smaller sizes, where aerosol organic mass fractions of non-refractory components were between 70–90%. Corresponding aerosol hygroscopicity was observed to range from κ = 0.15–0.22, with hygroscopicity increasing with particle size. Aerosol chemical composition measured by an Aerosol Mass Spectrometer and calculated from hygroscopicity measurements agreed very well during the intensive study with an assumed value of κorg = 0.13 resulting in the best agreement.

scholarly journals Offline analysis of the chemical composition and hygroscopicity of sub-micrometer aerosol at an Asian outflow receptor site and comparison with online measurements

2021 ◽  
Author(s):  
Yange Deng ◽  
Hiroaki Fujinari ◽  
Hikari Yai ◽  
Kojiro Shimada ◽  
Yuzo Miyazaki ◽  
...  
Keyword(s):  
Organic Matter ◽  
Chemical Composition ◽  
East Asian ◽  
Receptor Site ◽  
Water Soluble ◽  
Inorganic Salts ◽  
Chemical Compositions ◽  
Online Analysis ◽  
Offline Analysis ◽  
Aerosol Hygroscopicity

Abstract. Filter-based offline analysis of atmospheric aerosol hygroscopicity coupled to composition analysis provides information complementary to that obtained from online analysis. However, its application itself and comparison to online analysis have remained limited to date. In this study, daily submicrometer aerosol particles (PM0.95, 50 % cutoff diameter: 0.95 μm) were collected onto quartz fiber filters in Okinawa Island, a receptor of East Asian outflow, in the autumn of 2015. The chemical composition of water-soluble matter (WSM) in PM0.95 and PM0.95 itself, and their respective hygroscopicities were characterized through the offline use of an aerosol mass spectrometer and a hygroscopicity tandem differential mobility analyzer. Thereafter, results were compared with those obtained from online analyses. Sulfate dominated the WSM mass (60 %), followed by water-soluble organic matter (WSOM, 20 %) and ammonium (13 %). WSOM accounted for most (93 %) of the mass of extracted organic matter (EOM) and the atomic O to C ratios (O : C) of WSOM and EOM were high (mean ± standard deviation were, respectively, 0.84 ± 0.08 and 0.79 ± 0.08), both of which indicate highly aged characteristics of the observed aerosol. The hygroscopic growth curves showed clear hysteresis for most samples. At 85 % RH, the calculated hygroscopicity parameter κ of the WSM (κWSM), WSOM, EOM, and PM0.95 (κPM0.95) were, respectively, 0.50 ± 0.03, 0.22 ± 0.12, 0.20 ± 0.11, and 0.47 ± 0.03. An analysis using the thermodynamic E-AIM model shows, on average, that inorganic salts and WSOM respectively contributed 88 % and 12 % of the κWSM (or κPM0.95). High similarities were found between offline and online analysis for chemical compositions that are related to particle hygroscopicity (the mass fractions and O : C of organics, and the degree of neutralization), and also for aerosol hygroscopicity. As possible factors governing the variation of κWSM, the influences of WSOM abundance and the neutralization of inorganic salts were assessed. At high RH (70–90 %), the hygroscopicity of WSM and PM0.95 was affected considerably by the presence of organic components; at low RH (20–50 %), the degree of neutralization could be important. This study not only characterized aerosol hygroscopicity at the receptor site of East Asian outflow, but also shows that the offline hygroscopicity analysis is an appropriate method, at least for aerosols of the studied type. The results encourage further applications to other environments and to more in-depth hygroscopicity analysis, in particular for organic fractions.

scholarly journals Chemical composition of PM<sub>10</sub> and PM<sub>1</sub> at the high-altitude Himalayan station Nepal Climate Observatory-Pyramid (NCO-P) (5079 m a.s.l.)

2009 ◽  
Vol 9 (6) ◽  
pp. 25487-25522 ◽  
Author(s):  
S. Decesari ◽  
M. C. Facchini ◽  
C. Carbone ◽  
L. Giulianelli ◽  
M. Rinaldi ◽  
...  
Keyword(s):  
Organic Matter ◽  
Chemical Composition ◽  
High Altitude ◽  
Seasonal Cycle ◽  
Mineral Dust ◽  
Monsoon Season ◽  
Optically Active ◽  
Moist Convection ◽  
Anthropogenic Aerosols ◽  
High Himalayas

Abstract. We report chemical composition data for PM10 and PM1 from the Nepal Climate Observatory-Pyramid (NCO-P), the world's highest aerosol observatory, located at 5079 m a.s.l. at the foothills of Mt. Everest. Despite its high altitude, the average PM10 mass apportioned by the chemical analyses is of the order of 6 μg m−3 (i.e., 10 μg/scm), with almost a half of this mass accounted for by organic matter, elemental carbon (EC) and inorganic ions, the rest being mineral dust. Organic matter, in particular, accounted for by 2.0 μg m−3 (i.e., 3.6 μg/scm) on a yearly basis, and it is by far the major PM10 component beside mineral oxides. Non-negligible concentrations of EC were also observed (0.36 μg/scm), confirming that optically-active aerosol produced from combustion sources can be efficiently transported up the altitudes of Himalayan glaciers. The concentrations of carbonaceous and ionic aerosols follow a common time trend with a maximum in the premonsoon season, a minimum during the monsoon and a slow "ramp-up" period in the postmonsoon and dry seasons, which is the same phenomenology observed for other Nepalese Himalayan sites in previous studies. Such seasonal cycle can be explained by the seasonal variations of dry and moist convection and of wet scavenging processes characterizing the climate of north Indian subcontinent. We document the effect of orographic transport of carbonaceous and sulphate particles upslope the Himalayas, showing that the valley breeze circulation, which is almost permanently active during the out-of-monsoon season, greatly impacts the chemical composition of PM10 and PM1 in the high Himalayas and provides an efficient mechanism for bringing anthropogenic optically-active aerosols into the Asian upper troposphere (>5000 m a.s.l.). The concentrations of mineral dust are impacted to a smaller extent by valley breezes and follow a unique seasonal cycle which suggest multiple source areas in central and south-west Asia. Our findings, based on two years of observations of the aerosol chemical composition, provide clear evidence that the southern side of the high Himalayas are impacted by transport of anthropogenic aerosols which constitute the Asian brown cloud.

scholarly journals Change in global aerosol composition since preindustrial times

2006 ◽  
Vol 6 (3) ◽  
pp. 5585-5628 ◽  
Author(s):  
K. Tsigaridis ◽  
M. Krol ◽  
F. J. Dentener ◽  
Y. Balkanski ◽  
J. Lathière ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Atmospheric Aerosols ◽  
Transport Model ◽  
Sea Salt ◽  
Carbonaceous Aerosol ◽  
Aerosol Formation ◽  
Aerosol Composition ◽  
Aerosol Mass ◽  
Composition Changes ◽  
Aerosol Chemical Composition

Abstract. To elucidate human induced changes of aerosol load and composition in the atmosphere, a coupled aerosol and gas-phase chemistry transport model of the troposphere and lower stratosphere has been used. This is the first 3-d modeling study that focuses on aerosol chemical composition change since preindustrial times considering the secondary organic aerosol formation together with all other main aerosol components including nitrate. In particular, we evaluate non-sea-salt sulfate (nss-SO4=), ammonium (NH4+), nitrate (NO3-), black carbon (BC), sea-salt, dust, primary and secondary organics (POA and SOA) with a focus on the importance of secondary organic aerosols. Our calculations show that the aerosol optical depth (AOD) has increased by about 21% since preindustrial times. This enhancement of AOD is attributed to a rise in the atmospheric load of BC, nss-SO4=, NO3-, POA and SOA by factors of 3.3, 2.6, 2.7, 2.3 and 1.2, respectively, whereas we assumed that the natural dust and sea-salt sources remained constant. The nowadays increase in carbonaceous aerosol loading is dampened by a 34–42% faster conversion of hydrophobic to hydrophilic carbonaceous aerosol leading to higher removal rates. These changes between the various aerosol components resulted in significant modifications of the aerosol chemical composition. The relative importance of the various aerosol components is critical for the aerosol climatic effect, since atmospheric aerosols behave differently when their chemical composition changes. According to this study, the aerosol composition changed significantly over the different continents and with height since preindustrial times. The presence of anthropogenically emitted primary particles in the atmosphere facilitates the condensation of the semi-volatile species that form SOA onto the aerosol phase, particularly in the boundary layer. The SOA burden that is dominated by the natural component has increased by 24% while its contribution to the AOD has increased by 11%. The increase in oxidant levels and preexisting aerosol mass since preindustrial times is the reason of the burden change, since emissions have not changed significantly. The computed aerosol composition changes translate into about 2.5 times more water associated with non sea-salt aerosol. Additionally, aerosols contain 2.7 times more inorganic components nowadays than during the preindustrial times. We find that the increase in emissions of inorganic aerosol precursors is much larger than the corresponding aerosol increase, reflecting a non-linear atmospheric response.

scholarly journals Estimation of aerosol water and chemical composition from AERONET Sun–sky radiometer measurements at Cabauw, the Netherlands

2014 ◽  
Vol 14 (12) ◽  
pp. 5969-5987 ◽  
Author(s):  
A. J. van Beelen ◽  
G. J. H. Roelofs ◽  
O. P. Hasekamp ◽  
J. S. Henzing ◽  
T. Röckmann
Keyword(s):  
Refractive Index ◽  
Organic Matter ◽  
Chemical Composition ◽  
Relative Humidity ◽  
Volume Fraction ◽  
Inorganic Salts ◽  
Water Volume ◽  
Aerosol Composition ◽  
Water Volume Fraction ◽  
The Individual

Abstract. Remote sensing of aerosols provides important information on atmospheric aerosol abundance. However, due to the hygroscopic nature of aerosol particles observed aerosol optical properties are influenced by atmospheric humidity, and the measurements do not unambiguously characterize the aerosol dry mass and composition, which complicates the comparison with aerosol models. In this study we derive aerosol water and chemical composition by a modeling approach that combines individual measurements of remotely sensed aerosol properties (e.g., optical thickness, single-scattering albedo, refractive index and size distribution) from an AERONET (Aerosol Robotic Network) Sun–sky radiometer with radiosonde measurements of relative humidity. The model simulates water uptake by aerosols based on the chemical composition (e.g., sulfates, ammonium, nitrate, organic matter and black carbon) and size distribution. A minimization method is used to calculate aerosol composition and concentration, which are then compared to in situ measurements from the Intensive Measurement Campaign At the Cabauw Tower (IMPACT, May 2008, the Netherlands). Computed concentrations show good agreement with campaign-average (i.e., 1–14 May) surface observations (mean bias is 3% for PM10 and 4–25% for the individual compounds). They follow the day-to-day (synoptic) variability in the observations and are in reasonable agreement for daily average concentrations (i.e., mean bias is 5% for PM10 and black carbon, 10% for the inorganic salts and 18% for organic matter; root-mean-squared deviations are 26% for PM10 and 35–45% for the individual compounds). The modeled water volume fraction is highly variable and strongly dependent on composition. During this campaign we find that it is >0.5 at approximately 80% relative humidity (RH) when the aerosol composition is dominated by hygroscopic inorganic salts, and <0.1 when RH is below 40%, especially when the composition is dominated by less hygroscopic compounds such as organic matter. The scattering enhancement factor (f(RH), the ratio of the scattering coefficient at 85% RH and its dry value at 676 nm) during 1–14 May is 2.6 ± 0.5. The uncertainty in AERONET (real) refractive index (0.025–0.05) is the largest source of uncertainty in the modeled aerosol composition and leads to an uncertainty of 0.1–0.25 (50–100%) in aerosol water volume fraction. Our methodology performs relatively well at Cabauw, but a better performance may be expected for regions with higher aerosol loading where the uncertainties in the AERONET inversions are smaller.

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