Chemical composition and source apportionment of atmospheric aerosols on the Namibian coast

Abstract. The chemical composition of aerosols is of particular importance to assess their interactions with radiation, clouds and trace gases in the atmosphere and consequently their effects on air quality and the regional climate. In this study, we present the results of the first long-term dataset of the aerosol chemical composition at an observatory on the coast of Namibia, facing the south-eastern Atlantic Ocean. Aerosol samples in the mass fraction of particles smaller than 10 µm in aerodynamic diameter (PM10) were collected during 26 weeks between 2016 and 2017 at the ground-based Henties Bay Aerosol Observatory (HBAO; 22∘6′ S, 14∘30′ E; 30 m above mean sea level). The resulting 385 filter samples were analysed by X-ray fluorescence and ion chromatography for 24 inorganic elements and 15 water-soluble ions. Statistical analysis by positive matrix factorisation (PMF) identified five major components, sea salt (mass concentration: 74.7±1.9 %), mineral dust (15.7±1.4 %,), ammonium neutralised (6.1±0.7 %), fugitive dust (2.6±0.2 %) and industry (0.9±0.7 %). While the contribution of sea salt aerosol was persistent, as the dominant wind direction was south-westerly and westerly from the open ocean, the occurrence of mineral dust was episodic and coincided with high wind speeds from the south-south-east and the north-north-west, along the coastline. Concentrations of heavy metals measured at HBAO were higher than reported in the literature from measurements over the open ocean. V, Cd, Pb and Nd were attributed to fugitive dust emitted from bare surfaces or mining activities. As, Zn, Cu, Ni and Sr were attributed to the combustion of heavy oils in commercial ship traffic across the Cape of Good Hope sea route, power generation, smelting and other industrial activities in the greater region. Fluoride concentrations up to 25 µg m−3 were measured, as in heavily polluted areas in China. This is surprising and a worrisome result that has profound health implications and deserves further investigation. Although no clear signature for biomass burning could be determined, the PMF ammonium-neutralised component was described by a mixture of aerosols typically emitted by biomass burning, but also by other biogenic activities. Episodic contributions with moderate correlations between NO3-, nss-SO42- (higher than 2 µg m−3) and nss-K+ were observed, further indicative of the potential for an episodic source of biomass burning. Sea salt accounted for up to 57 % of the measured mass concentrations of SO42-, and the non-sea salt fraction was contributed mainly by the ammonium-neutralised component and small contributions from the mineral dust component. The marine biogenic contribution to the ammonium-neutralised component is attributed to efficient oxidation in the moist marine atmosphere of sulfur-containing gas phase emitted by marine phytoplankton in the fertile waters offshore in the Benguela Upwelling System. The data presented in this paper provide the first ever information on the temporal variability of aerosol concentrations in the Namibian marine boundary layer. This data also provide context for intensive observations in the area.

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Chemical composition and source apportionment of atmospheric aerosols on the Namibian coast

10.5194/acp-2020-388 ◽

2020 ◽

Author(s):

Danitza Klopper ◽

Paola Formenti ◽

Andreas Namwoonde ◽

Mathieu Cazaunau ◽

Servanne Chevaillier ◽

...

Keyword(s):

Heavy Metals ◽

Chemical Composition ◽

Biomass Burning ◽

Mineral Dust ◽

Open Ocean ◽

Sea Salt ◽

Water Soluble ◽

Marine Phytoplankton ◽

Back Trajectory ◽

Secondary Products

Abstract. The chemical composition of aerosols is of particular importance to assess their interactions with radiation, clouds and trace gases in the atmosphere, and consequently their effects on air quality and the regional climate. In this study, we present the results of the first long-term dataset of the aerosol chemical composition at an observatory on the coast of Namibia, facing the southeast Atlantic Ocean. Aerosol samples in the mass fraction of particles smaller than 10 µm in aerodynamic diameter (PM10) were collected during 26 weeks between 2016 and 2017 at the ground-based Henties Bay Aerosol Observatory (HBAO; 22°6’ S, 14°30’ E, 30 m above mean sea level). The resulting 385 filter samples were analysed by X-ray fluorescence and ion-chromatography for 24 inorganic elements and 15 water-soluble ions. Statistical analysis by positive matrix factorization and back-trajectory modelling identified five major sources, sea salt (mass concentration: 70.8 ± 0.2 %), marine biogenic (13.5 ± 0.8 %), mineral dust (9.9 ± 0.1 %), secondary products (3.2 ± 1.0 %) and heavy metals (2.3 ± 2.5 %). While the contribution of sea salt aerosol was persistent, as the dominant wind direction was south-westerly and westerly from the open ocean, the occurrence of mineral dust was episodic and coincided with high wind speeds from the south-southeast and the north-northwest, along the coastline. Concentrations of heavy metals measured at HBAO were higher than reported in the literature from measurements over the open ocean. The heavy metals (V, Cr, Nd and Mn) measured at the site were attributed to mining activities and the combustion of heavy fuels in commercial ship traffic across the Cape of Good Hope sea route. Fluoride concentrations up to 25 µg m−3 were measured, as in heavily polluted areas in China. This is surprising and a worrisome result that has profound health implications and deserves further investigation. Although no clear signature for biomass burning could be determined, the source of secondary products identified by PMF was described by a mixture of aerosols typically emitted by biomass burning, but also by other biogenic activities. Episodic contributions with moderate correlations between NO3−, nss-SO42− (higher than 2 µg m−3) and nss-K+, were observed, further indicative of the potential for an episodic source of biomass burning. Sea salt accounted for up to 57 % of the measured mass concentrations of SO42− and the non-sea salt fraction contributed mainly to the secondary product and marine biogenic sources identified by PMF. The marine biogenic contribution is attributed to efficient oxidation in the moist marine atmosphere of sulphur-containing gas-phase emitted by marine phytoplankton in the fertile waters offshore in the Benguela Upwelling System. The data presented in this paper provide first-ever information on the temporal variability of aerosol concentrations in the Namibian marine boundary layer and the links to meteorological conditions shaping the transport patterns of aerosols from different sources. This data can be used to provide context for intensive observations in the area.

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Seasonal Variation in Chemical Composition of Size-Segregated Aerosols Over the Northeastern Arabian Sea

Frontiers in Environmental Science ◽

10.3389/fenvs.2020.619174 ◽

2021 ◽

Vol 8 ◽

Author(s):

Ankush Kaushik ◽

Ashwini Kumar ◽

M. A Aswini ◽

P. P. Panda ◽

Garima Shukla ◽

...

Keyword(s):

Chemical Composition ◽

Arabian Sea ◽

Mineral Dust ◽

Sea Salt ◽

Water Soluble ◽

Post Monsoon ◽

Chloride Depletion ◽

Inorganic Species ◽

The Impact

Water-soluble species constitute a significant fraction (up to 60–70%) of the total aerosol loading in the marine atmospheric boundary layer (MABL). The “indirect” effects, that is, climate forcing due to modification of cloud properties depend on the water-soluble composition of aerosols. Thus, the characterization of aerosols over the MABL is of greater relevance. Here, we present 1-year long aerosol chemical composition data of PM10 and PM2.5 at a costal location in the northeastern Arabian Sea (Goa; 15.45°N, 73.20°E, 56 m above the sea level). Average water-soluble ionic concentration (sum of anion and cation) is highest (25.5 ± 6.9 and 19.6 ± 5.8 μg·m−3 for PM10 and PM2.5, respectively) during winter season and lowest during post-monsoon (17.3 ± 9.1 and 14.4 ± 8.1 μg·m−3 for PM10 and PM2.5, respectively). Among water-soluble ionic spices, SO42- ion was found to be dominant species in anions and NH4+ is dominant in cations, for both PM10 and PM2.5 during all the seasons. These observations clearly hint to the contribution from anthropogenic emission and significant secondary inorganic species formation. Sea-salt (calculated based on Na+ and Cl−) concentration shows significant temporal variability with highest contribution during summer seasons in both fractions. Sea-salt corrected Ca2+, an indicator of mineral dust is found mostly during summer months, particularly in PM10 samples, indicates contribution from mineral dust emissions from arid/semiarid regions located in the north/northwestern India and southwest Asia. These observations are corroborated with back-trajectory analyses, wherein air parcels were found to derive from the desert area in summer and Indo-Gangetic Plains (a hot spot for anthropogenic emissions) during winter. In addition, we also observe the presence of nss-K+ (sea-salt corrected), for PM2.5, particularly during winter months, indicating influence of biomass burning emissions. The impact on aerosol chemistry is further assessed based on chloride depletion. Chloride depletion is observed very significant during post-monsoon months (October and November), wherein more than 80 up to 100% depletion is found, mediated by excess sulfates highlighting the role of secondary species in atmospheric chemistry. Regional scale characterization of atmospheric aerosols is important for their better parameterization in chemical transport model and estimation of radiative forcing.

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Remote sensing of aerosols by synergy of caliop and modis

EPJ Web of Conferences ◽

10.1051/epjconf/201817608012 ◽

2018 ◽

Vol 176 ◽

pp. 08012

Author(s):

Rei Kudo ◽

Tomoaki Nishizawa ◽

Akiko Higurashi ◽

Eiji Oikawa

Keyword(s):

Remote Sensing ◽

Biomass Burning ◽

Sea Salt ◽

Water Soluble ◽

Dust Particles ◽

Vertical Profiles ◽

Dust Event ◽

Carbonaceous Particles ◽

The Individual ◽

Better Than

For the monitoring of the global 3-D distribution of aerosol components, we developed the method to retrieve the vertical profiles of water-soluble, light absorbing carbonaceous, dust, and sea salt particles by the synergy of CALIOP and MODIS data. The aerosol product from the synergistic method is expected to be better than the individual products of CALIOP and MODIS. We applied the method to the biomass-burning event in Africa and the dust event in West Asia. The reasonable results were obtained; the much amount of the water-soluble and light absorbing carbonaceous particles were estimated in the biomass-burning event, and the dust particles were estimated in the dust event.

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Analysis of CCN activity of Arctic aerosol and Canadian biomass burning during summer 2008

Atmospheric Chemistry and Physics ◽

10.5194/acp-13-2735-2013 ◽

2013 ◽

Vol 13 (5) ◽

pp. 2735-2756 ◽

Cited By ~ 92

Author(s):

T. L. Lathem ◽

A. J. Beyersdorf ◽

K. L. Thornhill ◽

E. L. Winstead ◽

M. J. Cubison ◽

...

Keyword(s):

Chemical Composition ◽

Biomass Burning ◽

Industrial Pollution ◽

Physical Aging ◽

Volume Fraction ◽

Cloud Condensation Nuclei ◽

Water Soluble ◽

The Arctic ◽

High Concentration ◽

Air Masses

Abstract. The NASA DC-8 aircraft characterized the aerosol properties, chemical composition, and cloud condensation nuclei (CCN) concentrations of the summertime Arctic during the 2008 NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. Air masses characteristic of fresh and aged biomass burning, boreal forest, Arctic background, and anthropogenic industrial pollution were sampled. Observations were spatially extensive (50–85° N and 40–130° W) and exhibit significant variability in aerosol and CCN concentrations. The chemical composition was dominated by highly oxidized organics (66–94% by volume), with a water-soluble mass fraction of more than 50%. The aerosol hygroscopicity parameter, κ, ranged between κ = 0.08–0.32 for all air mass types. Industrial pollution had the lowest κ of 0.08 ± 0.01, while the Arctic background had the highest and most variable κ of 0.32 ± 0.21, resulting from a lower and more variable organic fraction. Both fresh and aged (long-range transported) biomass burning air masses exhibited remarkably similar κ (0.18 ± 0.13), consistent with observed rapid chemical and physical aging of smoke emissions in the atmosphere, even in the vicinity of fresh fires. The organic hygroscopicity (κorg) was parameterized by the volume fraction of water-soluble organic matter (εWSOM), with a κ = 0.12, such that κorg = 0.12εWSOM. Assuming bulk (size-independent) composition and including the κorg parameterization enabled CCN predictions to within 30% accuracy for nearly all environments sampled. The only exception was for industrial pollution from Canadian oil sands exploration, where an external mixture and size-dependent composition was required. Aerosol mixing state assumptions (internal vs. external) in all other environments did not significantly affect CCN predictions; however, the external mixing assumption provided the best results, even though the available observations could not determine the true degree of external mixing and therefore may not always be representative of the environments sampled. No correlation was observed between κorg and O : C. A novel correction of the CCN instrument supersaturation for water vapor depletion, resulting from high concentrations of CCN, was also employed. This correction was especially important for fresh biomass burning plumes where concentrations exceeded 1.5×104 cm−3 and introduced supersaturation depletions of &geq;25%. Not accounting for supersaturation depletion in these high concentration environments would therefore bias CCN closure up to 25% and inferred κ by up to 50%.

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Optical, physical and chemical characteristics of Australian continental aerosols: results from a field experiment

Atmospheric Chemistry and Physics ◽

10.5194/acp-10-5925-2010 ◽

2010 ◽

Vol 10 (13) ◽

pp. 5925-5942 ◽

Cited By ~ 24

Author(s):

M. Radhi ◽

M. A. Box ◽

G. P. Box ◽

R. M. Mitchell ◽

D. D. Cohen ◽

...

Keyword(s):

Northern Hemisphere ◽

Ion Chromatography ◽

Biomass Burning ◽

Mineral Dust ◽

Ion Beam ◽

Water Soluble ◽

Size Distributions ◽

Ion Beam Analysis ◽

Beam Analysis ◽

Scatter Plots

Abstract. Mineral dust is one of the major components of the world's aerosol mix, having a number of impacts within the Earth system. However, the climate forcing impact of mineral dust is currently poorly constrained, with even its sign uncertain. As Australian deserts are more reddish than those in the Northern Hemisphere, it is important to better understand the physical, chemical and optical properties of this important aerosol. We have investigated the properties of Australian desert dust at a site in SW Queensland, which is strongly influenced by both dust and biomass burning aerosol. Three years of ground-based monitoring of spectral optical thickness has provided a statistical picture of gross aerosol properties. The aerosol optical depth data showed a clear though moderate seasonal cycle with an annual mean of 0.06 ± 0.03. The Angstrom coefficient showed a stronger cycle, indicating the influence of the winter-spring burning season in Australia's north. AERONET size distributions showed a generally bimodal character, with the coarse mode assumed to be mineral dust, and the fine mode a mixture of fine dust, biomass burning and marine biogenic material. In November 2006 we undertook a field campaign which collected 4 sets of size-resolved aerosol samples for laboratory analysis – ion beam analysis and ion chromatography. Ion beam analysis was used to determine the elemental composition of all filter samples, although elemental ratios were considered the most reliable output. Scatter plots showed that Fe, Al and Ti were well correlated with Si, and Co reasonably well correlated with Si, with the Fe/Al ratio somewhat higher than values reported from Northern Hemisphere sites (as expected). Scatter plots for Ca, Mn and K against Si showed clear evidence of a second population, which in some cases could be identified with a particular sample day or size fraction. These data may be used to attempt to build a signature of soil in this region of the Australian interior. Ion chromatography was used to quantify water soluble ions for 2 of our sample sets, complementing the picture provided by ion beam analysis. The strong similarities between the MSA and SO42− size distributions argue strongly for a marine origin of much of the SO42−. The similarity of the Na+, Cl− and Mg2+ size distributions also argue for a marine contribution. Further, we believe that both NO3− and NH4+ are the result of surface reactions with appropriate gases.

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Investigation of aged aerosols in size-resolved Asian dust storm particles transported from Beijing, China to Incheon, Korea using low-<i>Z</i> particle EPMA

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-13-27971-2013 ◽

2013 ◽

Vol 13 (10) ◽

pp. 27971-28016 ◽

Cited By ~ 1

Author(s):

H. Geng ◽

H. J. Hwang ◽

X. Liu ◽

S. Dong ◽

C.-U. Ro

Keyword(s):

Organic Carbon ◽

Dust Storm ◽

Aging Process ◽

Mineral Dust ◽

Asian Dust ◽

Sea Salt ◽

Water Soluble ◽

The Yellow Sea ◽

Asian Dust Storm ◽

Beijing China

Abstract. This is the first study of Asian dust storm (ADS) particles collected in Beijing, China and Incheon, Korea during the same spring ADS event. Using a seven-stage May impactor and a quantitative electron probe X-ray microanalysis (ED-EPMA, also known as low-Z particle EPMA), we examined the composition and morphology of 4200 aerosol particles at stages 1–6 (with a size cut-off of 16, 8, 4, 2, 1, and 0.5 μm in equivalent aerodynamic diameter, respectively) collected during an ADS event on 28–29 April 2005. The results showed that there were large differences in the chemical compositions between particles in sample S1 collected in Beijing immediately after the peak time of the ADS and in samples S2 and S3, which were collected in Incheon approximately 5 h and 24 h later, respectively. In sample S1, mineral dust particles accounted for more than 88% in relative number abundance at stages 1–5, and organic carbon (OC) and reacted NaCl-containing particles accounted for 24% and 32%, respectively, at stage 6. On the other hand, in samples S2 and S3, in addition to approximately 60% mineral dust, many sea salt particles reacted with airborne SO2 and NOx, often mixed with mineral dust, were encountered at stages 1–5, and (C, N, O, S)-rich particles (likely a mixture of water-soluble organic carbon with (NH4)2SO4 and NH4NO3) and K-containing particles were abundantly observed at stage 6. This suggests that the secondary aerosols and the internal mixture of mineral dust with sea spray aerosol increased when the ADS particles passed over the Yellow Sea. In the reacted or aged mineral dust and sea salt particles, nitrate-containing and both nitrate- and sulfate-containing species vastly outnumbered the sulfate-containing species, implying that ambient nitrogen oxides had a greater influence on the atmospheric particles during the ADS episode than SO2. In addition to partially- or totally-reacted CaCO3, reacted or aged Mg-containing aluminosilicates (likely including amesite, allophite, vermiculite, illite, and montmorillonite) were observed frequently in samples S2 and S3; and furthermore, both the atomic concentration ratios of [Mg]/[Al] and [Mg]/[Si] were elevated compared to that in sample S1. This shows that a great evolution or aging process must have occurred on the mineral dust. This indicates that the number abundance, reactivity with gaseous pollutants, and ratios of [Mg]/[Al] and [Mg]/[Si] of Mg-containing aluminosilicates are promising indices of the aging process of ADS particles during long-range transport.

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

Atmospheric Chemistry and Physics ◽

10.5194/acp-21-18147-2021 ◽

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.

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Coastal and open ocean aerosol characteristics: investigating the representativeness of coastal aerosol sampling over the North-East Atlantic Ocean

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-8-19035-2008 ◽

2008 ◽

Vol 8 (6) ◽

pp. 19035-19062 ◽

Cited By ~ 1

Author(s):

M. Rinaldi ◽

M. C. Facchini ◽

S. Decesari ◽

C. Carbone ◽

E. Finessi ◽

...

Keyword(s):

Chemical Composition ◽

Atlantic Ocean ◽

Size Distribution ◽

Surf Zone ◽

Open Ocean ◽

Water Soluble ◽

Research Station ◽

Coastal Site ◽

Physical And Chemical ◽

Aerosol Properties

Abstract. In order to achieve a better understanding of the modifications of the physical and chemical properties of marine aerosol particles during transport from offshore to the coast, size distribution and chemical composition were measured concurrently in clean air masses over the open North Atlantic Ocean and at an Irish coastal site. Open ocean sampling was performed on board the oceanographic vessel Celtic Explorer sailing 100–300 km off the Irish west coast, while coastal measurements were performed at the Mace Head GAW station. The experiment took place between 11 June and 6 July 2006, during the period of phytoplankton bloom. The number size distribution and size-resolved chemical composition of coastal and open ocean samples were very similar, indicating homogeneous physical and chemical aerosol properties over a wide region in the marine boundary layer. The results also show that submicron chemical and physical aerosol properties measured at the coastal Mace Head Atmospheric Research Station were not unduly influenced by coastal artefacts and are thus representative of open water properties. Greater differences between the coastal site and the open ocean were observed for the aerosol supermicron sea spray components; this could be due to a variety of reasons, ranging from higher local wind speeds at the coastal site over the comparison period, to differences in sampling heights and increased local surf-zone production. Evidence of ageing processes was observed: at the costal site the ratio between non-sea-salt sulphate and methanesulphonic acid was higher, and the aerosol water soluble organic compounds were more oxidized than in the open ocean.

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A new method to quantify mineral dust and other aerosol species from aircraft platforms using single-particle mass spectrometry

Atmospheric Measurement Techniques ◽

10.5194/amt-12-6209-2019 ◽

2019 ◽

Vol 12 (11) ◽

pp. 6209-6239 ◽

Cited By ~ 5

Author(s):

Karl D. Froyd ◽

Daniel M. Murphy ◽

Charles A. Brock ◽

Pedro Campuzano-Jost ◽

Jack E. Dibb ◽

...

Keyword(s):

Mass Spectrometry ◽

Biomass Burning ◽

Single Particle ◽

Atmospheric Aerosol ◽

Mineral Dust ◽

Sea Salt ◽

Particle Mass ◽

Mode Analysis ◽

Single Particle Mass Spectrometry ◽

Mass Concentrations

Abstract. Single-particle mass spectrometry (SPMS) instruments characterize the composition of individual aerosol particles in real time. Their fundamental ability to differentiate the externally mixed particle types that constitute the atmospheric aerosol population enables a unique perspective into sources and transformation. However, quantitative measurements by SPMS systems are inherently problematic. We introduce a new technique that combines collocated measurements of aerosol composition by SPMS and size-resolved absolute particle concentrations on aircraft platforms. Quantitative number, surface area, volume, and mass concentrations are derived for climate-relevant particle types such as mineral dust, sea salt, and biomass burning smoke. Additionally, relative ion signals are calibrated to derive mass concentrations of internally mixed sulfate and organic material that are distributed across multiple particle types. The NOAA Particle Analysis by Laser Mass Spectrometry (PALMS) instrument measures size-resolved aerosol chemical composition from aircraft. We describe the identification and quantification of nine major atmospheric particle classes, including sulfate–organic–nitrate mixtures, biomass burning, elemental carbon, sea salt, mineral dust, meteoric material, alkali salts, heavy fuel oil combustion, and a remainder class. Classes can be sub-divided as necessary based on chemical heterogeneity, accumulated secondary material during aging, or other atmospheric processing. Concentrations are derived for sizes that encompass the accumulation and coarse size modes. A statistical error analysis indicates that particle class concentrations can be determined within a few minutes for abundances above ∼10 ng m−3. Rare particle types require longer sampling times. We explore the instrumentation requirements and the limitations of the method for airborne measurements. Reducing the size resolution of the particle data increases time resolution with only a modest increase in uncertainty. The principal limiting factor to fast time response concentration measurements is statistically relevant sampling across the size range of interest, in particular, sizes D < 0.2 µm for accumulation-mode studies and D > 2 µm for coarse-mode analysis. Performance is compared to other airborne and ground-based composition measurements, and examples of atmospheric mineral dust concentrations are given. The wealth of information afforded by composition-resolved size distributions for all major aerosol types represents a new and powerful tool to characterize atmospheric aerosol properties in a quantitative fashion.

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Characterization of the organic composition of aerosols from Rondônia, Brazil, during the LBA-SMOCC 2002 experiment and its representation through model compounds

Atmospheric Chemistry and Physics ◽

10.5194/acp-6-375-2006 ◽

2006 ◽

Vol 6 (2) ◽

pp. 375-402 ◽

Cited By ~ 214

Author(s):

S. Decesari ◽

S. Fuzzi ◽

M. C. Facchini ◽

M. Mircea ◽

L. Emblico ◽

...

Keyword(s):

Chemical Composition ◽

Biomass Burning ◽

Functional Group ◽

Group Analysis ◽

Water Soluble ◽

Total Carbon ◽

Individual Compound ◽

Model Compounds ◽

Functional Group Analysis

Abstract. The chemical composition of carbonaceous aerosols collected during the LBA-SMOCC field experiment, conducted in Rondônia, Brazil, in 2002 during the transition from the dry to the wet season, was investigated by a suite of state-of-the-art analytical techniques. The period of most intense biomass burning was characterized by high concentrations of submicron particles rich in carbonaceous material and water-soluble organic compounds (WSOC). At the onset of the rainy period, submicron total carbon (TC) concentrations decreased by about 20 times. In contrast, the concentration of supermicron TC was fairly constant throughout the experiment, pointing to a constant emission of coarse particles from the natural background. About 6–8% of TC (9–11% of WSOC) was speciated at the molecular level by GC-MS and liquid chromatography. Polyhydroxylated compounds, aliphatic and aromatic acids were the main classes of compounds accounted for by individual compound analysis. Functional group analysis by proton NMR and chromatographic separation on ion-exchange columns allowed characterization of ca. 50–90% of WSOC into broad chemical classes (neutral species/light acids/humic-like substances). In spite of the significant change in the chemical composition of tracer compounds from the dry to the wet period, the functional groups and the general chemical classes of WSOC changed only to a small extent. Model compounds representing size-resolved WSOC chemical composition for the different periods of the campaign are then proposed in this paper, based on the chemical characterization by both individual compound analysis and functional group analysis deployed during the LBA-SMOCC experiment. Model compounds reproduce quantitatively the average chemical structure of WSOC and can be used as best-guess surrogates in microphysical models involving organic aerosol particles over tropical areas affected by biomass burning.

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