Sea spray aerosol chemical composition: elemental and molecular mimics for laboratory studies of heterogeneous and multiphase reactions.

Science.gov (United States)

Bertram, Timothy H; Cochran, Richard E; Grassian, Vicki H; Stone, Elizabeth A

2018-04-03

Sea spray aerosol particles (SSA), formed through wave breaking at the ocean surface, contribute to natural aerosol particle concentrations in remote regions of Earth's atmosphere, and alter the direct and indirect effects of aerosol particles on Earth's radiation budget. In addition, sea spray aerosol serves as suspended surface area that can catalyze trace gas reactions. It has been shown repeatedly that sea spray aerosol is heavily enriched in organic material compared to the surface ocean. The selective enrichment of organic material complicates the selection of representative molecular mimics of SSA for laboratory or computational studies. In this review, we first provide a short introduction to SSA formation processes and discuss chemical transformations of SSA that occur in polluted coastal regions and remote pristine air. We then focus on existing literature of the chemical composition of nascent SSA generated in controlled laboratory experiments and field investigations. We combine the evidence on the chemical properties of nascent SSA with literature measurements of SSA water uptake to assess SSA molecular composition and liquid water content. Efforts to speciate SSA organic material into molecular classes and specific molecules have led to the identification of saccharides, alkanes, free fatty acids, anionic surfactants, dicarboxylic acids, amino acids, proteinaceous matter, and other large macromolecules. However to date, less than 25% of the organic mass of nascent SSA has been quantified at a molecular level. As discussed here, quantitative measurements of size resolved elemental ratios, combined with determinations of water uptake properties, provides unique insight on the concentration of ions within SSA as a function of particle size, pointing to a controlling role for relative humidity and the hygroscopicity of SSA organic material at small particle diameters.

Aerosol Chemical Mass Closure during the EUROTRAC-2 AEROSOL Intercomparison 2000

Czech Academy of Sciences Publication Activity Database

Maenhaut, W.; Schwarz, Jaroslav; Cafmeyer, J.; Chi, X.

2002-01-01

Roč. 186, - (2002), s. 233-237 ISSN 0168-583X Institutional research plan: CEZ:AV0Z4072921 Keywords : ion chromatography * chemical composition * atmospheric aerosols Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 1.158, year: 2002

Coastal Antarctic aerosol: the seasonal pattern of its chemical composition and radionuclide content

International Nuclear Information System (INIS)

Wagenbach, D.; Goerlach, U.; Moser, K.; Muennich, K.O.

1988-01-01

At the German Antarctic research station (70 degrees S, 8 degrees W), long-term observations of the chemical and radio-chemical composition of atmospheric particulate matter were started in spring 1983. Based on the analysis of high-volume aerosol filters sampled continuously for nearly 5 years, concentration records of the following aerosol components are presented here: (a) major ions (sea-salt, sulfate, nitrate); (b) cosmogenic 7 Be and terrigeneous 210 Pb; (c) trace elements (crustal Mn, heavy metal Pb). All species mentioned, with the exception of stable and radioactive Pb, show annual cycles. The maximum occurs in austral summer for 7 Be, sulfate, and crustal Mn. For sea-salt, however, the maximum is found in local autumn, and for nitrate in local spring. In local summer, the enhanced 7 Be to 210 Pb ratio is attributed to intenser large scale vertical mixing. The pattern of total sulfate seems to be controlled by the nss-sulfate production from marine organo-sulfur species during local summer, whereas in polar night, nss-sulfate shows very low or even negative concentration. Crustal aerosol (indicated by Mn) shows a mean summer contribution of 16 ng/SCM which exceeds the mean winter level by more than a factor of two. Based on a mean wash-out ratio of 0.27x10 6 observed for 210 Pb bearing aerosol particles, a Pb snow concentration of 3.0 pg/g is deduced from the mean air concentration of 11 pg/SCM. (authors)

Evolution of biomass burning aerosol over the Amazon: airborne measurements of aerosol chemical composition, microphysical properties, mixing state and optical properties during SAMBBA

Science.gov (United States)

Morgan, W.; Allan, J. D.; Flynn, M.; Darbyshire, E.; Hodgson, A.; Liu, D.; O'Shea, S.; Bauguitte, S.; Szpek, K.; Johnson, B.; Haywood, J.; Longo, K.; Artaxo, P.; Coe, H.

2013-12-01

Biomass burning represents one of the largest sources of particulate matter to the atmosphere, resulting in a significant perturbation to the Earth's radiative balance coupled with serious impacts on public health. On regional scales, the impacts are substantial, particularly in areas such as the Amazon Basin where large, intense and frequent burning occurs on an annual basis for several months. Absorption by atmospheric aerosols is underestimated by models over South America, which points to significant uncertainties relating to Black Carbon (BC) aerosol properties. Initial results from the South American Biomass Burning Analysis (SAMBBA) field experiment, which took place during September and October 2012 over Brazil on-board the UK Facility for Airborne Atmospheric Measurement (FAAM) BAe-146 research aircraft, are presented here. Aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) and a DMT Single Particle Soot Photometer (SP2). The physical, chemical and optical properties of the aerosols across the region will be characterized in order to establish the impact of biomass burning on regional air quality, weather and climate. The aircraft sampled a range of conditions including sampling of pristine Rainforest, fresh biomass burning plumes, regional haze and elevated biomass burning layers within the free troposphere. The aircraft sampled biomass burning aerosol across the southern Amazon in the states of Rondonia and Mato Grosso, as well as in a Cerrado (Savannah-like) region in Tocantins state. This presented a range of fire conditions, in terms of their number, intensity, vegetation-type and their combustion efficiencies. Near-source sampling of fires in Rainforest environments suggested that smouldering combustion dominated, while flaming combustion dominated in the Cerrado. This led to significant differences in aerosol chemical composition, particularly in terms of the BC content, with BC being enhanced in the Cerrado

Aerosol size and chemical composition measurements at the Polar Environment Atmospheric Research Lab (PEARL) in Eureka, Nunavut

Science.gov (United States)

Hayes, P. L.; Tremblay, S.; Chang, R. Y. W.; Leaitch, R.; Kolonjari, F.; O'Neill, N. T.; Chaubey, J. P.; AboEl Fetouh, Y.; Fogal, P.; Drummond, J. R.

2016-12-01

This study presents observations of aerosol chemical composition and particle number size distribution at the Polar Environment Atmospheric Research Laboratory (PEARL) in the Canadian High Arctic (80N, 86W). The current aerosol measurement program at PEARL has been ongoing for more than a year providing long-term observations of Arctic aerosol size distributions for both coarse and fine modes. Particle nucleation events were frequently observed during the summers of 2015 and 2016. The size distribution data are also compared against similar measurements taken at the Alert Global Atmospheric Watch Observatory (82N, 62W) for July and August 2015. The nucleation events are correlated at the two sites, despite a distance of approximately 500 km, suggesting regional conditions favorable for particle nucleation and growth during this period. Size resolved chemical composition measurements were also carried out using an aerosol mass spectrometer. The smallest measured particles between 40 and 60 nm are almost entirely organic aerosol (OA) indicating that the condensation of organic vapors is responsible for particle growth events and possibly particle nucleation. This conclusion is further supported by the relatively high oxygen content of the OA, which is consistent with secondary formation of OA via atmospheric oxidation.Lastly, surface measurements of the aerosol scattering coefficient are compared against the coefficient values calculated using Mie theory and the measured aerosol size distribution. Both the actual and the calculated scattering coefficients are then compared to sun photometer measurements to understand the relationship between surface and columnar aerosol optical properties. The measurements at PEARL provide a unique combination of surface and columnar data sets on aerosols in the High Arctic, a region where such measurements are scarce despite the important impact of aerosols on Arctic climate.PEARL research is supported by the Natural Sciences and

Aerosol sources and their contribution to the chemical composition of aerosols in the Eastern Mediterranean Sea during summertime

Directory of Open Access Journals (Sweden)

J. Sciare

2003-01-01

Full Text Available A detailed study on the temporal variability of compounds important in controlling aerosol chemical composition was performed during a one-month experiment conducted during summer 2000 at a background site on Crete, in the Eastern Mediterranean Sea. Contribution of different aerosol sources in the Eastern Mediterranean Basin could be investigated at this location since the site is influenced by a wide range of air masses originating mainly in Europe and Africa. Chemical apportionment was performed for various air mass origins and showed a strong impact of anthropogenic emissions in the Turkey and Central Europe sectors, with black carbon (BC and non-sea-salt sulfate (nss-SO4 concentrations higher than observed in the Eastern and Western Europe sectors. High levels of non-sea-salt calcium (nss-Ca were associated with air masses from Africa but also from Central Turkey. Evidence was found that BC calculation based on light absorbance during dust events was biased. This quality-controlled high temporal resolution dataset allowed to investigate in detail the source-receptor relationships responsible for the levels of BC, nss-SO4 and sulfur dioxide (SO2, observed in Crete. Among the results obtained from this model, the major contribution of Turkey and Central Europe was confirmed in terms of anthropogenic emissions. Comparisons with remote optical properties obtained from Satellite observations (SEAWIFS north of Crete indicates that our ground based aerosol characterization was suitable for describing aerosol properties in the atmospheric column for most of the time during the campaign.

Influence of trace aromatics on the chemical growth mechanisms of Titan aerosol analogues

Science.gov (United States)

Gautier, Thomas; Sebree, Joshua A.; Li, Xiang; Pinnick, Veronica T.; Grubisic, Andrej; Loeffler, Mark J.; Getty, Stephanie A.; Trainer, Melissa G.; Brinckerhoff, William B.

2017-06-01

The chemical structure and formation pathways of Titan aerosols remain largely unknown. In this work, we studied the effect of trace aromatics on the chemical composition and formation pathways of laboratory analogues of Titan's organic aerosols. The aerosol analogues were produced using four different trace aromatic molecules, comprised of one or two aromatic rings, each with or without a nitrogen heteroatom. Samples were then analyzed by laser desorption/ionization Mass Spectrometry (LDMS), revealing a high variability in the sample composition depending on the trace aromatic used. Our work reveals that the final chemical structure of the aerosols depends strongly on the number of aromatic rings in the trace molecule, leading either to a polymeric or to a random co-polymeric growth of the sample. These different chemical structures can affect the physical properties of the aerosol. Future analysis of Titan's aerosols using better resolution could potentially determine whether either of the growth hypotheses are preferred.

Biomass burning aerosol over the Amazon during SAMBBA: impact of chemical composition on radiative properties

Science.gov (United States)

Morgan, William; Allan, James; Flynn, Michael; Darbyshire, Eoghan; Hodgson, Amy; Liu, Dantong; O'shea, Sebastian; Bauguitte, Stephane; Szpek, Kate; Langridge, Justin; Johnson, Ben; Haywood, Jim; Longo, Karla; Artaxo, Paulo; Coe, Hugh

2014-05-01

Biomass burning represents one of the largest sources of particulate matter to the atmosphere, resulting in a significant perturbation to the Earth's radiative balance coupled with serious impacts on public health. Globally, biomass burning aerosols are thought to exert a small warming effect but with the uncertainty being 4 times greater than the central estimate. On regional scales, the impact is substantially greater, particularly in areas such as the Amazon Basin where large, intense and frequent burning occurs on an annual basis for several months. Absorption by atmospheric aerosols is underestimated by models over South America, which points to significant uncertainties relating to Black Carbon (BC) aerosol properties. Initial results from the South American Biomass Burning Analysis (SAMBBA) field experiment, which took place during September and October 2012 over Brazil on-board the UK Facility for Airborne Atmospheric Measurement (FAAM) BAe-146 research aircraft, are presented here. Aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) and a DMT Single Particle Soot Photometer (SP2). The physical, chemical and optical properties of the aerosols across the region will be characterized in order to establish the impact of biomass burning on regional air quality, weather and climate. The aircraft sampled a range of conditions including sampling of pristine Rainforest, fresh biomass burning plumes, regional haze and elevated biomass burning layers within the free troposphere. The aircraft sampled biomass burning aerosol across the southern Amazon in the states of Rondonia and Mato Grosso, as well as in a Cerrado (Savannah-like) region in Tocantins state. This presented a range of fire conditions, both in terms of their number, intensity, vegetation-type and their combustion efficiencies. Near-source sampling of fires in Rainforest environments suggested that smouldering combustion dominated, while flaming combustion dominated

Chemically aged and mixed aerosols over the Central Atlantic Ocean - Potential impacts

NARCIS (Netherlands)

Astitha, M.; Kallos, G.; Spyrou, C.; O'Hirok, W.; Lelieveld, J.; Denier Gon, H.A.C. van der

2010-01-01

Detailed information on the chemical and physical properties of aerosols is important for assessing their role in air quality and climate. This work explores the origin and fate of continental aerosols transported over the Central Atlantic Ocean, in terms of chemical composition, number and size

Variability of Aerosols and Chemical Composition of PM10, PM2.5 and PM1 on a Platform of the Prague Underground Metro

Czech Academy of Sciences Publication Activity Database

Cusack, Michael; Talbot, Nicholas; Ondráček, Jakub; Minguillón, M.C.; Martins, V.; Klouda, K.; Schwarz, Jaroslav; Ždímal, Vladimír

2015-01-01

Roč. 118, OCT 2015 (2015), s. 176-183 ISSN 1352-2310 EU Projects: European Commission(XE) 315760 Institutional support: RVO:67985858 Keywords : subway aerosol * chemical composition * aerosol dynamics Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 3.459, year: 2015

Chemical composition and source apportionment of aerosol over the Klang valley

International Nuclear Information System (INIS)

Shamsiah Abdul Rahman; Mohd Suhaimi Hamzah; Abdul Khalik Wood; Nazaratul Ashifa Abdullah Salim; Mohd Suhaimi Elias; Eswiza Sanuri

2009-01-01

This paper reports the study of aerosol chemical composition of fine particles (PM 2.5) and possible sources of air pollution over the Klang Valley, Kuala Lumpur, based on the samples collected for a period of 6 years from July 2000 to Jun 2006. Samples collected were measured for mass, black carbon and elemental content of Na, Mg, Al, Si, P, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, As, Br and Pb. The fine aerosol mass concentration ranged from 11 - 110 ?g/m3. Black carbon is the major component of the fine aerosol with the weight fraction of 20%, whilst S is the major elemental content with the weight fraction about 5% as relative to the fine particle mass. The factor analysis method, positive matrix factorization (PMF) was then used to confirm the possible sources. The result of PMF analysis produced five-factor sources that contribute to the fine particles in the Klang Valley area. The five factors represent sea spray, industry, motor vehicles, smoke and soil. Motor vehicle is the main source of particulates in the area, with an average contribution of 51% of the fine mass concentration, followed by industry, smoke, sea spray and soil, with average contribution of 28%, 14%, 3.6% and 2.1%, respectively. (Author)

Elucidating determinants of aerosol composition through particle-type-based receptor modeling

Science.gov (United States)

McGuire, M. L.; Jeong, C.-H.; Slowik, J. G.; Chang, R. Y.-W.; Corbin, J. C.; Lu, G.; Mihele, C.; Rehbein, P. J. G.; Sills, D. M. L.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

2011-08-01

An aerosol time-of-flight mass spectrometer (ATOFMS) was deployed at a semi-rural site in southern Ontario to characterize the size and chemical composition of individual particles. Particle-type-based receptor modelling of these data was used to investigate the determinants of aerosol chemical composition in this region. Individual particles were classified into particle-types and positive matrix factorization (PMF) was applied to their temporal trends to separate and cross-apportion particle-types to factors. The extent of chemical processing for each factor was assessed by evaluating the internal and external mixing state of the characteristic particle-types. The nine factors identified helped to elucidate the coupled interactions of these determinants. Nitrate-laden dust was found to be the dominant type of locally emitted particles measured by ATOFMS. Several factors associated with aerosol transported to the site from intermediate local-to-regional distances were identified: the Organic factor was associated with a combustion source to the north-west; the ECOC Day factor was characterized by nearby local-to-regional carbonaceous emissions transported from the south-west during the daytime; and the Fireworks factor consisted of pyrotechnic particles from the Detroit region following holiday fireworks displays. Regional aerosol from farther emissions sources was reflected through three factors: two Biomass Burning factors and a highly chemically processed Long Range Transport factor. The Biomass Burning factors were separated by PMF due to differences in chemical processing which were in part elucidated by the passage of two thunderstorm gust fronts with different air mass histories. The remaining two factors, ECOC Night and Nitrate Background, represented the night-time partitioning of nitrate to pre-existing particles of different origins. The distinct meteorological conditions observed during this month-long study in the summer of 2007 provided a unique

Measurements of the aerosol chemical composition and mixing state in the Po Valley using multiple spectroscopic techniques

Science.gov (United States)

Decesari, S.; Allan, J.; Plass-Duelmer, C.; Williams, B. J.; Paglione, M.; Facchini, M. C.; O'Dowd, C.; Harrison, R. M.; Gietl, J. K.; Coe, H.; Giulianelli, L.; Gobbi, G. P.; Lanconelli, C.; Carbone, C.; Worsnop, D.; Lambe, A. T.; Ahern, A. T.; Moretti, F.; Tagliavini, E.; Elste, T.; Gilge, S.; Zhang, Y.; Dall'Osto, M.

2014-11-01

The use of co-located multiple spectroscopic techniques can provide detailed information on the atmospheric processes regulating aerosol chemical composition and mixing state. So far, field campaigns heavily equipped with aerosol mass spectrometers have been carried out mainly in large conurbations and in areas directly affected by their outflow, whereas lesser efforts have been dedicated to continental areas characterised by a less dense urbanisation. We present here the results obtained at a background site in the Po Valley, Italy, in summer 2009. For the first time in Europe, six state-of-the-art spectrometric techniques were used in parallel: aerosol time-of-flight mass spectrometer (ATOFMS), two aerosol mass spectrometers (high-resolution time-of-flight aerosol mass spectrometer - HR-ToF-AMS and soot particle aerosol mass spectrometer - SP-AMS), thermal desorption aerosol gas chromatography (TAG), chemical ionisation mass spectrometry (CIMS) and (offline) proton nuclear magnetic resonance (1H-NMR) spectroscopy. The results indicate that, under high-pressure conditions, atmospheric stratification at night and early morning hours led to the accumulation of aerosols produced by anthropogenic sources distributed over the Po Valley plain. Such aerosols include primary components such as black carbon (BC), secondary semivolatile compounds such as ammonium nitrate and amines and a class of monocarboxylic acids which correspond to the AMS cooking organic aerosol (COA) already identified in urban areas. In daytime, the entrainment of aged air masses in the mixing layer is responsible for the accumulation of low-volatility oxygenated organic aerosol (LV-OOA) and also for the recycling of non-volatile primary species such as black carbon. According to organic aerosol source apportionment, anthropogenic aerosols accumulating in the lower layers overnight accounted for 38% of organic aerosol mass on average, another 21% was accounted for by aerosols recirculated in

Atmo-metabolomics: a new measurement approach for investigating aerosol composition and ecosystem functioning.

Science.gov (United States)

Rivas-Ubach, A.; Liu, Y.; Sardans, J.; Tfaily, M. M.; Kim, Y. M.; Bourrianne, E.; Paša-Tolić, L.; Penuelas, J.; Guenther, A. B.

2016-12-01

Aerosols play crucial roles in the processes controlling the composition of the atmosphere and the functioning of ecosystems. Gaining a deeper understanding of the chemical composition of aerosols is one of the major challenges for atmospheric and climate scientists and is beginning to be recognized as important for ecological research. Better comprehension of aerosol chemistry can potentially provide valuable information on atmospheric processes such as oxidation of organics and the production of cloud condensation nuclei as well as provide an approximation of the general status of an ecosystem through the measurement of certain stress biomarkers. In this study, we describe an efficient aerosol sampling method, the metabolite extraction and the analytical procedures for the chemical characterization of aerosols, namely, the atmo-metabolome. We used mass spectrometry (MS) coupled to liquid chromatography (LC-MS), gas chromatography (GC-MS) and Fourier transform ion cyclotron resonance (FT-ICR-MS) to characterize the atmo-metabolome of two marked seasons; spring and summer. Our sampling and extraction methods demonstrated to be suitable for aerosol chemical characterization with any of the analytical platforms used in this study. The atmo-metabolome between spring and summer showed overall statistically differences. We identified several metabolites that can be attributed to pollen and other plant-related aerosols. Spring aerosols exhibit higher concentrations of metabolites linked to higher plant activity while summer samples had higher concentrations of metabolites that may reflect certain oxidative stresses in primary producers. Moreover, the elemental composition of aerosols showed clear different between seasons. Summer aerosols were generally higher in molecular weight and with higher O/C ratios, indicating higher oxidation levels and condensation of compounds relative to spring. Our method represents an advanced approach for characterizing the composition of

Complex chemical composition of colored surface films formed from reactions of propanal in sulfuric acid at upper troposphere/lower stratosphere aerosol acidities.

Science.gov (United States)

Van Wyngarden, A L; Pérez-Montaño, S; Bui, J V H; Li, E S W; Nelson, T E; Ha, K T; Leong, L; Iraci, L T

Particles in the upper troposphere and lower stratosphere (UT/LS) consist mostly of concentrated sulfuric acid (40-80 wt %) in water. However, airborne measurements have shown that these particles also contain a significant fraction of organic compounds of unknown chemical composition. Acid-catalyzed reactions of carbonyl species are believed to be responsible for significant transfer of gas phase organic species into tropospheric aerosols and are potentially more important at the high acidities characteristic of UT/LS particles. In this study, experiments combining sulfuric acid (H 2 SO 4 ) with propanal and with mixtures of propanal with glyoxal and/or methylglyoxal at acidities typical of UT/LS aerosols produced highly colored surface films (and solutions) that may have implications for aerosol properties. In order to identify the chemical processes responsible for the formation of the surface films, attenuated total reflectance-Fourier transform infrared (ATR-FTIR) and 1 H nuclear magnetic resonance (NMR) spectroscopies were used to analyze the chemical composition of the films. Films formed from propanal were a complex mixture of aldol condensation products, acetals and propanal itself. The major aldol condensation products were the dimer (2-methyl-2-pentenal) and 1,3,5-trimethylbenzene that was formed by cyclization of the linear aldol condensation trimer. Additionally, the strong visible absorption of the films indicates that higher-order aldol condensation products must also be present as minor species. The major acetal species were 2,4,6-triethyl-1,3,5-trioxane and longer-chain linear polyacetals which are likely to separate from the aqueous phase. Films formed on mixtures of propanal with glyoxal and/or methylglyoxal also showed evidence of products of cross-reactions. Since cross-reactions would be more likely than self-reactions under atmospheric conditions, similar reactions of aldehydes like propanal with common aerosol organic species like glyoxal

Size-segregated aerosol in a hot-spot pollution urban area: Chemical composition and three-way source apportionment.

Science.gov (United States)

Bernardoni, V; Elser, M; Valli, G; Valentini, S; Bigi, A; Fermo, P; Piazzalunga, A; Vecchi, R

2017-12-01

In this work, a comprehensive characterisation and source apportionment of size-segregated aerosol collected using a multistage cascade impactor was performed. The samples were collected during wintertime in Milan (Italy), which is located in the Po Valley, one of the main pollution hot-spot areas in Europe. For every sampling, size-segregated mass concentration, elemental and ionic composition, and levoglucosan concentration were determined. Size-segregated data were inverted using the program MICRON to identify and quantify modal contributions of all the measured components. The detailed chemical characterisation allowed the application of a three-way (3-D) receptor model (implemented using Multilinear Engine) for size-segregated source apportionment and chemical profiles identification. It is noteworthy that - as far as we know - this is the first time that three-way source apportionment is attempted using data of aerosol collected by traditional cascade impactors. Seven factors were identified: wood burning, industry, resuspended dust, regional aerosol, construction works, traffic 1, and traffic 2. Further insights into size-segregated factor profiles suggested that the traffic 1 factor can be associated to diesel vehicles and traffic 2 to gasoline vehicles. The regional aerosol factor resulted to be the main contributor (nearly 50%) to the droplet mode (accumulation sub-mode with modal diameter in the range 0.5-1 μm), whereas the overall contribution from the two factors related to traffic was the most important one in the other size modes (34-41%). The results showed that applying a 3-D receptor model to size-segregated samples allows identifying factors of local and regional origin while receptor modelling on integrated PM fractions usually singles out factors characterised by primary (e.g. industry, traffic, soil dust) and secondary (e.g. ammonium sulphate and nitrate) origin. Furthermore, the results suggested that the information on size

Aerosols in Northern Morocco: Input pathways and their chemical fingerprint

Science.gov (United States)

Benchrif, A.; Guinot, B.; Bounakhla, M.; Cachier, H.; Damnati, B.; Baghdad, B.

2018-02-01

The Mediterranean basin is one of the most sensitive regions in the world regarding climate change and air quality. Deserts and marine aerosols combine with combustion aerosols from maritime traffic, large urban centers, and at a larger scale from populated industrialized regions in Europe. From Tetouan city located in the North of Morocco, we attempted to better figure out the main aerosol transport pathways and their respective aerosol load and chemical profile by examining air mass back trajectory patterns and aerosol chemical compositions from May 2011 to April 2012. The back trajectory analysis throughout the sampling period led to four clusters, for which meteorological conditions and aerosol chemical characteristics have been investigated. The most frequent cluster (CL3: 39%) corresponds to polluted air masses coming from the Mediterranean Basin, characterized by urban and marine vessels emissions out of Spain and of Northern Africa. Two other polluted clusters were characterized. One is of local origin (CL1: 22%), with a marked contribution from urban aerosols (Rabat, Casablanca) and from biomass burning aerosols. The second (CL2: 32%) defines air masses from the near Atlantic Ocean, affected by pollutants emitted from the Iberian coast. A fourth cluster (CL4: 7%) is characterized by rather clean, fast and rainy oceanic air masses, influenced during their last 24 h before reaching Tetouan by similar sources with those affecting CL2, but to a lesser extent. The chemical data show that carbonaceous species are found in the fine aerosols fraction and are generally from local primary sources (low OC/EC) rather than long-range transported. In addition to fresh traffic and maritime vessel aerosols, our results suggest the contribution of local biomass burning.

Modelling the chemically aged and mixed aerosols over the eastern central Atlantic Ocean-potential impacts

NARCIS (Netherlands)

Astitha, M.; Kallos, G.; Spyrou, C.; O'Hirok, W.; Lelieveld, J.; Denier Gon, H.A.C. van der

2010-01-01

Detailed information on the chemical and physical properties of aerosols is important for assessing their role in air quality and climate. This work explores the origin and fate of continental aerosols transported over the Central Atlantic Ocean, in terms of chemical composition, number and size

Long-term measurement of aerosol chemical composition in Athens, Greece.

Science.gov (United States)

Paraskevopoulou, Despina; Liakakou, Eleni; Theodosi, Christina; Gerasopoulos, Evangelos; Mihalopoulos, Nikolaos

2014-05-01

The collection of our samples was conducted for a period of five years (2008 - 2013) in Athens, Greece. The site is situated at the premises of the National Observatory of Athens on Penteli Hill, northeast Athens suburbs, and is considered an urban background station. The aim of our study was a first long-term estimation of the chemical mass closure of aerosol. For the purposes of the study, we applied three filter samplers during the sampling period: two Partisol FRM Model 2000 air samplers (one of them collecting PM10 and the other PM2.5 fractions of aerosol) and one Dichotomous Partisol auto-sampler (with PM2.5 and PM2.5-10 inlet). Aerosols were collected on Whatman QM-A quartz fiber filters and the mass of the collected samples was estimated by weighing the pre-combusted filters before and after sampling, under controlled conditions, using a microbalance. All quartz filters were analysed for organic (OC) and elemental carbon (EC) by a thermal - optical transmission technique. The concentration of water soluble organic carbon (WSOC) was defined for each filter using a total organic carbon analyzer, while the content in main water soluble ions (Cl-, Br-, NO-3, SO4-2, PO4-3, C2O4-2, NH4+, K+, Na+, Mg+2, Ca+2) was determined by ion chromatography. Additionally the filters were analyzed for trace metals by inductively coupled plasma optical emission spectrometry (ICP-OES). Aerosol chemical mass closure calculations were conducted for the PM2.5 fraction. The area of Athens is characterized by aged aerosol that can originate from the marine boundary layer, the European mainland and occasionally from North African desert areas. The contribution of dust and particulate organic matter on PM levels was estimated taking into consideration the location of the sampling site, while identification and evaluation of sources was performed. Additionally, non-sea salt concentrations of the main ions were estimated to complete the chemical closure in the extended area. According to

Wintertime aerosol chemical composition and source apportionment of the organic fraction across Ireland

Science.gov (United States)

Ovadnevaite, J.; Lin, C.; Ceburnis, D.; Huang, R. J. J.; O'Dowd, C. D. D.

2017-12-01

A national wide characterization of PM1 was studied for the first time using a high-time resolution Aerosol Chemical Speciation Monitor (ACSM) and Aethalometer in Ireland during the heating season. Dublin, the capital of Ireland, is the most polluted area with an average PM1 of 7.6 μg/m3, with frequent occurrence of peak concentration over 200 μg/m3 primarily due to solid fuels burning, while Mace Head, in the west coast, is least polluted with an average PM1 of 0.8 μg/m3 due to the distance from the emission sources. The organic aerosol is the most dominant species across Ireland, contributing 65%, 58%, 32%, 33% to total PM1 mass in Dublin, Birr, Carnsore Point, and Mace Head, respectively. Birr, a small town in the midland of Ireland, has comparable PM1 levels (4.8 μg/m3) and similar chemical compositions with that in Dublin. Carnsore Point, on the southeast coast, has similar composition with that at Mace Head, but nearly 3 times the levels of PM1 mass due to its relative closeness to other European countries. Positive matrix factorization (PMF) with the multi-linear engine (ME-2) was performed on the organic matrix to quantify the contribution of factor candidates. Peat burning was found to be the dominant factor across Ireland, contributing more than 40% of the total organic mass in Dublin and Birr while OOA is dominant at rural Carnsore Point and Mace Head. Possible geographic origins of PM1 species and organic factors using polar plots were explored. The findings of solid fuels burning (primarily peat burning) driving the pollution episodes suggest an elimination or controlled emission of solid fuels burning would reduce PM1 by at least 50%.

Sources of atmospheric aerosol from long-term measurements (5 years) of chemical composition in Athens, Greece.

Science.gov (United States)

Paraskevopoulou, D; Liakakou, E; Gerasopoulos, E; Mihalopoulos, N

2015-09-15

To identify the sources of aerosols in Greater Athens Area (GAA), a total of 1510 daily samples of fine (PM 2.5) and coarse (PM 10-2,5) aerosols were collected at a suburban site (Penteli), during a five year period (May 2008-April 2013) corresponding to the period before and during the financial crisis. In addition, aerosol sampling was also conducted in parallel at an urban site (Thissio), during specific, short-term campaigns during all seasons. In all these samples mass and chemical composition measurements were performed, the latest only at the fine fraction. Particulate organic matter (POM) and ionic masses (IM) are the main contributors of aerosol mass, equally contributing by accounting for about 24% of the fine aerosol mass. In the IM, nss-SO4(-2) is the prevailing specie followed by NO3(-) and NH4(+) and shows a decreasing trend during the 2008-2013 period similar to that observed for PM masses. The contribution of water in fine aerosol is equally significant (21 ± 2%), while during dust transport, the contribution of dust increases from 7 ± 2% to 31 ± 9%. Source apportionment (PCA and PMF) and mass closure exercises identified the presence of six sources of fine aerosols: secondary photochemistry, primary combustion, soil, biomass burning, sea salt and traffic. Finally, from winter 2012 to winter 2013 the contribution of POM to the urban aerosol mass is increased by almost 30%, reflecting the impact of wood combustion (dominant fuel for domestic heating) to air quality in Athens, which massively started in winter 2013. Copyright © 2015 Elsevier B.V. All rights reserved.

Relationship between chemical composition and oxidative potential of secondary organic aerosol from polycyclic aromatic hydrocarbons

Science.gov (United States)

Wang, Shunyao; Ye, Jianhuai; Soong, Ronald; Wu, Bing; Yu, Legeng; Simpson, André J.; Chan, Arthur W. H.

2018-03-01

Owing to the complex nature and dynamic behaviors of secondary organic aerosol (SOA), its ability to cause oxidative stress (known as oxidative potential, or OP) and adverse health outcomes remains poorly understood. In this work, we probed the linkages between the chemical composition of SOA and its OP, and investigated impacts from various SOA evolution pathways, including atmospheric oligomerization, heterogeneous oxidation, and mixing with metal. SOA formed from photooxidation of the two most common polycyclic aromatic hydrocarbons (naphthalene and phenanthrene) were studied as model systems. OP was evaluated using the dithiothreitol (DTT) assay. The oligomer-rich fraction separated by liquid chromatography dominates DTT activity in both SOA systems (52 ± 10 % for naphthalene SOA (NSOA), and 56 ± 5 % for phenanthrene SOA (PSOA)). Heterogeneous ozonolysis of NSOA was found to enhance its OP, which is consistent with the trend observed in selected individual oxidation products. DTT activities from redox-active organic compounds and metals were found to be not additive. When mixing with highly redox-active metal (Cu), OP of the mixture decreased significantly for 1,2-naphthoquinone (42 ± 7 %), 2,3-dihydroxynaphthalene (35 ± 1 %), NSOA (50 ± 6 %), and PSOA (43 ± 4 %). Evidence from proton nuclear magnetic resonance (1H NMR) spectroscopy illustrates that such OP reduction upon mixing can be ascribed to metal-organic binding interactions. Our results highlight the role of aerosol chemical composition under atmospheric aging processes in determining the OP of SOA, which is needed for more accurate and explicit prediction of the toxicological impacts from particulate matter.

Optical properties of the urban aerosol and their relation to chemical composition

International Nuclear Information System (INIS)

Leaderer, B.P.; Stolwijk, J.A.J.

1980-01-01

Light extinction and resulting visibility degradation in an unsaturated precipitation-free atmosphere are determined by light absorption and scattering and are caused by a complex mix of natural components and anthropogenic pollutants. The paper reviews correlation studies relating light scattering and light extinction (visibility) to concentrations of sulfate mass, nitrate mass, the remainder of the mass, and in some cases organic aerosol mass, while accounting for variations in relative humidity. It is found that sulfate aerosol mass is the dominant chemical aerosol species affecting light scattering and extinction. The dominant effect of sulfate mass on light scattering and extinction, even when sulfates account for a relatively small fraction of the total mass, results from the fact that sulfates are secondary aerosols and are mostly found in the 0.1-1.0 micron size range

Chemical composition, sources and evolution processes of aerosol at an urban site in Yangtze River Delta, China during wintertime

Science.gov (United States)

Zhang, Yunjiang; Tang, Lili; Yu, Hongxia; Wang, Zhuang; Sun, Yele; Qin, Wei; Chen, Wentai; Chen, Changhong; Ding, Aijun; Wu, Jing; Ge, Shun; Chen, Cheng; Zhou, Hong-cang

2015-12-01

To investigate the composition, sources and evolution processes of submicron aerosol during wintertime, a field experiment was conducted during December 1-31, 2013 in urban Nanjing, a megacity in Yangtze River Delta of China. Non-refractory submicron aerosol (NR-PM1) species were measured with an Aerodyne Aerosol Chemical Speciation Monitor. NR-PM1 is dominated by secondary inorganic aerosol (55%) and organic aerosol (OA, 42%) during haze periods. Six OA components were identified by positive matrix factorization of the OA mass spectra. The hydrocarbon-like OA and cooking-related OA represent the local traffic and cooking sources, respectively. A highly oxidized factor related to biomass burning OA accounted for 15% of the total OA mass during haze periods. Three types of oxygenated OA (OOA), i.e., a less-oxidized OOA (LO-OOA), a more-oxidized OOA (MO-OOA), and a low-volatility OOA (LV-OOA), were identified. LO-OOA is likely associated with fresh urban secondary OA. MO-OOA likely represents photochemical products showing a similar diurnal cycle to nitrate with a pronounced noon peak. LV-OOA appears to be a more oxidized factor with a pronounced noon peak. The OA composition is dominated by secondary species, especially during haze events. LO-OOA, MO-OOA and LV-OOA on average account for 11%, (18%), 24% (21%) and 23% (18%) of the total OA mass for the haze (clean) periods respectively. Analysis of meteorological influence suggested that regional transport from the northern and southeastern areas of the city is responsible for large secondary and low-volatility aerosol formation.

Two years of near real-time chemical composition of submicron aerosols in the region of Paris using an Aerosol Chemical Speciation Monitor (ACSM) and a multi-wavelength Aethalometer

Science.gov (United States)

Petit, J.-E.; Favez, O.; Sciare, J.; Crenn, V.; Sarda-Estève, R.; Bonnaire, N.; Močnik, G.; Dupont, J.-C.; Haeffelin, M.; Leoz-Garziandia, E.

2015-03-01

parameters controlling their temporal variations (sources, meteorological parameters). Finally, a careful investigation of all the major pollution episodes observed over the region of Paris between 2011 and 2013 was performed and classified in terms of chemical composition and the BC-to-sulfate ratio used here as a proxy of the local/regional/advected contribution of PM. In conclusion, these first 2-year quality-controlled measurements of ACSM clearly demonstrate their great potential to monitor on a long-term basis aerosol sources and their geographical origin and provide strategic information in near real time during pollution episodes. They also support the capacity of the ACSM to be proposed as a robust and credible alternative to filter-based sampling techniques for long-term monitoring strategies.

Chemical Properties of Brown Carbon Aerosol Generated at the Missoula Fire Sciences Laboratory

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Washenfelder, R. A.; Womack, C.; Franchin, A.; Middlebrook, A. M.; Wagner, N.; Manfred, K.

2017-12-01

Aerosol scattering and absorption are still among the largest uncertainties in quantifying radiative forcing. Biomass burning is a major source of light-absorbing carbonaceous aerosol in the United States. These aerosol are generally classified into two categories: black carbon (graphitic-like aerosol that absorbs broadly across the ultraviolet and visible spectral regions) and brown carbon (organic aerosol that absorbs strongly in the ultraviolet and near-visible spectral regions). The composition, volatility, and chemical aging of brown carbon are poorly known, but are important to understanding its radiative effects. We deployed three novel instruments to the Missoula Fire Sciences Laboratory in 2016 to measure brown carbon absorption: a photoacoustic spectrometer, broadband cavity enhanced spectrometer, and particle-into-liquid sampler coupled to a liquid waveguide capillary cell. The instruments sampled from a shared inlet with well-characterized dilution and thermal denuding. We sampled smoke from 32 controlled burns of fuels relevant to western U.S. wildfires. We use these measurements to determine the volatility of water-soluble brown carbon, and compare this to the volatility of water-soluble organic aerosol and total organic aerosol. We further examine the wavelength-dependence of the water-soluble brown carbon absorption as a function of denuder temperature. Together this gives new information about the solubility, volatility, and chemical composition of brown carbon.

Chemical composition and characteristics of ambient aerosols and rainwater residues during Indian summer monsoon: Insight from aerosol mass spectrometry

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Chakraborty, Abhishek; Gupta, Tarun; Tripathi, Sachchida N.

2016-07-01

Real time composition of non-refractory submicron aerosol (NR-PM1) is measured via Aerosol mass spectrometer (AMS) for the first time during Indian summer monsoon at Kanpur, a polluted urban location located at the heart of Indo Gangetic Plain (IGP). Submicron aerosols are found to be dominated by organics followed by nitrate. Source apportionment of organic aerosols (OA) via positive matrix factorization (PMF) revealed several types of secondary/oxidized and primary organic aerosols. On average, OA are completely dominated by oxidized OA with a very little contribution from biomass burning OA. During rain events, PM1 concentration is decreased almost by 60%, but its composition remains nearly the same. Oxidized OA showed slightly more decrease than primary OAs, probably due to their higher hygroscopicity. The presence of organo nitrates (ON) is also detected in ambient aerosols. Apart from real-time sampling, collected fog and rainwater samples were also analyzed via AMS in offline mode and in the ICP-OES (Inductively coupled plasma - Optical emission spectrometry) for elements. The presence of sea salt, organo nitrates and sulfates has been observed. Rainwater residues are also dominated by organics but their O/C ratios are 15-20% lower than the observed values for ambient OA. Alkali metals such as Ca, Na, K are found to be most abundant in the rainwater followed by Zn. Rainwater residues are also found to be much less oxidized than the aerosols present inside the fog water, indicating presence of less oxidized organics. These findings indicate that rain can act as an effective scavenger of different types of pollutants even for submicron particle range. Rainwater residues also contain organo sulfates which indicate that some portion of the dissolved aerosols has undergone aqueous processing, possibly inside the cloud. Highly oxidized and possibly hygroscopic OA during monsoon period compared to other seasons (winter, post monsoon), indicates that they can act

Chemical, physical, and optical evolution of biomass burning aerosols: a case study

Science.gov (United States)

Adler, G.; Flores, J. M.; Abo Riziq, A.; Borrmann, S.; Rudich, Y.

2011-02-01

In-situ chemical composition measurements of ambient aerosols have been used for characterizing the evolution of submicron aerosols from a large anthropogenic biomass burning (BB) event in Israel. A high resolution Time of Flight Aerosol Mass Spectrometer (HR-RES-TOF-AMS) was used to follow the chemical evolution of BB aerosols during a night-long, extensive nationwide wood burning event and during the following day. While these types of extensive BB events are not common in this region, burning of agricultural waste is a common practice. The aging process of the BB aerosols was followed through their chemical, physical and optical properties. Mass spectrometric analysis of the aerosol organic component showed that aerosol aging is characterized by shifting from less oxidized fresh BB aerosols to more oxidized aerosols. Evidence for aerosol aging during the day following the BB event was indicated by an increase in the organic mass, its oxidation state, the total aerosol concentration, and a shift in the modal particle diameter. The effective broadband refractive index (EBRI) was derived using a white light optical particle counter (WELAS). The average EBRI for a mixed population of aerosols dominated by open fires was m = 1.53(±0.03) + 0.07i(±0.03), during the smoldering phase of the fires we found the EBRI to be m = 1.54(±0.01) + 0.04i(±0.01) compared to m = 1.49(±0.01) + 0.02i(±0.01) of the aged aerosols during the following day. This change indicates a decrease in the overall aerosol absorption and scattering. Elevated levels of particulate Polycyclic Aromatic Hydrocarbons (PAHs) were detected during the entire event, which suggest possible implications for human health during such extensive event.

Chemical evolution of Titan’s aerosol analogues under VUV irradiation

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Carrasco, Nathalie; Gavilan, Lisseth; Tigrine, Sarah; Vettier, Ludovic; Nahon, Laurent; Pernot, Pascal

2017-10-01

Since the Cassini-CAPS measurements, organic aerosols are known to be present and formed at high altitudes in the diluted and partially ionized medium that is Titan’s ionosphere [1].After production in the ionosphere, Titan’s aerosols evolve through microphysics during their sedimentation down to Titan’s surface [2]. Starting with a few nanomers size in the upper atmosphere, they reach a fractal structure of a few hundreds nanometers close to the surface [3]. During sedimentation, aerosols are also submitted to solar irradiation. As laboratory analogs of Titan’s atmospheric aerosols (tholins) show a strong UV absorption [4], we suspect that VUV irradiation could also induce a chemical evolution of Titan’s aerosols during their descent in Titan’s atmosphere.The aim of this work ist to simulate the irradiation process occuring on the aerosols in Titan’s atmosphere and to address whether this irradiation impacts the chemical composition of the organic solids. First aerosol analogues were produced in a N2-CH4 plasma discharge as thin organic films of a few hundreds of nanometers thick [5]. Then those were irradiated at Lyman-α wavelength, the strongest VUV line in the solar spectrum, with a high photon flux on a synchrotron VUV beamline. We will present and discuss the significant chemical evolutions observed on the analogues after VUV irradiation by mid-IR absorption spectroscopy.[1] Waite et al. (2009) Science , 316, p. 870[2] Lavvas et al. (2011) Astrophysical Journal, 728:80[3] Tomasko et al. (2008) Planetary and Space Science, 56, p. 669[4] Mahjoub et al. (2012) Icarus 221, P. 670[5] Carrasco et al. (2016) Planetary and Space Science, 128, p. 52

XPS and EPXMA investigation and chemical speciation of aerosol samples formed in LWR core melting experiments

International Nuclear Information System (INIS)

Moers, H.; Jenett, H.; Kaufmann, R.; Klewe-Nebenius, H.; Pfennig, G.; Ache, H.J.

1985-09-01

Aerosol samples consisting of fission products and elements of light water reactor structural materials were collected during simulating in a laboratory scale the heat-up phase of a core melt accident. The aerosol particles were formed in a steam atmosphere at temperatures between 1200 and 1900 0 C of the melting charge. The investigation of the samples by use of X-ray photoelectron spectroscopy (XPS) permitted the chemical speciation of the detected aerosol constituents silver, cadmium, indium, tellurium, iodine, and cesium. A comparison of the elemental analysis results obtained from XPS with those achieved from electron probe X-ray micro analysis (EPXMA) revealed that aerosol particle surface and aerosol particle bulk are principally composed of the same elements and that these compositions vary with release temperature. In addition, quantitative differences between the composition of surface and bulk have only been observed for those aerosol samples which were collected at higher melting charge temperatures. In order to obtain direct information on chemical species below the surface selected samples were argon ion bombarded. Changes in composition and chemistry were monitored by XPS, and the results were interpreted in light of the effects, which were observed when appropriate standard samples were sputtered. (orig.) [de

Single particle composition measurements of artificial Calcium Carbonate aerosols

Science.gov (United States)

Zorn, S. R.; Mentel, T. F.; Schwinger, T.; Croteau, P. L.; Jayne, J.; Worsnop, D. R.; Trimborn, A.

2012-12-01

Mineral dust, with an estimated total source from natural and anthropogenic emissions of up to 2800 Tg/yr, is one of the two largest contributors to total aerosol mass, with only Sea salt having a similar source strength (up to 2600 Tg/yr). The composition of dust particles varies strongly depending on the production process and, most importantly, the source location. Therefore, the composition of single dust particles can be used both to trace source regions of air masses as well as to identify chemical aging processes. Here we present results of laboratory studies on generating artificial calcium carbonate (CaCO3) particles, a model compound for carbonaceous mineral dust particles. Particles were generated by atomizing an aqueous hydrogen carbonate solution. Water was removed using a silica diffusion dryer., then the particles were processed in an oven at temperatures up to 900°C, converting the hydrogen carbonate to its anhydrous form. The resulting aerosol was analyzed using an on-line single particle laser ablation aerosol particle time-of-flight mass spectrometer (LAAPTOF). The results confirm the conversion to calcium carbonate, and validate that the produced particles indeed can be used as a model compound for carbonaceous dust aerosols.

Systematic Relationships Between Lidar Observables and Sizes And Mineral Composition Of Dust Aerosols

Science.gov (United States)

Van Diedenhoven, Bastiaan; Stangl, Alexander; Perlwitz, Jan; Fridlind, Ann M.; Chowdhary, Jacek; Cairns, Brian

2015-01-01

The physical and chemical properties of soil dust aerosol particles fundamentally affect their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, heterogeneous formation of sulfates and nitrates on the surface of dust particles, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Lidar measurements, such as extinction-to-backscatter, color and depolarization ratios, are frequently used to distinguish between aerosol types with different physical and chemical properties. The chemical composition of aerosol particles determines their complex refractive index, hence affecting their backscattering properties. Here we present a study on how dust aerosol backscattering and depolarization properties at wavelengths of 355, 532 and 1064 nm are related to size and complex refractive index, which varies with the mineral composition of the dust. Dust aerosols are represented by collections of spheroids with a range of prolate and oblate aspect ratios and their optical properties are obtained using T-matrix calculations. We find simple, systematic relationships between lidar observables and the dust size and complex refractive index that may aid the use of space-based or airborne lidars for direct retrieval of dust properties or for the evaluation of chemical transport models using forward simulated lidar variables. In addition, we present first results on the spatial variation of forward-simulated lidar variables based on a dust model that accounts for the atmospheric cycle of eight different mineral types plus internal mixtures of seven mineral types with iron oxides, which was recently implemented in the NASA GISS Earth System ModelE2.

Chemical composition of free tropospheric aerosol for PM1 and coarse mode at the high alpine site Jungfraujoch

Directory of Open Access Journals (Sweden)

J. Cozic

2008-01-01

Full Text Available The chemical composition of submicron (fine mode and supermicron (coarse mode aerosol particles has been investigated at the Jungfraujoch high alpine research station (3580 m a.s.l., Switzerland as part of the GAW aerosol monitoring program since 1999. A clear seasonality was observed for all major components throughout the period with low concentrations in winter (predominantly free tropospheric aerosol and higher concentrations in summer (enhanced vertical transport of boundary layer pollutants. In addition, mass closure was attempted during intensive campaigns in March 2004, February–March 2005 and August 2005. Ionic, carbonaceous and non-refractory components of the aerosol were quantified as well as the PM1 and coarse mode total aerosol mass concentrations. A relatively low conversion factor of 1.8 for organic carbon (OC to particulate organic matter (OM was found in winter (February–March 2005. Organics, sulfate, ammonium, and nitrate were the major components of the fine aerosol fraction that were identified, while calcium and nitrate were the only two measured components contributing to the coarse mode. The aerosol mass concentrations for fine and coarse mode aerosol measured during the intensive campaigns were not typical of the long-term seasonality due largely to dynamical differences. Average fine and coarse mode concentrations during the intensive field campaigns were 1.7 μg m⁻³ and 2.4 μg m⁻³ in winter and 2.5 μg m⁻³ and 2.0 μg m⁻³ in summer, respectively. The mass balance of aerosols showed higher contributions of calcium and nitrate in the coarse mode during Saharan dust events (SDE than without SDE.

Elemental composition and oxidation of chamber organic aerosol

Directory of Open Access Journals (Sweden)

P. S. Chhabra

2011-09-01

Full Text Available Recently, graphical representations of aerosol mass spectrometer (AMS spectra and elemental composition have been developed to explain the oxidative and aging processes of secondary organic aerosol (SOA. It has been shown previously that oxygenated organic aerosol (OOA components from ambient and laboratory data fall within a triangular region in the f₄₄ vs. f₄₃ space, where f₄₄ and f₄₃ are the ratios of the organic signal at m/z 44 and 43 to the total organic signal in AMS spectra, respectively; we refer to this graphical representation as the "triangle plot." Alternatively, the Van Krevelen diagram has been used to describe the evolution of functional groups in SOA. In this study we investigate the variability of SOA formed in chamber experiments from twelve different precursors in both "triangle plot" and Van Krevelen domains. Spectral and elemental data from the high-resolution Aerodyne aerosol mass spectrometer are compared to offline species identification analysis and FTIR filter analysis to better understand the changes in functional and elemental composition inherent in SOA formation and aging. We find that SOA formed under high- and low-NO_x conditions occupy similar areas in the "triangle plot" and Van Krevelen diagram and that SOA generated from already oxidized precursors allows for the exploration of areas higher on the "triangle plot" not easily accessible with non-oxidized precursors. As SOA ages, it migrates toward the top of the triangle along a path largely dependent on the precursor identity, which suggests increasing organic acid content and decreasing mass spectral variability. The most oxidized SOA come from the photooxidation of methoxyphenol precursors which yielded SOA O/C ratios near unity. α-pinene ozonolysis and naphthalene photooxidation SOA systems have had the highest degree of mass closure in previous chemical characterization studies and also show the

Aerosol chemical physics

International Nuclear Information System (INIS)

Marlow, W.H.

1982-01-01

A classification of the research fields in the chemical physics of aerosol microparticles is given. The emphasis lies on the microphysics of isolated particles and clusters and on physical transformations and thermodynamics. (LDN)

A case study of highly time-resolved evolution of aerosol chemical composition and optical properties during severe haze pollution in Shanghai, China

Science.gov (United States)

Zhu, W.; Cheng, Z.; Lou, S.

2017-12-01

Despite of extensive efforts into characterization of the sources in severe haze pollution periods in the megacity of Shanghai, the study of aerosol composition, mass-size distribution and optical properties to PM1 in the pollution periods remain poorly understood. Here we conducted a 47days real-time measurement of submicron aerosol (PM1) composition and size distribution by a High-Resolution Time-of-Flight Aerosol Mass spectrometer (HR-TOF-AMS), particle light scattering by a Cavity Attenuated Phase Shift ALBedo monitor (CAPS-ALB) and Photoacoustic Extinctionmeter (PAX) in Shanghai, China, from November 28, 2016 to January 12, 2017. The average PM1 concentration was 85.9(±14.7) μg/m3 during the pollution period, which was nearly 4 times higher than that of clean period. Increased scattering coefficient during EP was associated with higher secondary inorganic aerosols and organics. We also observed organics mass size distribution for different pollution extents showing different distribution characteristics. There were no obvious differences for ammonium nitrate and ammonium sulfate among the pollution periods, which represented single peak distributions, and peaks ranged at 650-700nm and 700nm, respectively. A strong relationship can be expected between PM1 compounds mass concentration size distribution and scattering coefficient, suggesting that chemical composition, size distribution of the particles and their variations could also contribute to the extinction coefficients. Organics and secondary inorganic species to particle light scattering were quantified. The results showed that organics and ammonium nitrate were the largest contribution to scattering coefficients of PM1. The contribution of (NH4)2SO4 to the light scattering exceeded that of NH4NO3 during clean period due to the enhanced sulfate concentrations. Our results elucidate substantial changes of aerosol composition, formation mechanisms, size distribution and optical properties due to local

Predicting the mineral composition of dust aerosols - Part 1: Representing key processes

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Perlwitz, J. P.; Pérez García-Pando, C.; Miller, R. L.

2015-02-01

Soil dust aerosols created by wind erosion are typically assigned globally uniform physical and chemical properties within Earth system models, despite known regional variations in the mineral content of the parent soil. Mineral composition of the aerosol particles is important to their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, coating by heterogeneous uptake of sulfates and nitrates, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Here, aerosol mineral composition is derived by extending a method that provides the composition of a wet-sieved soil. The extension accounts for measurements showing significant differences between the mineral fractions of the wet-sieved soil and the resulting aerosol concentration. For example, some phyllosilicate aerosols are more prevalent at silt sizes, even though they are nearly absent in a soil whose aggregates are dispersed by wet sieving during analysis. We reconstruct the undispersed size distribution of the original soil that is subject to wind erosion. An empirical constraint upon the relative emission of clay and silt is applied that further differentiates the soil and aerosol mineral composition. In addition, a method is proposed for mixing minerals with small impurities composed of iron oxides. These mixtures are important for transporting iron far from the dust source, because pure iron oxides are more dense and vulnerable to gravitational removal than most minerals comprising dust aerosols. A limited comparison to measurements from North Africa shows that the extension brings the model into better agreement, consistent with a more extensive comparison to global observations as well as measurements of elemental composition downwind of the Sahara, as described in companion articles.

Long-term Chemical Characterization of Submicron Aerosol Particles in the Amazon Forest - ATTO Station

Science.gov (United States)

Carbone, S.; Brito, J.; Rizzo, L. V.; Holanda, B. A.; Cirino, G. G.; Saturno, J.; Krüger, M. L.; Pöhlker, C.; Ng, N. L.; Xu, L.; Andreae, M. O.; Artaxo, P.

2015-12-01

The study of the chemical composition of aerosol particles in the Amazon forest represents a step forward to understand the strong coupling between the atmosphere and the forest. For this reason submicron aerosol particles were investigated in the Amazon forest, where biogenic and anthropogenic aerosol particles coexist at the different seasons (wet/dry). The measurements were performed at the ATTO station, which is located about 150 km northeast of Manaus. At ATTO station the Aerosol chemical speciation monitor (ACSM, Aerodyne) and the Multiangle absorption photometer (MAAP, Thermo 5012) have been operated continuously from March 2014 to July 2015. In this study, long-term measurements (near-real-time, ~30 minutes) of PM1 chemical composition were investigated for the first time in this environment.The wet season presented lower concentrations than the dry season (~5 times). In terms of chemical composition, both seasons were dominated by organics (75 and 63%) followed by sulfate (11 and 13%). Nitrate presented different ratio values between the mass-to-charges 30 to 46 (main nitrate fragments) suggesting the presence of nitrate as inorganic and organic nitrate during both seasons. The results indicated that about 75% of the nitrate signal was from organic nitrate during the dry season. In addition, several episodes with elevated amount of chloride, likely in the form of sea-salt from the Atlantic Ocean, were observed during the wet season. During those episodes, chloride comprised up to 7% of the PM1. During the dry season, chloride was also observed; however, with different volatility, which suggested that Chloride was present in different form and source. Moreover, the constant presence of sulfate and BC during the wet season might be related to biomass burning emissions from Africa. BC concentration was 2.5 times higher during the dry season. Further characterization of the organic fraction was accomplished with the positive matrix factorization (PMF), which

Chemical Composition of Aerosol from an E-Cigarette: A Quantitative Comparison with Cigarette Smoke.

Science.gov (United States)

Margham, Jennifer; McAdam, Kevin; Forster, Mark; Liu, Chuan; Wright, Christopher; Mariner, Derek; Proctor, Christopher

2016-10-17

There is interest in the relative toxicities of emissions from electronic cigarettes and tobacco cigarettes. Lists of cigarette smoke priority toxicants have been developed to focus regulatory initiatives. However, a comprehensive assessment of e-cigarette chemical emissions including all tobacco smoke Harmful and Potentially Harmful Constituents, and additional toxic species reportedly present in e-cigarette emissions, is lacking. We examined 150 chemical emissions from an e-cigarette (Vype ePen), a reference tobacco cigarette (Ky3R4F), and laboratory air/method blanks. All measurements were conducted by a contract research laboratory using ISO 17025 accredited methods. The data show that it is essential to conduct laboratory air/method measurements when measuring e-cigarette emissions, owing to the combination of low emissions and the associated impact of laboratory background that can lead to false-positive results and overestimates. Of the 150 measurands examined in the e-cigarette aerosol, 104 were not detected and 21 were present due to laboratory background. Of the 25 detected aerosol constituents, 9 were present at levels too low to be quantified and 16 were generated in whole or in part by the e-cigarette. These comprised major e-liquid constituents (nicotine, propylene glycol, and glycerol), recognized impurities in Pharmacopoeia-quality nicotine, and eight thermal decomposition products of propylene glycol or glycerol. By contrast, approximately 100 measurands were detected in mainstream cigarette smoke. Depending on the regulatory list considered and the puffing regime used, the emissions of toxicants identified for regulation were from 82 to >99% lower on a per-puff basis from the e-cigarette compared with those from Ky3R4F. Thus, the aerosol from the e-cigarette is compositionally less complex than cigarette smoke and contains significantly lower levels of toxicants. These data demonstrate that e-cigarettes can be developed that offer the potential

Chemical composition of wildland fire emissions

Science.gov (United States)

Shawn P. Urbanski; Wei Min Hao; Stephen Baker

2009-01-01

Wildland fires are major sources of trace gases and aerosol, and these emissions are believed to significantly influence the chemical composition of the atmosphere and the earth's climate system. The wide variety of pollutants released by wildland fire include greenhouse gases, photochemically reactive compounds, and fine and coarse particulate matter. Through...

Aerosolization, Chemical Characterization, Hygroscopicity and Ice Formation of Marine Biogenic Particles

Science.gov (United States)

Alpert, P. A.; Radway, J.; Kilthau, W.; Bothe, D.; Knopf, D. A.; Aller, J. Y.

2013-12-01

The oceans cover the majority of the earth's surface, host nearly half the total global primary productivity and are a major source of atmospheric aerosol particles. However, effects of biological activity on sea spray generation and composition, and subsequent cloud formation are not well understood. Our goal is to elucidate these effects which will be particularly important over nutrient rich seas, where microorganisms can reach concentrations of 10^9 per mL and along with transparent exopolymer particles (TEP) can become aerosolized. Here we report the results of mesocosm experiments in which bubbles were generated by two methods, either recirculating impinging water jets or glass frits, in natural or artificial seawater containing bacteria and unialgal cultures of three representative phytoplankton species, Thalassiosira pseudonana, Emiliania huxleyi, and Nannochloris atomus. Over time we followed the size distribution of aerosolized particles as well as their hygroscopicity, heterogeneous ice nucleation potential, and individual physical-chemical characteristics. Numbers of cells and the mass of dissolved and particulate organic carbon (DOC, POC), TEP (which includes polysaccharide-containing microgels and nanogels >0.4 μm in diameter) were determined in the bulk water, the surface microlayer, and aerosolized material. Aerosolized particles were also impacted onto substrates for ice nucleation and water uptake experiments, elemental analysis using computer controlled scanning electron microscopy and energy dispersive analysis of X-rays (CCSEM/EDX), and determination of carbon bonding with scanning transmission X-ray microscopy and near-edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS). Regardless of bubble generation method, the overall concentration of aerosol particles, TEP, POC and DOC increased as concentrations of bacterial and phytoplankton cells increased, stabilized, and subsequently declined. Particles cloud formation and potential

A review of current knowledge concerning PM2. 5 chemical composition, aerosol optical properties and their relationships across China

Science.gov (United States)

Tao, Jun; Zhang, Leiming; Cao, Junji; Zhang, Renjian

2017-08-01

To obtain a thorough knowledge of PM2. 5 chemical composition and its impact on aerosol optical properties across China, existing field studies conducted after the year 2000 are reviewed and summarized in terms of geographical, interannual and seasonal distributions. Annual PM2. 5 was up to 6 times the National Ambient Air Quality Standards (NAAQS) in some megacities in northern China. Annual PM2. 5 was higher in northern than southern cities, and higher in inland than coastal cities. In a few cities with data longer than a decade, PM2. 5 showed a slight decrease only in the second half of the past decade, while carbonaceous aerosols decreased, sulfate (SO42-) and ammonium (NH4+) remained at high levels, and nitrate (NO3-) increased. The highest seasonal averages of PM2. 5 and its major chemical components were typically observed in the cold seasons. Annual average contributions of secondary inorganic aerosols to PM2. 5 ranged from 25 to 48 %, and those of carbonaceous aerosols ranged from 23 to 47 %, both with higher contributions in southern regions due to the frequent dust events in northern China. Source apportionment analysis identified secondary inorganic aerosols, coal combustion and traffic emission as the top three source factors contributing to PM2. 5 mass in most Chinese cities, and the sum of these three source factors explained 44 to 82 % of PM2. 5 mass on annual average across China. Biomass emission in most cities, industrial emission in industrial cities, dust emission in northern cities and ship emission in coastal cities are other major source factors, each of which contributed 7-27 % to PM2. 5 mass in applicable cities. The geographical pattern of scattering coefficient (bsp) was similar to that of PM2. 5, and that of aerosol absorption coefficient (bap) was determined by elemental carbon (EC) mass concentration and its coating. bsp in ambient condition of relative humidity (RH) = 80 % can be amplified by about 1.8 times that under dry conditions

The Impact of Aerosol Particle Mixing State on the Hygroscopicity of Sea Spray Aerosol.

Science.gov (United States)

Schill, Steven R; Collins, Douglas B; Lee, Christopher; Morris, Holly S; Novak, Gordon A; Prather, Kimberly A; Quinn, Patricia K; Sultana, Camille M; Tivanski, Alexei V; Zimmermann, Kathryn; Cappa, Christopher D; Bertram, Timothy H

2015-06-24

Aerosol particles influence global climate by determining cloud droplet number concentrations, brightness, and lifetime. Primary aerosol particles, such as those produced from breaking waves in the ocean, display large particle-particle variability in chemical composition, morphology, and physical phase state, all of which affect the ability of individual particles to accommodate water and grow into cloud droplets. Despite such diversity in molecular composition, there is a paucity of methods available to assess how particle-particle variability in chemistry translates to corresponding differences in aerosol hygroscopicity. Here, an approach has been developed that allows for characterization of the distribution of aerosol hygroscopicity within a chemically complex population of atmospheric particles. This methodology, when applied to the interpretation of nascent sea spray aerosol, provides a quantitative framework for connecting results obtained using molecular mimics generated in the laboratory with chemically complex ambient aerosol. We show that nascent sea spray aerosol, generated in situ in the Atlantic Ocean, displays a broad distribution of particle hygroscopicities, indicative of a correspondingly broad distribution of particle chemical compositions. Molecular mimics of sea spray aerosol organic material were used in the laboratory to assess the volume fractions and molecular functionality required to suppress sea spray aerosol hygroscopicity to the extent indicated by field observations. We show that proper accounting for the distribution and diversity in particle hygroscopicity and composition are important to the assessment of particle impacts on clouds and global climate.

Global chemical composition of ambient fine particulate matter for exposure assessment.

Science.gov (United States)

Philip, Sajeev; Martin, Randall V; van Donkelaar, Aaron; Lo, Jason Wai-Ho; Wang, Yuxuan; Chen, Dan; Zhang, Lin; Kasibhatla, Prasad S; Wang, Siwen; Zhang, Qiang; Lu, Zifeng; Streets, David G; Bittman, Shabtai; Macdonald, Douglas J

2014-11-18

Epidemiologic and health impact studies are inhibited by the paucity of global, long-term measurements of the chemical composition of fine particulate matter. We inferred PM2.5 chemical composition at 0.1° × 0.1° spatial resolution for 2004-2008 by combining aerosol optical depth retrieved from the MODIS and MISR satellite instruments, with coincident profile and composition information from the GEOS-Chem global chemical transport model. Evaluation of the satellite-model PM2.5 composition data set with North American in situ measurements indicated significant spatial agreement for secondary inorganic aerosol, particulate organic mass, black carbon, mineral dust, and sea salt. We found that global population-weighted PM2.5 concentrations were dominated by particulate organic mass (11.9 ± 7.3 μg/m(3)), secondary inorganic aerosol (11.1 ± 5.0 μg/m(3)), and mineral dust (11.1 ± 7.9 μg/m(3)). Secondary inorganic PM2.5 concentrations exceeded 30 μg/m(3) over East China. Sensitivity simulations suggested that population-weighted ambient PM2.5 from biofuel burning (11 μg/m(3)) could be almost as large as from fossil fuel combustion sources (17 μg/m(3)). These estimates offer information about global population exposure to the chemical components and sources of PM2.5.

Chemical composition and sources of atmospheric aerosols at Djougou (Benin)

Science.gov (United States)

Ouafo-Leumbe, Marie-Roumy; Galy-Lacaux, Corinne; Liousse, Catherine; Pont, Veronique; Akpo, Aristide; Doumbia, Thierno; Gardrat, Eric; Zouiten, Cyril; Sigha-Nkamdjou, Luc; Ekodeck, Georges Emmanuel

2017-06-01

In the framework of the INDAAF (International Network to study Deposition and Atmospheric chemistry in AFrica) program, atmospheric aerosols were collected in PM2.5 and PM10 size fractions at Djougou, Benin, in the West Africa, from November, 2005 to October, 2009. Particulate carbon, ionic species, and trace metals were analyzed. Weekly PM2.5 and PM10 total mass concentrations varied between 0.7 and 47.3 µg m-3 and 1.4-148.3 µg m-3, respectively. We grouped the aerosol chemical compounds into four classes: dust, particulate organic matter (POM), elemental carbon (EC), and ions. We studied the annual variation of each class to determine their contribution in the total aerosol mass concentration and finally to investigate their potential emission sources. On an annual basis, the species presented a well-marked seasonality, with the peak of mass concentration for both sizes registered in dry season, 67 ± 2 to 86 ± 9 versus 14 ± 9 to 34 ± 5% in wet season. These values emphasized the seasonality of the emissions and the relative weak interannual standard deviation indicates the low variability of the seasonality. At the seasonal scale, major contributions to the aerosol chemistry in the dry season are: dust (26-59%), POM (30-59%), EC (5-9%), and ions (3-5%), suggesting a predominance of Sahelian and Saharan dust emissions and biomass burning source in this season. In the wet season, POM is predominant, followed by dust, EC, and ions. These results point out the contribution of surrounded biofuel combustion used for cooking and biogenic emissions during the wet season.

Assessment of microphysical and chemical factors of aerosols over seas of the Russian Artic Eastern Section

Science.gov (United States)

Golobokova, Liudmila; Polkin, Victor

2014-05-01

The newly observed kickoff of the Northern Route development drew serious attention to state of the Arctic Resource environment. Occurring climatic and environmental changes are more sensitively seen in polar areas in particular. Air environment control allows for making prognostic assessments which are required for planning hazardous environmental impacts preventive actions. In August - September 2013, RV «Professor Khlustin» Northern Sea Route expeditionary voyage took place. En-route aerosol sampling was done over the surface of the Beringov, Chukotka and Eastern-Siberia seas (till the town of Pevek). The purpose of sampling was to assess spatio-temporal variability of optic, microphysical and chemical characteristics of aerosol particles of the surface layer within different areas adjacent to the Northern Sea Route. Aerosol test made use of automated mobile unit consisting of photoelectric particles counter AZ-10, aetalometr MDA-02, aspirator on NBM-1.2 pump chassis, and the impactor. This set of equipment allows for doing measurements of number concentration, dispersed composition of aerosols within sizes d=0.3-10 mkm, mass concentration of submicron sized aerosol, and filter-conveyed aerosols sampling. Filter-conveyed aerosols sampling was done using method accepted by EMEP and EANET monitoring networks. The impactor channel was upgraded to separate particles bigger than 1 mkm in size, and the fine grain fraction settled down on it. Reverse 5-day and 10-day trajectories of air mass transfer executed at heights of 10, 1500 and 3500 m were analyzed. The heights were selected by considerations that 3000 m is the height which characterizes air mass trend in the lower troposphere. 1500 m is the upper border of the atmospheric boundary layer, and the sampling was done in the Earth's surface layer at less than 10 m. Minimum values of the bespoken microphysical characteristics are better characteristic of higher latitudes where there are no man induced sources of

Chemical and isotopic composition of secondary organic aerosol generated by α-pinene ozonolysis

DEFF Research Database (Denmark)

Meusinger, Carl; Dusek, Ulrike; King, Stephanie M.

2017-01-01

-NOx conditions, with OH scavengers and in the absence of seed particles. The excess of ozone and long residence time in the flow chamber ensured that virtually all α-pinene had reacted. Product SOA was collected on two sequential quartz filters. The filters were analysed offline by heating them stepwise from 100...... it is difficult to apply because neither the isotopic composition of aerosol precursors nor the fractionation of aerosol forming processes is well characterised. In this paper, SOA formation from ozonolysis of α-pinene - an important precursor and perhaps the best-known model system used in laboratory studies...... - was investigated using position-dependent and average determinations of 13C in α-pinene and advanced analysis of reaction products using thermal-desorption proton-transfer-reaction mass spectrometry (PTR-MS). The total carbon (TC) isotopic composition δ13C of the initial α-pinene was measured, and the δ13C...

Chemical characteristics of submicron particles at the central Tibetan Plateau: insights from aerosol mass spectrometry

Science.gov (United States)

Xu, Jianzhong; Zhang, Qi; Shi, Jinsen; Ge, Xinlei; Xie, Conghui; Wang, Junfeng; Kang, Shichang; Zhang, Ruixiong; Wang, Yuhang

2018-01-01

Recent studies have revealed a significant influx of anthropogenic aerosol from South Asia to the Himalayas and Tibetan Plateau (TP) during pre-monsoon period. In order to characterize the chemical composition, sources, and transport processes of aerosol in this area, we carried out a field study during June 2015 by deploying a suite of online instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) and a multi-angle absorption photometer (MAAP) at Nam Co station (90°57' E, 30°46' N; 4730 m a.s.l.) at the central of the TP. The measurements were made at a period when the transition from pre-monsoon to monsoon occurred. The average ambient mass concentration of submicron particulate matter (PM1) over the whole campaign was ˜ 2.0 µg m-3, with organics accounting for 68 %, followed by sulfate (15 %), black carbon (8 %), ammonium (7 %), and nitrate (2 %). Relatively higher aerosol mass concentration episodes were observed during the pre-monsoon period, whereas persistently low aerosol concentrations were observed during the monsoon period. However, the chemical composition of aerosol during the higher aerosol concentration episodes in the pre-monsoon season was on a case-by-case basis, depending on the prevailing meteorological conditions and air mass transport routes. Most of the chemical species exhibited significant diurnal variations with higher values occurring during afternoon and lower values during early morning, whereas nitrate peaked during early morning in association with higher relative humidity and lower air temperature. Organic aerosol (OA), with an oxygen-to-carbon ratio (O / C) of 0.94, was more oxidized during the pre-monsoon period than during monsoon (average O / C ratio of 0.72), and an average O / C was 0.88 over the entire campaign period, suggesting overall highly oxygenated aerosol in the central TP. Positive matrix factorization of the high-resolution mass spectra of OA identified two oxygenated

Nanoparticulate cerium dioxide and cerium dioxide-titanium dioxide composite thin films on glass by aerosol assisted chemical vapour deposition

International Nuclear Information System (INIS)

Qureshi, Uzma; Dunnill, Charles W.; Parkin, Ivan P.

2009-01-01

Two series of composite thin films were deposited on glass by aerosol assisted chemical vapour deposition (AACVD)-nanoparticulate cerium dioxide and nanoparticulate cerium dioxide embedded in a titanium dioxide matrix. The films were analysed by a range of techniques including UV-visible absorption spectroscopy, X-ray diffraction, scanning electron microscopy and energy dispersive analysis by X-rays. The AACVD prepared films showed the functional properties of photocatalysis and super-hydrophilicity. The CeO 2 nanoparticle thin films displaying photocatalysis and photo-induced hydrophilicity almost comparable to that of anatase titania.

Observations of Chemical Composition in Frost Flower Growth Process and Their Implication in Aerosol Production and Bromine Activation Chemistry

Science.gov (United States)

Alvarez-Aviles, L.; Simpson, W. R.; Douglas, T. A.; Sturm, M.; Perovich, D. K.

2006-12-01

Frost flowers are believed to be responsible for most of the salt aerosol and possibly the bromine in the gas phase during springtime in Polar Regions. Frost flowers are vapor deposited ice crystals that form on new forming sea ice and wick brine from the sea-ice surface resulting in high salinities. We propose a conceptual model of frost flower growth and chemical fractionation using chemical analysis to support this model. We also consider how the chemical composition of frost flowers can tell us about the role of frost flowers in bromine activation and aerosol production. Our conceptual model is centered in two important events that occur when sea ice grows and the ice surface temperature gets colder. Brine on the sea-ice surface is drawn up the frost flower by capillary forces, therefore the high salinity values found. Secondarily salt hydrates begin to precipitate at certain temperatures. These precipitation reactions modify the chemical composition of the frost flowers and residual brine, and are the main topic of this research. We found variability and generally depletion of sulfate as compared to sea-water composition in most of the mature frost flowers. This result is in agreement with the literature, which proposes the depletion in sulfate occurs because mirabilite (Na2SO4 · 10H2O) precipitates before the brine is wicked. The observation of some slightly sulfate-enhanced samples in addition to depleted samples indicates that the brine/frost flower environment is the location where mirabilite precipitation and separation from residual brine occurs. Frost flowers bromide enhancement factors are all, within analytical limits, identical to sea water, although nearby snow is depleted in bromide. Because of the high salt concentrations in frost flowers, significant bromine activation could occur from frost flowers without being detected by this measurement. However, if all bromide activation occurred on frost flowers, and frost flowers are not depleted in

Real-Time Characterization of Aerosol Particle Composition above the Urban Canopy in Beijing: Insights into the Interactions between the Atmospheric Boundary Layer and Aerosol Chemistry.

Science.gov (United States)

Sun, Yele; Du, Wei; Wang, Qingqing; Zhang, Qi; Chen, Chen; Chen, Yong; Chen, Zhenyi; Fu, Pingqing; Wang, Zifa; Gao, Zhiqiu; Worsnop, Douglas R

2015-10-06

Despite extensive efforts into the characterization of air pollution during the past decade, real-time characterization of aerosol particle composition above the urban canopy in the megacity Beijing has never been performed to date. Here we conducted the first simultaneous real-time measurements of aerosol composition at two different heights at the same location in urban Beijing from December 19, 2013 to January 2, 2014. The nonrefractory submicron aerosol (NR-PM1) species were measured in situ by a high-resolution aerosol mass spectrometer at near-ground level and an aerosol chemical speciation monitor at 260 m on a 325 m meteorological tower in Beijing. Secondary aerosol showed similar temporal variations between ground level and 260 m, whereas much weaker correlations were found for the primary aerosol. The diurnal evolution of the ratios and correlations of aerosol species between 260 m and the ground level further illustrated a complex interaction between vertical mixing processes and local source emissions on aerosol chemistry in the atmospheric boundary layer. As a result, the aerosol compositions at the two heights were substantially different. Organic aerosol (OA), mainly composed of primary OA (62%), at the ground level showed a higher contribution to NR-PM1 (65%) than at 260 m (54%), whereas a higher concentration and contribution (15%) of nitrate was observed at 260 m, probably due to the favorable gas-particle partitioning under lower temperature conditions. In addition, two different boundary layer structures were observed, each interacting differently with the evolution processes of aerosol chemistry.

Instrumentation for tropospheric aerosol characterization

Energy Technology Data Exchange (ETDEWEB)

Shi, Z.; Young, S.E.; Becker, C.H.; Coggiola, M.J. [SRI International, Menlo Park, CA (United States); Wollnik, H. [Giessen Univ. (Germany)

1997-12-31

A new instrument has been developed that determines the abundance, size distribution, and chemical composition of tropospheric and lower stratospheric aerosols with diameters down to 0.2 {mu}m. In addition to aerosol characterization, the instrument also monitors the chemical composition of the ambient gas. More than 25.000 aerosol particle mass spectra were recorded during the NASA-sponsored Subsonic Aircraft: Contrail and Cloud Effects Special Study (SUCCESS) field program using NASA`s DC-8 research aircraft. (author) 7 refs.

Instrumentation for tropospheric aerosol characterization

Energy Technology Data Exchange (ETDEWEB)

Shi, Z; Young, S E; Becker, C H; Coggiola, M J [SRI International, Menlo Park, CA (United States); Wollnik, H [Giessen Univ. (Germany)

1998-12-31

A new instrument has been developed that determines the abundance, size distribution, and chemical composition of tropospheric and lower stratospheric aerosols with diameters down to 0.2 {mu}m. In addition to aerosol characterization, the instrument also monitors the chemical composition of the ambient gas. More than 25.000 aerosol particle mass spectra were recorded during the NASA-sponsored Subsonic Aircraft: Contrail and Cloud Effects Special Study (SUCCESS) field program using NASA`s DC-8 research aircraft. (author) 7 refs.

Nonurban aerosol composition near Beijing, China

International Nuclear Information System (INIS)

Winchester, J.W.; Darzi, M.; Leslie, A.C.D.; Wang, M.; Ren, L.; Lue, W.; Hansson, H.C.; Lannefors, H.

1981-01-01

The urban aerosol plume of Beijing has been sampled as a function of particle size and time at a site 110 km NE of the city, 9-16 March 1980, during the season for space heating by coal combustion. A fine particle mode, contained mostly in the 0.5-2 μm aerodynamic diameter range, could be distinguished from a coarse mode of dust having terrestrial composition by reference to the size distribution of Ca. Elemental composition determined by PIXE analysis for 17 elements, including S and heavy metals, indicates fine mode concentrations higher than background aerosol but with a similarity to cleaner air with respect to both relative elemental abundances and elemental particle size distributions. The results indicate that elements contained in aged coal combustion aerosol occur mainly in 0.5-2 μMAD particles, not smaller, and the aerosol is not substantially different from background aerosol except in overall concentrations. This result may simplify the prediction of the impact of coal combustion on air quality. The results also hint that the background aerosol in more remote continental areas may also be combustion derived. (orig.)

Chemical characteristics of submicron particles at the central Tibetan Plateau: insights from aerosol mass spectrometry

Directory of Open Access Journals (Sweden)

J. Xu

2018-01-01

Full Text Available Recent studies have revealed a significant influx of anthropogenic aerosol from South Asia to the Himalayas and Tibetan Plateau (TP during pre-monsoon period. In order to characterize the chemical composition, sources, and transport processes of aerosol in this area, we carried out a field study during June 2015 by deploying a suite of online instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS and a multi-angle absorption photometer (MAAP at Nam Co station (90°57′ E, 30°46′ N; 4730 m a.s.l. at the central of the TP. The measurements were made at a period when the transition from pre-monsoon to monsoon occurred. The average ambient mass concentration of submicron particulate matter (PM1 over the whole campaign was  ∼  2.0 µg m−3, with organics accounting for 68 %, followed by sulfate (15 %, black carbon (8 %, ammonium (7 %, and nitrate (2 %. Relatively higher aerosol mass concentration episodes were observed during the pre-monsoon period, whereas persistently low aerosol concentrations were observed during the monsoon period. However, the chemical composition of aerosol during the higher aerosol concentration episodes in the pre-monsoon season was on a case-by-case basis, depending on the prevailing meteorological conditions and air mass transport routes. Most of the chemical species exhibited significant diurnal variations with higher values occurring during afternoon and lower values during early morning, whereas nitrate peaked during early morning in association with higher relative humidity and lower air temperature. Organic aerosol (OA, with an oxygen-to-carbon ratio (O ∕ C of 0.94, was more oxidized during the pre-monsoon period than during monsoon (average O ∕ C ratio of 0.72, and an average O ∕ C was 0.88 over the entire campaign period, suggesting overall highly oxygenated aerosol in the central TP. Positive matrix factorization of the

Two year-long continuous monitoring of PM1 aerosol chemical composition at the Cyprus Atmospheric Observatory. Source apportionment of the Organic content and geographic origins.

Science.gov (United States)

Stavroulas, Iasonas; Pikridas, Michael; Oikonomou, Kostantina; Vasiliadou, Emily; Savvides, Chrysanthos; Vrekoussis, Mihalis; Mihalopoulos, Nikolaos; Gros, Valerie; Sciare, Jean

2017-04-01

Particulate matter with diameter smaller than 1{μ}m (PM1) induces direct and indirect effects on local and regional pollution, global climate and health. As of the beginning of 2015, the chemical composition of submicron aerosols, is continuously being monitored at the newly established Cyprus Atmospheric Observatory (CAO, http://www.cyi.ac.cy/index.php/cao.html), a national facility of the ACTRIS Research Infrastructure operated by The Cyprus Institute. Cyprus, an island located in the Eastern Mediterranean Middle East region and influenced by diverse air masses throughout the year, is ideal for monitoring photochemically aged aerosols and gaseous pollutants of both natural and anthropogenic origin. Furthermore this is a unique dataset for this area in such proximity to the Middle East, a poorly documented area in terms of atmospheric aerosol observations. An Aerodyne Quadrupole Aerosol Chemical Speciation Monitor (Q-ACSM) is currently deployed at the CAO premises (35.04N - 33.06E) situated at the rural area of Agia Marina Xyliatou on the foothill of mount Troodos at an elevation of 532m above sea level (asl). The ACSM delivers chemical composition of the major non-refractory aerosol (PM1) chemical constituents (organics, sulfate, nitrate, ammonium, chloride) with an effective (close to 100{%}) collection efficiency for particles in the diameter range of 65-700 nm at a 30 minute temporal resolution. Black Carbon (BC) was also monitored using both Magee Scientific AE-31 and AE-33 aethalometers. Quality control of the PM chemical dataset was conducted by comparison with chemical analysis performed on collocated 24-h filter samples (PM1) and comparison with 1-h PM2.5 derived from a Thermo Scientific TEOM (1400a) Monitor. Positive Matrix Factorization (PMF) was conducted and different organic aerosol factors were distinguished using the Igor based SoFi toolkit utilizing the ME-2 multilinear engine. Air mass origin was investigated for each measurement day using the

Chemical and geochemical composition of spring-summer Arctic aerosol collected at Ny Alesund, Svalbard Islands.

Science.gov (United States)

Udisti, Roberto; Becagli, Silvia; Caiazzo, Laura; Cappelletti, David; Giardi, Fabio; Grotti, Marco; Lucarelli, Franco; Moroni, Beatrice; Nava, Silvia; Severi, Mirko; Traversi, Rita

2017-04-01

Since March 2010, spring-summer (usually March - September) campaigns were continuously carried out at the Italian Gruvebadet Observatory, Ny Alesund, Svalbard Island. Aerosol was sampled by PM10 (daily) and 4-stage (4-day resolution) collector devices and size distribution was evaluated at 10 min resolution in the range 10 nm - 20 um (106 size classes by a TSI SMPS-APS integrated system). Six-year (2010-2015) PM10 and size-segregated (>10, 10-2.5, 2.5-1, metal content (major and trace metals, including Rare Earth Elements - REEs, by PIXE and ICP-MS), Pb isotopic composition (by ICP-MS) and Elemental and Organic Carbon (EC-OC) concentrations. The data set was elaborated by multi-parametric statistical analysis (Positive Matrix Factorization - PMF), in order to identifying and quantifying the contribution of the main anthropic and natural aerosol sources. Particular attention was spent in evaluating the anthropic contribution of nss-sulphate, nitrate, EC and heavy metals during the Arctic Haze in spring. The isotopic composition of Pb was used in identifying the source areas (North America, Greenland, North Europe, Siberia, Iceland) of anthropic emissions as a function of seasonality (different atmospheric circulation pathway). Crustal metals and, especially, REEs anomalies (with respect to the Chondrite-normalized profile) allowed characterizing the dust emissions from their Potential Source Areas (PSA). Biogenic markers (especially methane sulfonic acid - MSA - and bio-nss-sulphate) was used to obtain relevant information about the relationship between marine biogenic activity (primary productivity) and sea ice coverage and atmospheric conditions (irradiance, temperature, circulation pathways). The seasonal pattern of the nitrate deposition was also investigated. Chemical and geochemical measurements were compared with high-resolution size distribution and back-trajectory cluster analysis in order to understand the seasonal pattern of the contributions of long

Chemical Composition Based Aerosol Optical Properties According to Size Distribution and Mixture Types during Smog and Asian Dust Events in Seoul, Korea

Science.gov (United States)

Jung, Chang Hoon; Lee, Ji Yi; Um, Junshik; Lee, Seung Soo; Kim, Yong Pyo

2018-02-01

This study investigated the optical properties of aerosols involved in different meteorological events, including smog and Asian dust days. Carbonaceous components and inorganic species were measured in Seoul, Korea between 25 and 31 March 2012. Based on the measurements, the optical properties of aerosols were calculated by considering composition, size distribution, and mixing state of aerosols. To represent polydisperse size distributions of aerosols, a lognormal size distribution with a wide range of geometric mean diameters and geometric standard deviations was used. For the optical property calculations, the Mie theory was used to compute single-scattering properties of aerosol particles with varying size and composition. Analysis of the sampled data showed that the water-soluble components of organic matter increased on smog days, whereas crustal elements increased on dust days. The water content significantly influenced the optical properties of aerosols during the smog days as a result of high relative humidity and an increase in the water-soluble component. The absorption coefficients depended on the aerosol mixture type and the aerosol size distributions. Therefore, to improve our knowledge on radiative impacts of aerosols, especially the regional impacts of aerosols in East Asia, accurate measurements of aerosols, such as size distribution, composition, and mixture type, under different meteorological conditions are required.

Influence of mineral dust transport on the chemical composition and physical properties of the Eastern Mediterranean aerosol

Science.gov (United States)

Koçak, M.; Theodosi, C.; Zarmpas, P.; Séguret, M. J. M.; Herut, B.; Kallos, G.; Mihalopoulos, N.; Kubilay, N.; Nimmo, M.

2012-09-01

Bulk aerosol samples were collected from three different coastal rural sites located around the Eastern Mediterranean, (i) Erdemli (ER), Turkey, (ii) Heraklion (HR), Crete, Greece, and (iii) Tel Shikmona (TS), Israel, during two distinct mineral dust periods (October, 2007 and April, 2008) in order to explore the temporal and geographical variability in the aerosol chemical composition. Samples were analyzed for trace elements (Al, Fe, Mn, Ca, Cr, Zn, Cu, V, Ni, Cd, Pb) and water-soluble ions (Cl-, NO3-, SO42-, C2O42-, Na+, NH4+, K+, Mg2+ and Ca2+). The dust events were categorized on the basis of Al concentrations >1000 ng m-3, SKIRON dust forecast model and 3-day back trajectories into three groups namely, Middle East, Mixed and Saharan desert. ER and TS were substantially affected by dust events originating from the Middle East, particularly in October, whilst HR was not influenced by dust transport from the Middle East. Higher AOT values were particularly associated with higher Al concentrations. Contrary to the highest Al concentration: 6300 ng m-3, TS showed relatively lower AI and AOT. Al concentrations at ER were similar for October and April, whilst OMI-AI and AOT values were ˜2 times higher in April. This might be attributed to the weak sensitivity of the TOMS instrument to absorbing aerosols near the ground and optical difference between Middle East and Saharan desert dusts. The lowest enhancement of anthropogenic aerosol species was observed at HR during dust events (nssSO42-/nssCa2+ ˜ 0.13). These species were particularly enhanced when mineral dust arrived at sites after passing through populated and industrialized urban areas.

Chemical composition and sources of organic aerosols over London from the ClearfLo 2012 campaigns

Science.gov (United States)

Finessi, Emanuela; Holmes, Rachel; Hopkins, James; Lee, James; Harrison, Roy; Hamilton, Jacqueline

2014-05-01

Air quality in urban areas represents a major public health issue with around one third of the European population concentrated in cities and numbers expected to increase at global scale, particularly in developing countries. Particulate matter (PM) represents a primary threat for human health as numerous studies have confirmed the association between increased levels of cardiovascular and respiratory diseases with the exposure to PM. Despite considerable efforts made in improving air quality and progressively stricter emissions regulations, the PM concentrations have not changed much over the past decades for reasons that remain unclear, and highlight that studies on PM source apportionment are required for the formulation of effective policy. We investigated the chemical composition of organic aerosol (OA) collected during two intensive field campaigns held in winter and summer 2012 in the frame of the project Clean air for London (http://www.clearflo.ac.uk/). PM samples were collected both at a city background site (North Kensington) and at a rural site 50 km southeast of London (Detling) with 8 to 24 hours sampling schedule and analysed using off-line methods. Thermal-optical analysis was used to quantify OC-EC components while a suite of soft ionization mass spectrometric techniques was deployed for detailed chemical characterization. Liquid chromatography mass Spectrometry (LC-MSn) was mostly used for the simultaneous detection and quantification of various tracers for both primary and secondary OA sources. Well-established markers for wood burning primary OA like levoglucosan and azelaic acid were quantified together with various classes of nitroaromatics including methyl-nitrocatechols that are potential tracers for wood burning secondary OA. In addition, oxidation products of biogenic VOCs such as isoprene and monoterpenes were also quantified for both seasons and sites. A non-negligible contribution from biogenic SOA to urban OA was found in summertime

Modelling the chemically aged and mixed aerosols over the eastern central Atlantic Ocean – potential impacts

Directory of Open Access Journals (Sweden)

M. Astitha

2010-07-01

Full Text Available Detailed information on the chemical and physical properties of aerosols is important for assessing their role in air quality and climate. This work explores the origin and fate of continental aerosols transported over the Central Atlantic Ocean, in terms of chemical composition, number and size distribution, using chemistry-transport models, satellite data and in situ measurements. We focus on August 2005, a period with intense hurricane and tropical storm activity over the Atlantic Ocean. A mixture of anthropogenic (sulphates, nitrates, natural (desert dust, sea salt and chemically aged (sulphate and nitrate on dust aerosols is found entering the hurricane genesis region, most likely interacting with clouds in the area. Results from our modelling study suggest rather small amounts of accumulation mode desert dust, sea salt and chemically aged dust aerosols in this Atlantic Ocean region. Aerosols of smaller size (Aitken mode are more abundant in the area and in some occasions sulphates of anthropogenic origin and desert dust are of the same magnitude in terms of number concentrations. Typical aerosol number concentrations are derived for the vertical layers near shallow cloud formation regimes, indicating that the aerosol number concentration can reach several thousand particles per cubic centimetre. The vertical distribution of the aerosols shows that the desert dust particles are often transported near the top of the marine cloud layer as they enter into the region where deep convection is initiated. The anthropogenic sulphate aerosol can be transported within a thick layer and enter the cloud deck through multiple ways (from the top, the base of the cloud, and by entrainment. The sodium (sea salt related aerosol is mostly found below the cloud base. The results of this work may provide insights relevant for studies that consider aerosol influences on cloud processes and storm development in the Central Atlantic region.

Hygroscopicity and chemical composition of Antarctic sub-micrometre aerosol particles and observations of new particle formation

Directory of Open Access Journals (Sweden)

E. Asmi

2010-05-01

Full Text Available The Antarctic near-coastal sub-micrometre aerosol particle features in summer were characterised based on measured data on aerosol hygroscopicity, size distributions, volatility and chemical ion and organic carbon mass concentrations. Hysplit model was used to calculate the history of the air masses to predict the particle origin. Additional measurements of meteorological parameters were utilised. The hygroscopic properties of particles mostly resembled those of marine aerosols. The measurements took place at 130 km from the Southern Ocean, which was the most significant factor affecting the particle properties. This is explained by the lack of additional sources on the continent of Antarctica. The Southern Ocean was thus a likely source of the particles and nucleating and condensing vapours. The particles were very hygroscopic (HGF 1.75 at 90 nm and very volatile. Most of the sub-100 nm particle volume volatilised below 100 °C. Based on chemical data, particle hygroscopic and volatile properties were explained by a large fraction of non-neutralised sulphuric acid together with organic material. The hygroscopic growth factors assessed from chemical data were similar to measured. Hygroscopicity was higher in dry continental air masses compared with the moist marine air masses. This was explained by the aging of the marine organic species and lower methanesulphonic acid volume fraction together with the changes in the inorganic aerosol chemistry as the aerosol had travelled long time over the continental Antarctica. Special focus was directed in detailed examination of the observed new particle formation events. Indications of the preference of negative over positive ions in nucleation could be detected. However, in a detailed case study, the neutral particles dominated the particle formation process. Freshly nucleated particles had the smallest hygroscopic growth factors, which increased subsequent to particle aging.

Predicting the Mineral Composition of Dust Aerosols. Part 1; Representing Key Processes

Science.gov (United States)

Perlwitz, J. P.; Garcia-Pando, C. Perez; Miller, R. L.

2015-01-01

Soil dust aerosols created by wind erosion are typically assigned globally uniform physical and chemical properties within Earth system models, despite known regional variations in the mineral content of the parent soil. Mineral composition of the aerosol particles is important to their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, heterogeneous formation of sulfates and nitrates, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Here, aerosol mineral composition is derived by extending a method that provides the composition of a wet-sieved soil. The extension accounts for measurements showing significant differences between the mineral fractions of the wetsieved soil and the emitted aerosol concentration. For example, some phyllosilicate aerosols are more prevalent at silt sizes, even though they are nearly absent at these diameters in a soil whose aggregates are dispersed by wet sieving. We calculate the emitted mass of each mineral with respect to size by accounting for the disintegration of soil aggregates during wet sieving. These aggregates are emitted during mobilization and fragmentation of the original undispersed soil that is subject to wind erosion. The emitted aggregates are carried far downwind from their parent soil. The soil mineral fractions used to calculate the aggregates also include larger particles that are suspended only in the vicinity of the source. We calculate the emitted size distribution of these particles using a normalized distribution derived from aerosol measurements. In addition, a method is proposed for mixing minerals with small impurities composed of iron oxides. These mixtures are important for transporting iron far from the dust source, because pure iron oxides are more dense and vulnerable to gravitational removal than most minerals comprising dust aerosols. A limited comparison to

Levels, chemical composition and sources of fine aerosol particles (PM1) in an area of the Mediterranean basin

International Nuclear Information System (INIS)

Caggiano, Rosa; Macchiato, Maria; Trippetta, Serena

2010-01-01

Daily samples of fine aerosol particles (i.e., PM1, aerosol particles with an aerodynamic diameter less than 1.0 μm) were collected in Tito Scalo - Southern Italy - from April 2006 to March 2007. Measurements were performed by means of a low-volume gravimetric sampler, and each PM1 sample was analyzed by means of Inductively Coupled Plasma Optical Emission Spectrometry (ICP-OES) or Atomic Absorption Spectrometry (GFAAS and FAAS) techniques in order to determine its content in fourteen trace elements (Al, Ca, Cd, Cr, Cu, Fe, K, Mg, Mn, Na, Ni, Pb, Ti and Zn). During the period examined, PM1 daily concentrations ranged between 0.3 μg m -3 and 55 μg m -3 with a mean value of 8 μg m -3 , a standard deviation of 7 μg m -3 and a median value of 6 μg m -3 . As far as PM1 chemical composition is concerned, the mean values of the trace element concentrations decreased in the following order: Ca > Fe > Al > Na > K > Cr > Mg > Pb > Ni ∼ Ti ∼ Zn > Cd ∼ Cu > Mn. Principal Component Analysis (PCA) allowed the identification of three probable PM1 sources: industrial emissions, traffic and re-suspension of soil dust. Moreover, the results of a procedure applied to study the potential long-range transport contribution to PM1 chemical composition, showed that trace element concentrations do not seem to be affected by air mass origin and path. This was probably due to the strong impact of the local emission sources and the lack of the concentration measurements of some important elements and compounds that could better reveal the long-range transport influence on PM1 measurements at ground level.

Levels, chemical composition and sources of fine aerosol particles (PM1) in an area of the Mediterranean basin.

Science.gov (United States)

Caggiano, Rosa; Macchiato, Maria; Trippetta, Serena

2010-01-15

Daily samples of fine aerosol particles (i.e., PM1, aerosol particles with an aerodynamic diameter less than 1.0mum) were collected in Tito Scalo - Southern Italy - from April 2006 to March 2007. Measurements were performed by means of a low-volume gravimetric sampler, and each PM1 sample was analyzed by means of Inductively Coupled Plasma Optical Emission Spectrometry (ICP-OES) or Atomic Absorption Spectrometry (GFAAS and FAAS) techniques in order to determine its content in fourteen trace elements (Al, Ca, Cd, Cr, Cu, Fe, K, Mg, Mn, Na, Ni, Pb, Ti and Zn). During the period examined, PM1 daily concentrations ranged between 0.3microgm(-3) and 55microgm(-3) with a mean value of 8 microg m(-3), a standard deviation of 7microgm(-3) and a median value of 6microgm(-3). As far as PM1 chemical composition is concerned, the mean values of the trace element concentrations decreased in the following order: Ca>Fe>Al>Na>K>Cr>Mg>Pb>Ni approximately Ti approximately Zn>Cd approximately Cu>Mn. Principal Component Analysis (PCA) allowed the identification of three probable PM1 sources: industrial emissions, traffic and re-suspension of soil dust. Moreover, the results of a procedure applied to study the potential long-range transport contribution to PM1 chemical composition, showed that trace element concentrations do not seem to be affected by air mass origin and path. This was probably due to the strong impact of the local emission sources and the lack of the concentration measurements of some important elements and compounds that could better reveal the long-range transport influence on PM1 measurements at ground level. Copyright 2009 Elsevier B.V. All rights reserved.

Chemical composition of cigarette smoke

Energy Technology Data Exchange (ETDEWEB)

Guerin, M. R.

1979-01-01

Cigarette smoke is a concentrated aerosol of liquid particles suspended in an atmosphere consisting mainly of nitrogen, oxygen, and carbon dioxide. While the precise chemical composition of the particulate and gaseous phases is dependent on the characteristics of the cigarette and the manner in which it is smoked, both phases contain tens of hundreds of individual constitutents. Notable among potentially hazardous constituents of smoke are tar, nicotine, carbon monoxide, nitric oxide, hydrogen cyanide, acrolein, benzo(a)pyrene, and N-nitrosamines.

Persistence of urban organic aerosols composition: Decoding their structural complexity and seasonal variability

International Nuclear Information System (INIS)

Matos, João T.V.; Duarte, Regina M.B.O.; Lopes, Sónia P.; Silva, Artur M.S.; Duarte, Armando C.

2017-01-01

Organic Aerosols (OAs) are typically defined as highly complex matrices whose composition changes in time and space. Focusing on time vector, this work uses two-dimensional nuclear magnetic resonance (2D NMR) techniques to examine the structural features of water-soluble (WSOM) and alkaline-soluble organic matter (ASOM) sequentially extracted from fine atmospheric aerosols collected in an urban setting during cold and warm seasons. This study reveals molecular signatures not previously decoded in NMR-related studies of OAs as meaningful source markers. Although the ASOM is less hydrophilic and structurally diverse than its WSOM counterpart, both fractions feature a core with heteroatom-rich branched aliphatics from both primary (natural and anthropogenic) and secondary origin, aromatic secondary organics originated from anthropogenic aromatic precursors, as well as primary saccharides and amino sugar derivatives from biogenic emissions. These common structures represent those 2D NMR spectral signatures that are present in both seasons and can thus be seen as an “annual background” profile of the structural composition of OAs at the urban location. Lignin-derived structures, nitroaromatics, disaccharides, and anhydrosaccharides signatures were also identified in the WSOM samples only from periods identified as smoke impacted, which reflects the influence of biomass-burning sources. The NMR dataset on the H–C molecules backbone was also used to propose a semi-quantitative structural model of urban WSOM, which will aid efforts for more realistic studies relating the chemical properties of OAs with their atmospheric behavior. - Highlights: • 2D NMR spectroscopy was used to decode urban organic aerosols. • Water and alkaline soluble components of urban organic aerosols have been compared. • Persistence of urban organic aerosols composition across different seasons. • Annual background profile of the structural features of urban organic aerosols. • Semi

Mass and chemically speciated size distribution of Prague aerosol using an aerosol dryer - The influence of air mass origin

Czech Academy of Sciences Publication Activity Database

Schwarz, Jaroslav; Štefancová, Lucia; Maenhaut, W.; Smolík, Jiří; Ždímal, Vladimír

2012-01-01

Roč. 437, OCT 15 (2012), s. 348-362 ISSN 0048-9697 R&D Projects: GA ČR GA205/09/2055; GA ČR GAP209/11/1342; GA MŠk ME 941 Grant - others:SRF GU(BE) 01S01306 Institutional support: RVO:67985858 Keywords : atmospheric aerosols * mass size distribution * chemical composition Subject RIV: DI - Air Pollution ; Quality Impact factor: 3.258, year: 2012

Aerosol sampler for analysis of fine and ultrafine aerosols

Czech Academy of Sciences Publication Activity Database

Mikuška, Pavel; Čapka, Lukáš; Večeřa, Zbyněk

2018-01-01

Roč. 1020 (2018), s. 123-133 ISSN 0003-2670 R&D Projects: GA ČR(CZ) GA14-25558S Institutional support: RVO:68081715 Keywords : atmospheric aerosols * aerosol collection * chemical composition Subject RIV: CB - Analytical Chemistry, Separation OBOR OECD: Analytical chemistry Impact factor: 4.950, year: 2016

Aerosol composition and sources during the Chinese Spring Festival: fireworks, secondary aerosol, and holiday effects

Science.gov (United States)

Jiang, Q.; Sun, Y. L.; Wang, Z.; Yin, Y.

2015-06-01

Aerosol particles were characterized by an Aerodyne aerosol chemical speciation monitor along with various collocated instruments in Beijing, China, to investigate the role of fireworks (FW) and secondary aerosol in particulate pollution during the Chinese Spring Festival of 2013. Three FW events, exerting significant and short-term impacts on fine particles (PM2.5), were observed on the days of Lunar New Year, Lunar Fifth Day, and Lantern Festival. The FW were shown to have a large impact on non-refractory potassium, chloride, sulfate, and organics in submicron aerosol (PM1), of which FW organics appeared to be emitted mainly in secondary, with its mass spectrum resembling that of secondary organic aerosol (SOA). Pollution events (PEs) and clean periods (CPs) alternated routinely throughout the study. Secondary particulate matter (SPM = SOA + sulfate + nitrate + ammonium) dominated the total PM1 mass on average, accounting for 63-82% during nine PEs in this study. The elevated contributions of secondary species during PEs resulted in a higher mass extinction efficiency of PM1 (6.4 m2 g-1) than during CPs (4.4 m2 g-1). The Chinese Spring Festival also provides a unique opportunity to study the impact of reduced anthropogenic emissions on aerosol chemistry in the city. Primary species showed ubiquitous reductions during the holiday period with the largest reduction being in cooking organic aerosol (OA; 69%), in nitrogen monoxide (54%), and in coal combustion OA (28%). Secondary sulfate, however, remained only slightly changed, and the SOA and the total PM2.5 even slightly increased. Our results have significant implications for controlling local primary source emissions during PEs, e.g., cooking and traffic activities. Controlling these factors might have a limited effect on improving air quality in the megacity of Beijing, due to the dominance of SPM from regional transport in aerosol particle composition.

Glassy aerosols with a range of compositions nucleate ice heterogeneously at cirrus temperatures

Directory of Open Access Journals (Sweden)

T. W. Wilson

2012-09-01

Full Text Available Atmospheric secondary organic aerosol (SOA is likely to exist in a semi-solid or glassy state, particularly at low temperatures and humidities. Previously, it has been shown that glassy aqueous citric acid aerosol is able to nucleate ice heterogeneously under conditions relevant to cirrus in the tropical tropopause layer (TTL. In this study we test if glassy aerosol distributions with a range of chemical compositions heterogeneously nucleate ice under cirrus conditions. Three single component aqueous solution aerosols (raffinose, 4-hydroxy-3-methoxy-DL-mandelic acid (HMMA and levoglucosan and one multi component aqueous solution aerosol (raffinose mixed with five dicarboxylic acids and ammonium sulphate were studied in both the liquid and glassy states at a large cloud simulation chamber. The investigated organic compounds have similar functionality to oxidised organic material found in atmospheric aerosol and have estimated temperature/humidity induced glass transition thresholds that fall within the range predicted for atmospheric SOA. A small fraction of aerosol particles of all compositions were found to nucleate ice heterogeneously in the deposition mode at temperatures relevant to the TTL (<200 K. Raffinose and HMMA, which form glasses at higher temperatures, nucleated ice heterogeneously at temperatures as high as 214.6 and 218.5 K respectively. We present the calculated ice active surface site density, n_s, of the aerosols tested here and also of glassy citric acid aerosol as a function of relative humidity with respect to ice (RH_i. We also propose a parameterisation which can be used to estimate heterogeneous ice nucleation by glassy aerosol for use in cirrus cloud models up to ~220 K. Finally, we show that heterogeneous nucleation by glassy aerosol may compete with ice nucleation on mineral dust particles in mid-latitudes cirrus.

X-ray methods for the chemical characterization of atmospheric aerosols

International Nuclear Information System (INIS)

Jaklevic, J.M.; Thompson, A.C.

1981-05-01

The development and use of several x-ray methods for the chemical characterization of atmospherical aerosol particulate samples are described. These methods are based on the emission, absorption, and scattering of x-ray photons with emphasis on the optimization for the non-destructive analysis of dilute specimens. Techniques discussed include photon induced energy dispersive x-ray fluorescence, extended x-ray absorption fine structure spectroscopy using synchrotron radiation and high-rate x-ray powder diffractometry using a position-sensitive gas proportional counter. These x-ray analysis methods were applied to the measurement of the chemical compositions of size-segregated aerosol particulate samples obtained with dichotomous samplers. The advantages of the various methods for use in such measurements are described and results are presented. In many cases, the complementary nature of the analytical information obtained from the various measurements is an important factor in the characterization of the sample. For example, the multiple elemental analyses obtained from x-ray fluorescence can be used as a cross check on the major compounds observed by powder diffraction

Chemical composition, sources and secondary processes of aerosols in Baoji city of northwest China

Science.gov (United States)

Wang, Y. C.; Huang, R.-J.; Ni, H. Y.; Chen, Y.; Wang, Q. Y.; Li, G. H.; Tie, X. X.; Shen, Z. X.; Huang, Y.; Liu, S. X.; Dong, W. M.; Xue, P.; Fröhlich, R.; Canonaco, F.; Elser, M.; Daellenbach, K. R.; Bozzetti, C.; El Haddad, I.; Prévôt, A. S. H.; Canagaratna, M. R.; Worsnop, D. R.; Cao, J. J.

2017-06-01

Particulate air pollution is a severe environmental problem in China, affecting visibility, air quality, climate and human health. However, previous studies focus mainly on large cities such as Beijing, Shanghai, and Guangzhou. In this study, an Aerodyne Aerosol Chemical Speciation Monitor was deployed in Baoji, a middle size inland city in northwest China from 26 February to 27 March 2014. The non-refractory submicron aerosol (NR-PM1) was dominated by organics (55%), followed by sulfate (16%), nitrate (15%), ammonium (11%) and chloride (3%). A source apportionment of the organic aerosol (OA) was performed with the Sofi (Source Finder) interface of ME-2 (Multilinear Engine), and six main sources/factors were identified and classified as hydrocarbon-like OA (HOA), cooking OA (COA), biomass burning OA (BBOA), coal combustion OA (CCOA), less oxidized oxygenated OA (LO-OOA) and more oxidized oxygenated OA (MO-OOA), which contributed 20%, 14%, 13%, 9%, 23% and 21% of total OA, respectively. The contribution of secondary components shows increasing trends from clean days to polluted days, indicating the importance of secondary aerosol formation processes in driving particulate air pollution. The formation of LO-OOA and MO-OOA is mainly driven by photochemical reactions, but significantly influenced by aqueous-phase chemistry during periods of low atmospheric oxidative capacity.

A size-composition resolved aerosol model for simulating the dynamics of externally mixed particles: SCRAM (v 1.0)

Science.gov (United States)

Zhu, S.; Sartelet, K. N.; Seigneur, C.

2015-06-01

The Size-Composition Resolved Aerosol Model (SCRAM) for simulating the dynamics of externally mixed atmospheric particles is presented. This new model classifies aerosols by both composition and size, based on a comprehensive combination of all chemical species and their mass-fraction sections. All three main processes involved in aerosol dynamics (coagulation, condensation/evaporation and nucleation) are included. The model is first validated by comparison with a reference solution and with results of simulations using internally mixed particles. The degree of mixing of particles is investigated in a box model simulation using data representative of air pollution in Greater Paris. The relative influence on the mixing state of the different aerosol processes (condensation/evaporation, coagulation) and of the algorithm used to model condensation/evaporation (bulk equilibrium, dynamic) is studied.

Physico-Chemical Evolution of Organic Aerosol from Wildfire Emissions

Science.gov (United States)

Croteau, P.; Jathar, S.; Akherati, A.; Galang, A.; Tarun, S.; Onasch, T. B.; Lewane, L.; Herndon, S. C.; Roscioli, J. R.; Yacovitch, T. I.; Fortner, E.; Xu, W.; Daube, C.; Knighton, W. B.; Werden, B.; Wood, E.

2017-12-01

Wildfires are the largest combustion-related source of carbonaceous emissions to the atmosphere; these include direct emissions of black carbon (BC), primary organic aerosol (POA) and semi-volatile, intermediate-volatility, and volatile organic compounds (SVOCs, IVOCs, and VOCs). However, there are large uncertainties surrounding the evolution of these carbonaceous emissions as they are physically and chemically transformed in the atmosphere. To understand these transformations, we performed sixteen experiments using an environmental chamber to simulate day- and night-time chemistry of gas- and aerosol-phase emissions from 6 different fuels at the Fire Laboratory in Missoula, MT. Across the test matrix, the experiments simulated 2 to 8 hours of equivalent day-time aging (with the hydroxyl radical and ozone) or several hours of night-time aging (with the nitrate radical). Aging resulted in an average organic aerosol (OA) mass enhancement of 28% although the full range of OA mass enhancements varied between -10% and 254%. These enhancement findings were consistent with chamber and flow reactor experiments performed at the Fire Laboratory in 2010 and 2012 but, similar to previous studies, offered no evidence to link the OA mass enhancement to fuel type or oxidant exposure. Experiments simulating night-time aging resulted in an average OA mass enhancement of 10% and subsequent day-time aging resulted in a decrease in OA mass of 8%. While small, for the first time, these experiments highlighted the continuous nature of the OA evolution as the wildfire smoke cycled through night- and day-time processes. Ongoing work is focussed on (i) quantifying bulk compositional changes in OA, (ii) comparing the near-field aging simulated in this work with far-field aging simulated during the same campaign (via a mini chamber and flow tube) and (iii) integrating wildfire smoke aging datasets over the past decade to examine the relationship between OA mass enhancement ratios, modified

Aerosol simulation including chemical and nuclear reactions

International Nuclear Information System (INIS)

Marwil, E.S.; Lemmon, E.C.

1985-01-01

The numerical simulation of aerosol transport, including the effects of chemical and nuclear reactions presents a challenging dynamic accounting problem. Particles of different sizes agglomerate and settle out due to various mechanisms, such as diffusion, diffusiophoresis, thermophoresis, gravitational settling, turbulent acceleration, and centrifugal acceleration. Particles also change size, due to the condensation and evaporation of materials on the particle. Heterogeneous chemical reactions occur at the interface between a particle and the suspending medium, or a surface and the gas in the aerosol. Homogeneous chemical reactions occur within the aersol suspending medium, within a particle, and on a surface. These reactions may include a phase change. Nuclear reactions occur in all locations. These spontaneous transmutations from one element form to another occur at greatly varying rates and may result in phase or chemical changes which complicate the accounting process. This paper presents an approach for inclusion of these effects on the transport of aerosols. The accounting system is very complex and results in a large set of stiff ordinary differential equations (ODEs). The techniques for numerical solution of these ODEs require special attention to achieve their solution in an efficient and affordable manner. 4 refs

Aerosol composition from Tlaxcoapan, Hidalgo in central Mexico

International Nuclear Information System (INIS)

Martinez C, M. A.; Solis, C.; Andrade, E.; Issac O, K.; Beltran H, R. I.; Medina M, S. A.; Martinez R, G.; Ramirez R, A.; Lucho C, C. A.; Del Razo, L. M.

2010-01-01

Air quality mexican regulations about atmospheric aerosols refer to particle sizes and to the total suspended particle. None of these norms establishes the allowed values based on the particulate chemical composition. Mexican environmental legislation also considers as critical zones those with high concentration of contaminants in the atmosphere. One of these zones is the Tula-Vito-Apasco corridor where no chemical composition characterization in terms of trace metal associated to the air particulate matter has been made. Along this corridor near Tlaxcoapan there are important contaminant sources as petrochemical and electric power plants, metal-mechanical industry, limestone quarry and contaminated soils. In this work PIXE and Sem-EDS were applied to the PM 10 fraction collected on filters. The trace element values thus determined were compared with those of a similar critical zone. It was found that most of the coarse particles come from limestone quarry as fugitive dusts while V, Ni, Cr and Pb values are moderately high and seems to be associated to industrial activities and contaminated soil as well. (Author)

Aerosol composition from Tlaxcoapan, Hidalgo in central Mexico

Energy Technology Data Exchange (ETDEWEB)

Martinez C, M. A.; Solis, C.; Andrade, E. [UNAM, Instituto de Fisica, Circuito Exterior, Ciudad Universitaria, 04510 Mexico D. F. (Mexico); Issac O, K. [Universidad Autonoma del Estado de Mexico, Facultad de Medicina, Paseo Tollocan y Jesus Carranza s/n, 50120 Toluca, Estado de Mexico (Mexico); Beltran H, R. I. [Universidad Autonoma del Estado de Hidalgo, Centro de Investigaciones Quimicas, Carretera Pachuca-Tulancingo Km. 4.5, 42174 Pachuca, Hidalgo (Mexico); Medina M, S. A.; Martinez R, G.; Ramirez R, A.; Lucho C, C. A. [Universidad Politecnica de Pachuca, Programa de Ingenieria en Biotecnologia, Carretera Pachuca-Cd. Sahagun Km. 20, Ex-Hacienda de Santa Barbara, Municipio de Zempoala, Hidalgo (Mexico); Del Razo, L. M. [IPN, Centro de Investigacion y de Estudios Avanzados, Seccion Externa de Toxicologia, Ticoman, 07360 Mexico D. F. (Mexico)

2010-02-15

Air quality mexican regulations about atmospheric aerosols refer to particle sizes and to the total suspended particle. None of these norms establishes the allowed values based on the particulate chemical composition. Mexican environmental legislation also considers as critical zones those with high concentration of contaminants in the atmosphere. One of these zones is the Tula-Vito-Apasco corridor where no chemical composition characterization in terms of trace metal associated to the air particulate matter has been made. Along this corridor near Tlaxcoapan there are important contaminant sources as petrochemical and electric power plants, metal-mechanical industry, limestone quarry and contaminated soils. In this work PIXE and Sem-EDS were applied to the PM{sub 10} fraction collected on filters. The trace element values thus determined were compared with those of a similar critical zone. It was found that most of the coarse particles come from limestone quarry as fugitive dusts while V, Ni, Cr and Pb values are moderately high and seems to be associated to industrial activities and contaminated soil as well. (Author)

Single particle measurements of the chemical composition of cirrus ice residue during CRYSTAL-FACE

Science.gov (United States)

Cziczo, D. J.; Murphy, D. M.; Hudson, P. K.; Thomson, D. S.

2004-02-01

The first real-time, in situ, investigation of the chemical composition of the residue of cirrus ice crystals was performed during July 2002. This study was undertaken on a NASA WB-57F high-altitude research aircraft as part of CRYSTAL-FACE, a field campaign which sought to further our understanding of the relation of clouds, water vapor, and climate by characterizing, among other parameters, anvil cirrus formed about the Florida peninsula. A counter flow virtual impactor (CVI) was used to separate cirrus ice from the unactivated interstitial aerosol particles and evaporate condensed-phase water. Residual material, on a crystal-by-crystal basis, was subsequently analyzed using the NOAA Aeronomy Laboratory's Particle Analysis by Laser Mass Spectrometry (PALMS) instrument. Sampling was performed from 5 to 15 km altitude and from 12° to 28° north latitude within cirrus originating over land and ocean. Chemical composition measurements provided several important results. Sea salt was often incorporated into cirrus, consistent with homogeneous ice formation by aerosol particles from the marine boundary layer. Size measurements showed that large particles preferentially froze over smaller ones. Meteoritic material was found within ice crystals, indicative of a relation between stratospheric aerosol particles and tropospheric clouds. Mineral dust was the dominant residue observed in clouds formed during a dust transport event from the Sahara, consistent with a heterogeneous freezing mechanism. These results show that chemical composition and size are important determinants of which aerosol particles form cirrus ice crystals.

Broadband optical properties of biomass-burning aerosol and identification of brown carbon chromophores: OPTICAL AND CHEMICAL PROPERTIES OF BROWN CARBON AEROSOLS

Energy Technology Data Exchange (ETDEWEB)

Bluvshtein, Nir [Department of Earth and Planetary Sciences, Weizmann Institute of Science, Rehovot Israel; Lin, Peng [Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland Washington USA; Flores, J. Michel [Department of Earth and Planetary Sciences, Weizmann Institute of Science, Rehovot Israel; Segev, Lior [Department of Earth and Planetary Sciences, Weizmann Institute of Science, Rehovot Israel; Mazar, Yinon [Department of Earth and Planetary Sciences, Weizmann Institute of Science, Rehovot Israel; Tas, Eran [The Robert H. Smith Faculty of Agriculture, Food and Environment, The Hebrew University of Jerusalem, Rehovot Israel; Snider, Graydon [Department of Physics and Atmospheric Science, Dalhousie University, Halifax Nova Scotia Canada; Weagle, Crystal [Department of Chemistry, Dalhousie University, Halifax Nova Scotia Canada; Brown, Steven S. [Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder Colorado USA; Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder Colorado USA; Laskin, Alexander [Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland Washington USA; Rudich, Yinon [Department of Earth and Planetary Sciences, Weizmann Institute of Science, Rehovot Israel

2017-05-23

The radiative effects of biomass burning aerosols on regional and global scale is substantial. Accurate modeling of the radiative effects of smoke aerosols require wavelength-dependent measurements and parameterizations of their optical properties in the UV and visible spectral ranges along with improved description of their chemical composition. To address this issue, we used a recently developed approach to retrieve the time- and spectral-dependent optical properties of ambient biomass burning aerosols between 300 and 650 nm wavelength during a regional bonfire festival in Israel. During the biomass burning event, the overall absorption at 400 nm increased by about two orders of magnitude, changing the size-weighted single scattering albedo from a background level of 0.95 to 0.7. Based on the new retrieval method, we provide parameterizations of the wavelength-dependent effective complex refractive index from 350 to 650 nm for freshly emitted and aged biomass burning aerosols. In addition, PM2.5 filter samples were collected for detailed off-line chemical analysis of the water soluble organics that contribute to light absorption. Nitrophenols were identified as the main organic species responsible for the increased absorption at 400-500 nm. These include species such as 4- nitrocatechol, 4-nitrophenol, nitro-syringol and nitro-guaiacol; oxidation-nitration products of methoxyphenols, known products of lignin pyrolysis. Our findings emphasize the importance of both primary and secondary organic aerosol from biomass burning in absorption of solar radiation and in effective radiative forcing.

Chemical apportionment of aerosol optical properties during the Asia-Pacific Economic Cooperation summit in Beijing, China

Science.gov (United States)

Han, Tingting; Xu, Weiqi; Chen, Chen; Liu, Xingang; Wang, Qingqing; Li, Jie; Zhao, Xiujuan; Du, Wei; Wang, Zifa; Sun, Yele

2015-12-01

We have investigated the chemical and optical properties of aerosol particles during the 2014 Asia-Pacific Economic Cooperation (APEC) summit in Beijing, China, using the highly time-resolved measurements by a high-resolution aerosol mass spectrometer and a cavity attenuated phase shift extinction monitor. The average (±σ) extinction coefficient (bext) and absorption coefficient (bap) were 186.5 (±184.5) M m-1 and 23.3 (±21.9) M m-1 during APEC, which were decreased by 63% and 56%, respectively, compared to those before APEC primarily due to strict emission controls. The aerosol composition and size distributions showed substantial changes during APEC; as a response, the mass scattering efficiency (MSE) of PM1 was decreased from 4.7 m2 g-1 to 3.5 m2 g-1. Comparatively, the average single-scattering albedo (SSA) remained relatively unchanged, illustrating the synchronous reductions of bext and bap during APEC. MSE and SSA were found to increase as function of the oxidation degree of organic aerosol (OA), indicating a change of aerosol optical properties during the aging processes. The empirical relationships between chemical composition and particle extinction were established using a multiple linear regression model. Our results showed the largest contribution of ammonium nitrate to particle extinction, accounting for 35.1% and 29.3% before and during APEC, respectively. This result highlights the important role of ammonium nitrate in the formation of severe haze pollution during this study period. We also observed very different optical properties of primary and secondary aerosol. Owing to emission controls in Beijing and surrounding regions and also partly the influences of meteorological changes, the average bext of secondary aerosol during APEC was decreased by 71% from 372.3 M m-1 to 108.5 M m-1, whereas that of primary aerosol mainly from cooking, traffic, and biomass burning emissions showed a smaller reduction from 136.7 M m-1 to 71.3 M m-1. As a result

Chemical composition, sources, and aging process of submicron aerosols in Beijing: Contrast between summer and winter

Science.gov (United States)

Hu, Weiwei; Hu, Min; Hu, Wei; Jimenez, Jose L.; Yuan, Bin; Chen, Wentai; Wang, Ming; Wu, Yusheng; Chen, Chen; Wang, Zhibin; Peng, Jianfei; Zeng, Limin; Shao, Min

2016-02-01

To investigate the seasonal characteristics of submicron aerosol (PM1) in Beijing urban areas, a high-resolution time-of-flight aerosol-mass-spectrometer (HR-ToF-AMS) was utilized at an urban site in summer (August to September 2011) and winter (November to December 2010), coupled with multiple state of the art online instruments. The average mass concentrations of PM1 (60-84 µg m-3) and its chemical compositions in different campaigns of Beijing were relatively consistent in recent years. In summer, the daily variations of PM1 mass concentrations were stable and repeatable. Eighty-two percent of the PM1 mass concentration on average was composed of secondary species, where 62% is secondary inorganic aerosol and 20% secondary organic aerosol (SOA). In winter, PM1 mass concentrations changed dramatically because of the different meteorological conditions. The high average fraction (58%) of primary species in PM1 including primary organic aerosol (POA), black carbon, and chloride indicates primary emissions usually played a more important role in the winter. However, aqueous chemistry resulting in efficient secondary formation during occasional periods with high relative humidity may also contribute substantially to haze in winter. Results of past OA source apportionment studies in Beijing show 45-67% of OA in summer and 22-50% of OA in winter can be composed of SOA. Based on the source apportionment results, we found 45% POA in winter and 61% POA in summer are from nonfossil sources, contributed by cooking OA in both seasons and biomass burning OA (BBOA) in winter. Cooking OA, accounting for 13-24% of OA, is an important nonfossil carbon source in all years of Beijing and should not be neglected. The fossil sources of POA include hydrocarbon-like OA from vehicle emissions in both seasons and coal combustion OA (CCOA) in winter. The CCOA and BBOA were the two main contributors (57% of OA) for the highest OA concentrations (>100 µg m-3) in winter. The POA

Wintertime aerosol chemical composition, volatility, and spatial variability in the greater London area

Directory of Open Access Journals (Sweden)

L. Xu

2016-02-01

Full Text Available The composition of PM1 (particulate matter with diameter less than 1 µm in the greater London area was characterized during the Clean Air for London (ClearfLo project in winter 2012. Two high-resolution time-of-flight aerosol mass spectrometers (HR-ToF-AMS were deployed at a rural site (Detling, Kent and an urban site (North Kensington, London. The simultaneous and high-temporal resolution measurements at the two sites provide a unique opportunity to investigate the spatial distribution of PM1. We find that the organic aerosol (OA concentration is comparable between the rural and urban sites, but the contribution from different sources is distinctly different between the two sites. The concentration of solid fuel OA at the urban site is about twice as high as at the rural site, due to elevated domestic heating in the urban area. While the concentrations of oxygenated OA (OOA are well-correlated between the two sites, the OOA concentration at the rural site is almost twice that of the urban site. At the rural site, more than 70 % of the carbon in OOA is estimated to be non-fossil, which suggests that OOA is likely related to aged biomass burning considering the small amount of biogenic SOA in winter. Thus, it is possible that the biomass burning OA contributes a larger fraction of ambient OA in wintertime than what previous field studies have suggested. A suite of instruments was deployed downstream of a thermal denuder (TD to investigate the volatility of PM1 species at the rural Detling site. After heating at 250 °C in the TD, 40 % of the residual mass is OA, indicating the presence of non-volatile organics in the aerosol. Although the OA associated with refractory black carbon (rBC; measured by a soot-particle aerosol mass spectrometer only accounts for < 10 % of the total OA (measured by a HR-ToF-AMS at 250 °C, the two measurements are well-correlated, suggesting that the non-volatile organics have similar sources or have

Field characterization of the PM2.5 Aerosol Chemical Speciation Monitor: insights into the composition, sources, and processes of fine particles in eastern China

Science.gov (United States)

Zhang, Yunjiang; Tang, Lili; Croteau, Philip L.; Favez, Olivier; Sun, Yele; Canagaratna, Manjula R.; Wang, Zhuang; Couvidat, Florian; Albinet, Alexandre; Zhang, Hongliang; Sciare, Jean; Prévôt, André S. H.; Jayne, John T.; Worsnop, Douglas R.

2017-12-01

A PM2.5-capable aerosol chemical speciation monitor (Q-ACSM) was deployed in urban Nanjing, China, for the first time to measure in situ non-refractory fine particle (NR-PM2.5) composition from 20 October to 19 November 2015, along with parallel measurements of submicron aerosol (PM1) species by a standard Q-ACSM. Our results show that the NR-PM2.5 species (organics, sulfate, nitrate, and ammonium) measured by the PM2.5-Q-ACSM are highly correlated (r2 > 0.9) with those measured by a Sunset Lab OC  /  EC analyzer and a Monitor for AeRosols and GAses (MARGA). The comparisons between the two Q-ACSMs illustrated similar temporal variations in all NR species between PM1 and PM2.5, yet substantial mass fractions of aerosol species were observed in the size range of 1-2.5 µm. On average, NR-PM1-2.5 contributed 53 % of the total NR-PM2.5, with sulfate and secondary organic aerosols (SOAs) being the two largest contributors (26 and 27 %, respectively). Positive matrix factorization of organic aerosol showed similar temporal variations in both primary and secondary OAs between PM1 and PM2.5, although the mass spectra were slightly different due to more thermal decomposition on the capture vaporizer of the PM2.5-Q-ACSM. We observed an enhancement of SOA under high relative humidity conditions, which is associated with simultaneous increases in aerosol pH, gas-phase species (NO2, SO2, and NH3) concentrations and aerosol water content driven by secondary inorganic aerosols. These results likely indicate an enhanced reactive uptake of SOA precursors upon aqueous particles. Therefore, reducing anthropogenic NOx, SO2, and NH3 emissions might not only reduce secondary inorganic aerosols but also the SOA burden during haze episodes in China.

Chemical Thermodynamics of Aqueous Atmospheric Aerosols: Modeling and Microfluidic Measurements

Science.gov (United States)

Nandy, L.; Dutcher, C. S.

2017-12-01

Accurate predictions of gas-liquid-solid equilibrium phase partitioning of atmospheric aerosols by thermodynamic modeling and measurements is critical for determining particle composition and internal structure at conditions relevant to the atmosphere. Organic acids that originate from biomass burning, and direct biogenic emission make up a significant fraction of the organic mass in atmospheric aerosol particles. In addition, inorganic compounds like ammonium sulfate and sea salt also exist in atmospheric aerosols, that results in a mixture of single, double or triple charged ions, and non-dissociated and partially dissociated organic acids. Statistical mechanics based on a multilayer adsorption isotherm model can be applied to these complex aqueous environments for predictions of thermodynamic properties. In this work, thermodynamic analytic predictive models are developed for multicomponent aqueous solutions (consisting of partially dissociating organic and inorganic acids, fully dissociating symmetric and asymmetric electrolytes, and neutral organic compounds) over the entire relative humidity range, that represent a significant advancement towards a fully predictive model. The model is also developed at varied temperatures for electrolytes and organic compounds the data for which are available at different temperatures. In addition to the modeling approach, water loss of multicomponent aerosol particles is measured by microfluidic experiments to parameterize and validate the model. In the experimental microfluidic measurements, atmospheric aerosol droplet chemical mimics (organic acids and secondary organic aerosol (SOA) samples) are generated in microfluidic channels and stored and imaged in passive traps until dehydration to study the influence of relative humidity and water loss on phase behavior.

Microphysical and chemical characteristics of near-water aerosol over White and Kara Seas

Science.gov (United States)

Terpugova, S. A.; Polkin, V. V.; Panchenko, M. V.; Golobokova, L. P.; Kozlov, V. S.; Shmargunov, V. P.; Shevchenko, V. P.; Lisitzin, A. P.

2009-04-01

The results are presented of five-year-long (2003-2007) study of the spatial - temporal variability of the near-water aerosol in the water area of White and Kara Seas (55, 64, 71 and 80-th cruises of RV "Professor Shtockman"; 53 and 54-th cruises of RV "Akademik Mstislav Keldysh"). Measurements of aerosol microphysical characteristics were carried out by means of the automated mobile aerosol complex consisting of nephelometer, photoelectric counter and aethalometer. The aerosol disperse composition was studied with photoelectric counter in 256 size intervals from 0.4 to 10 m. About 1500 series of measurements were carried out in White Sea, and about 1400 series in Kara Sea. Chemical characteristics of aerosol were determined from samples collected on aerosol filters (92 samples were collected in White Sea and 48 in Kara Sea). The ion composition was determined under laboratory conditions. The H+, Na+, K+, Ca2+, Mg2+, NH4+, Cl-, NO3-, HCO3-, SO42- ions were under examination. Comparing aerosol characteristics of two seas, one can note that the mean values of the aerosol content parameters in Kara Sea are less than in White Sea. The ratio of the aerosol mass concentration are from 2 (Yamal Peninsula, northern part of Novaya Zemlya) to 9 times (Blagopoluchia Bay, Ob' Gulf). The differences in the concentration of black carbon vary from 3 (Yamal Peninsula) to 17 times (Blagopoluchia Bay). The differences in the aerosol number concentration NA are not so big. The values NA near Kara Gate, Yamal Peninsula and northern part of Novaya Zemlya are practically the same as in White Sea. The concentration NA at Ob' gulf is one order of magnitude less than in White sea. The obtained aerosol volume size distributions were approximated by the sums of two fractions, submicron and coarse, with lognormal size distributions. The mean volume size distribution of submicron fraction in White Sea is approximated by the distribution with the variance of the radius logarithm s=0.6 and modal

Quantifying the Relationship between Organic Aerosol Composition and Hygroscopicity/CCN Activity

Energy Technology Data Exchange (ETDEWEB)

Ziemann, Paul J. [Univ. of California, Riverside, CA (United States); Kreidenweis, Sonia M. [Colorado State Univ., Fort Collins, CO (United States); Petters, Markus D. [North Carolina State Univ., Raleigh, NC (United States)

2013-06-30

The overall objective for this project was to provide the data and underlying process level understanding necessary to facilitate the dynamic treatment of organic aerosol CCN activity in future climate models. The specific objectives were as follows: (1) employ novel approaches to link organic aerosol composition and CCN activity, (2) evaluate the effects of temperature and relative humidity on organic aerosol CCN activity, and (3) develop parameterizations to link organic aerosol composition and CCN activity.

Aerosol chemical and optical properties over the Paris area within ESQUIF project

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A. Hodzic

2006-01-01

Full Text Available Aerosol chemical and optical properties are extensively investigated for the first time over the Paris Basin in July 2000 within the ESQUIF project. The measurement campaign offers an exceptional framework to evaluate the performances of the chemistry-transport model CHIMERE in simulating concentrations of gaseous and aerosol pollutants, as well as the aerosol-size distribution and composition in polluted urban environments against ground-based and airborne measurements. A detailed comparison of measured and simulated variables during the second half of July with particular focus on 19 and 31 pollution episodes reveals an overall good agreement for gas-species and aerosol components both at the ground level and along flight trajectories, and the absence of systematic biases in simulated meteorological variables such as wind speed, relative humidity and boundary layer height as computed by the MM5 model. A good consistency in ozone and NO concentrations demonstrates the ability of the model to reproduce the plume structure and location fairly well both on 19 and 31 July, despite an underestimation of the amplitude of ozone concentrations on 31 July. The spatial and vertical aerosol distributions are also examined by comparing simulated and observed lidar vertical profiles along flight trajectories on 31 July and confirm the model capacity to simulate the plume characteristics. The comparison of observed and modeled aerosol components in the southwest suburb of Paris during the second half of July indicates that the aerosol composition is rather correctly reproduced, although the total aerosol mass is underestimated by about 20%. The simulated Parisian aerosol is dominated by primary particulate matter that accounts for anthropogenic and biogenic primary particles (40%, and inorganic aerosol fraction (40% including nitrate (8%, sulfate (22% and ammonium (10%. The secondary organic aerosols (SOA represent 12% of the total aerosol mass, while the

Online Chemical Characterization of Food-Cooking Organic Aerosols: Implications for Source Apportionment.

Science.gov (United States)

Reyes-Villegas, Ernesto; Bannan, Thomas; Le Breton, Michael; Mehra, Archit; Priestley, Michael; Percival, Carl; Coe, Hugh; Allan, James D

2018-04-11

Food-cooking organic aerosols (COA) are one of the primary sources of submicron particulate matter in urban environments. However, there are still many questions surrounding source apportionment related to instrumentation as well as semivolatile partitioning because COA evolve rapidly in the ambient air, making source apportionment more complex. Online measurements of emissions from cooking different types of food were performed in a laboratory to characterize particles and gases. Aerosol mass spectrometer (AMS) measurements showed that the relative ionization efficiency for OA was higher (1.56-3.06) relative to a typical value of 1.4, concluding that AMS is over-estimating COA and suggesting that previous studies likely over-estimated COA concentrations. Food-cooking mass spectra were generated using AMS, and gas and particle food markers were identified with filter inlets for gases and aerosols-chemical ionization mass spectrometer (CIMS) measurements to be used in future food cooking-source apportionment studies. However, there is a considerable variability in both gas and particle markers, and dilution plays an important role in the particle mass budget, showing the importance of using these markers with caution during receptor modeling. These findings can be used to better understand the chemical composition of COA, and they provides useful information to be used in future source-apportionment studies.

Size distributions and chemical properties of aerosol at Ny Ålesund, Svalbard

Science.gov (United States)

Covert, David S.; Heintzenberg, Jost

Physical and chemical parameters of the arctic aerosol were investigated at Ny Ålesund, Svalbard, in March and April 1989 in connection with the third Arctic Gas and Aerosol Project (AGASP III). The number size distribution of the particles was measured over the range of 0.02-1.0 μm. Filter samples were analysed for elemental composition and two integral chemical properties, hygroscopic growth and volatility, were measured. Along with the latter measurements, the distribution of these properties at specific particle sizes, i.e. the degree of internal mixing, was determined. Both clean, marine conditions and "arctic haze" episodes were included in the series of measurements. The number size distribution indicated that the aerosol was well aged based on its narrowness and the relative low concentration of nuclei mode particles. It had a number mode at 0.22 μm diameter and geometric standard deviation of 1.4. Generally the particles exhibited uniform hygroscopic growth properties, i.e. they were largely internally mixed. The growth factor was 1.45 at 90% relative humidity. Approximately 40% of the overall particulate mass was volatile at a temperature of 50°C. The volatile fraction varied form particle to particle, i.e. the particles were externally mixed with respect to volatility.

Atmospheric aerosol system: An overview

International Nuclear Information System (INIS)

Prospero, J.M.; Charlson, R.J.; Mohnen, V.; Jaenicke, R.; Delany, A.C.; Moyers, J.; Zoller, W.; Rahn, K.

1983-01-01

Aerosols could play a critical role in many processes which impact on our lives either indirectly (e.g., climate) or directly (e.g., health). However, our ability to assess these possible impacts is constrained by our limited knowledge of the physical and chemical properties of aerosols, both anthropogenic and natural. This deficiency is attributable in part to the fact that aerosols are the end product of a vast array of chemical and physical processes. Consequently, the properties of the aerosol can exhibit a great deal of variability in both time and space. Furthermore, most aerosol studies have focused on measurements of a single aerosol characteristic such as composition or size distribution. Such information is generally not useful for the assessment of impacts because the degree of impact may depend on the integral properties of the aerosol, for example, the aerosol composition as a function of particle size. In this overview we discuss recent work on atmospheric aerosols that illustrates the complex nature of the aerosol chemical and physical system, and we suggest strategies for future research. A major conclusion is that man has had a great impact on the global budgets of certain species, especially sulfur and nitrogen, that play a dominant role in the atmospheric aerosol system. These changes could conceivably affect climate. Large-scale impacts are implied because it has recently been demonstrated that natural and pollutant aerosol episodes can be propagated over great distances. However, at present there is no evidence linking anthropogenic activities with a persistent increase in aerosol concentrations on a global scale. A major problem in assessing man's impact on the atmospheric aerosol system and on global budgets is the absence of aerosol measurements in remote marine and continental areas

Organic molecular composition of marine aerosols over the Arctic Ocean in summer: contributions of primary emission and secondary aerosol formation

Directory of Open Access Journals (Sweden)

P. Q. Fu

2013-02-01

Full Text Available Organic molecular composition of marine aerosol samples collected during the MALINA cruise in the Arctic Ocean was investigated by gas chromatography/mass spectrometry. More than 110 individual organic compounds were determined in the samples and were grouped into different compound classes based on the functionality and sources. The concentrations of total quantified organics ranged from 7.3 to 185 ng m⁻³ (mean 47.6 ng m⁻³, accounting for 1.8–11.0% (4.8% of organic carbon in the marine aerosols. Primary saccharides were found to be dominant organic compound class, followed by secondary organic aerosol (SOA tracers formed from the oxidation of biogenic volatile organic compounds (VOCs such as isoprene, α-pinene and β-caryophyllene. Mannitol, the specific tracer for airborne fungal spores, was detected as the most abundant organic species in the samples with a concentration range of 0.052–53.3 ng m⁻³ (9.2 ng m⁻³, followed by glucose, arabitol, and the isoprene oxidation products of 2-methyltetrols. Biomass burning tracers such as levoglucosan are evident in all samples with trace levels. On the basis of the tracer-based method for the estimation of fungal-spore OC and biogenic secondary organic carbon (SOC, we estimate that an average of 10.7% (up to 26.2% of the OC in the marine aerosols was due to the contribution of fungal spores, followed by the contribution of isoprene SOC (mean 3.8% and α-pinene SOC (2.9%. In contrast, only 0.19% of the OC was due to the photooxidation of β-caryophyllene. This study indicates that primary organic aerosols from biogenic emissions, both from long-range transport of mid-latitude aerosols and from sea-to-air emission of marine organics, as well as secondary organic aerosols formed from the photooxidation of biogenic VOCs are important factors controlling the organic chemical composition of marine aerosols in the Arctic Ocean.

Chemical and microphysical properties of the aerosol during foggy and nonfoggy episodes: a relationship between organic and inorganic content of the aerosol

Science.gov (United States)

Kaul, D. S.; Gupta, T.; Tripathi, S. N.

2012-06-01

An extensive field measurement during winter was carried out at a site located in the Indo-Gangetic Plain (IGP) which gets heavily influenced by the fog during winter almost every year. The chemical and microphysical properties of the aerosols during foggy and nonfoggy episodes and chemical composition of the fogwater are presented. Positive matrix factorization (PMF) as a tool for the source apportionment was employed to understand the sources of pollution. Four major sources viz. biomass burning, refractory, secondary and mineral dust were identified. Aerosols properties during foggy episodes were heavily influenced by almost all the sources and they caused considerable loading of almost all the organic and inorganic species during the period. The biomass generated aerosols were removed from the atmosphere by scavenging during foggy episodes. The wet removal of almost all the species by the fog droplets was observed. The K+, water soluble organic carbon (WSOC), water soluble inorganic carbon (WSIC) and NO3- were most heavily scavenged among the species and their concentrations consequently became lower than the nonfoggy episode concentrations. The production of secondary inorganic aerosol, mainly sulfate and ammonium, during foggy episodes was considerably higher than nitrate which was rather heavily scavenged and removed by the fog droplets. The fogwater analysis showed that dissolved inorganic species play a vital role in processing of organic carbon such as the formation of organo-sulfate and organo-nitrate inside the fog droplets. The formation of organo-sulfate and organo-nitrate in aerosol and the influence of acidity on the secondary organic aerosol (SOA) formation were rather found to be negligible. The study average inorganic component of the aerosol was considerably higher than the carbonaceous component during both foggy and nonfoggy episode. The secondary production of the aerosol changed the microphysical properties of aerosol which was reflected by

Source identification and airborne chemical characterisation of aerosol pollution from long-range transport over Greenland during POLARCAT summer campaign 2008

Science.gov (United States)

Schmale, J.; Schneider, J.; Ancellet, G.; Quennehen, B.; Stohl, A.; Sodemann, H.; Burkhart, J. F.; Hamburger, T.; Arnold, S. R.; Schwarzenboeck, A.; Borrmann, S.; Law, K. S.

2011-10-01

We deployed an aerosol mass spectrometer during the POLARCAT (Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate, Chemistry, Aerosols, and Transport) summer campaign in Greenland in June/July 2008 on the research aircraft ATR-42. Online size resolved chemical composition data of submicron aerosol were collected up to 7.6 km altitude in the region 60 to 71° N and 40 to 60° W. Biomass burning (BB) and fossil fuel combustion (FF) plumes originating from North America, Asia, Siberia and Europe were sampled. Transport pathways of detected plumes included advection below 700 hPa, air mass uplifting in warm conveyor belts, and high altitude transport in the upper troposphere. By means of the Lagrangian particle dispersion model FLEXPART, trace gas analysis of O3 and CO, particle size distributions and aerosol chemical composition 48 pollution events were identified and classified into five chemically distinct categories. Aerosol from North American BB consisted of 22% particulate sulphate, while with increasing anthropogenic and Asian influence aerosol in Asian FF dominated plumes was composed of up to 37% sulphate category mean value. Overall, it was found that the organic matter fraction was larger (85%) in pollution plumes than for background conditions (71%). Despite different source regions and emission types the particle oxygen to carbon ratio of all plume classes was around 1 indicating low-volatility highly oxygenated aerosol. The volume size distribution of out-of-plume aerosol showed markedly smaller modes than all other distributions with two Aitken mode diameters of 24 and 43 nm and a geometric standard deviation σg of 1.12 and 1.22, respectively, while another very broad mode was found at 490 nm (σg = 2.35). Nearly pure BB particles from North America exhibited an Aitken mode at 66 nm (σg = 1.46) and an accumulation mode diameter of 392 nm (σg = 1.76). An aerosol lifetime, including all processes from emission to

Aerosol particle transport modeling for preclosure safety studies of nuclear waste repositories

International Nuclear Information System (INIS)

Gelbard, F.

1989-01-01

An important concern for preclosure safety analysis of a nuclear waste repository is the potential release to the environment of respirable aerosol particles. Such particles, less than 10 μm in aerodynamic diameter, may have significant adverse health effects if inhaled. To assess the potential health effects of these particles, it is not sufficient to determine the mass fraction of respirable aerosol. The chemical composition of the particles is also of importance since different radionuclides may pose vastly different health hazards. Thus, models are needed to determine under normal and accident conditions the particle size and the chemical composition distributions of aerosol particles as a function of time and of position in the repository. In this work a multicomponent sectional aerosol model is used to determine the aerosol particle size and composition distributions in the repository. A range of aerosol mass releases with varying mean particle sizes and chemical compositions is used to demonstrate the sensitivities and uncertainties of the model. Decontamination factors for some locations in the repository are presented. 8 refs., 1 tab

Global and Regional Impacts of HONO on the Chemical Composition of Clouds and Aerosols

Science.gov (United States)

Elshorbany, Y. F.; Crutzen, P. J.; Steil, B.; Pozzer, A.; Tost, H.; Lelieveld, J.

2014-01-01

Recently, realistic simulation of nitrous acid (HONO) based on the HONO / NOx ratio of 0.02 was found to have a significant impact on the global budgets of HOx (OH + HO2) and gas phase oxidation products in polluted regions, especially in winter when other photolytic sources are of minor importance. It has been reported that chemistry-transport models underestimate sulphate concentrations, mostly during winter. Here we show that simulating realistic HONO levels can significantly enhance aerosol sulphate (S(VI)) due to the increased formation of H2SO4. Even though in-cloud aqueous phase oxidation of dissolved SO2 (S(IV)) is the main source of S(VI), it appears that HONO related enhancement of H2O2 does not significantly affect sulphate because of the predominantly S(IV) limited conditions, except over eastern Asia. Nitrate is also increased via enhanced gaseous HNO3 formation and N2O5 hydrolysis on aerosol particles. Ammonium nitrate is enhanced in ammonia-rich regions but not under ammonia-limited conditions. Furthermore, particle number concentrations are also higher, accompanied by the transfer from hydrophobic to hydrophilic aerosol modes. This implies a significant impact on the particle lifetime and cloud nucleating properties. The HONO induced enhancements of all species studied are relatively strong in winter though negligible in summer. Simulating realistic HONO levels is found to improve the model measurement agreement of sulphate aerosols, most apparent over the US. Our results underscore the importance of HONO for the atmospheric oxidizing capacity and corroborate the central role of cloud chemical processing in S(IV) formation

Wintertime aerosol chemical composition and source apportionment of the organic fraction in the metropolitan area of Paris

Directory of Open Access Journals (Sweden)

M. Crippa

2013-01-01

Full Text Available The effect of a post-industrial megacity on local and regional air quality was assessed via a month-long field measurement campaign in the Paris metropolitan area during winter 2010. Here we present source apportionment results from three aerosol mass spectrometers and two aethalometers deployed at three measurement stations within the Paris region. Submicron aerosol composition is dominated by the organic fraction (30–36% and nitrate (28–29%, with lower contributions from sulfate (14–16%, ammonium (12–14% and black carbon (7–13%.

Organic source apportionment was performed using positive matrix factorization, resulting in a set of organic factors corresponding both to primary emission sources and secondary production. The dominant primary sources are traffic (11–15% of organic mass, biomass burning (13–15% and cooking (up to 35% during meal hours. Secondary organic aerosol contributes more than 50% to the total organic mass and includes a highly oxidized factor from indeterminate and/or diverse sources and a less oxidized factor related to wood burning emissions. Black carbon was apportioned to traffic and wood burning sources using a model based on wavelength-dependent light absorption of these two combustion sources. The time series of organic and black carbon factors from related sources were strongly correlated. The similarities in aerosol composition, total mass and temporal variation between the three sites suggest that particulate pollution in Paris is dominated by regional factors, and that the emissions from Paris itself have a relatively low impact on its surroundings.

Characteristics and Composition of Atmospheric Aerosols in Phimai, Central Thailand During BASE-ASIA

Science.gov (United States)

Li, Can; Tsay, Si-Chee; Hsu, N. Christina; Kim, Jin Young; Howell, Steven G.; Huebert, Barry J.; Ji, Qiang; Jeong, Myeong-Jae; Wang, Sheng-Hsiang; Hansell, Richard A.;

Aerosol chemical compositions in the North China Plain and the impact on the visibility in Beijing and Tianjin

Science.gov (United States)

Zou, Jianan; Liu, Zirui; Hu, Bo; Huang, Xiaojuan; Wen, Tianxue; Ji, Dongsheng; Liu, Jingyun; Yang, Yang; Yao, Qing; Wang, Yuesi

2018-03-01

To better understand the characteristics of the chemical compositions of aerosols comprised of water soluble ions (WSIs) and carbonaceous aerosol (CA) and their impacts on the visibility throughout the North China Plain (NCP), four experimental sampling campaigns were carried out between June 2013 and May 2014. The sampling sites were located in Beijing, Xiangshan, Tianjin, Shijiazhuang, and Qinhuangdao. The air pollution episodes mainly occurred during the autumn and winter in the NCP. With regard to different particle size distributions, the ratio of anions to cations in the fine size (0.64) was greater than that in the coarse size (0.54) in the NCP. Coefficients of divergence indicate that aerosol pollution had similar characteristics in the five cities of the NCP and that the pollutants were characterized by mutual influences and regional transfer processes. There were different non-linear correlations between the visibility and mass concentrations of PM2.5 at different relative humidity (RH) conditions. When the RH was > 70%, the visibility was light extinction coefficients (LEC) from the measured concentrations of chemical species. Organic matter (OM), ammonium nitrate (AN), and ammonium sulfate (AS) were the three dominant species that contributed to the LEC in Beijing and had the highest proportions of total contributions to the LEC in the summer, accounting for 32.2%, 25.9%, and 24.4%, respectively. The LEC of sea salts did not change much throughout the year and accounted for 4.1-5.3% in Beijing and 4.8-7.4% in Tianjin. According to the Ambient Air Quality Standard, the days were divided into pollutional days (PD) and attained days (AD). The increasing concentrations of AN, AS and OM resulted in an increase in the LEC in the NCP, which led to the occurrences of low visibility events during the autumn and winter. NH4+, NO3-, and SO42 - mainly existed as fine size particles (diameter < 2.1 μm) in Beijing (73.5%, 80.7%, and 78.0% on PD and 63.3%, 79.4%, and

Biomass burning aerosols characterization from ground based and profiling measurements

Science.gov (United States)

Marin, Cristina; Vasilescu, Jeni; Marmureanu, Luminita; Ene, Dragos; Preda, Liliana; Mihailescu, Mona

2018-04-01

The study goal is to assess the chemical and optical properties of aerosols present in the lofted layers and at the ground. The biomass burning aerosols were evaluated in low level layers from multi-wavelength lidar measurements, while chemical composition at ground was assessed using an Aerosol Chemical Speciation Monitor (ACSM) and an Aethalometer. Classification of aerosol type and specific organic markers were used to explore the potential to sense the particles from the same origin at ground base and on profiles.

Characterizing the Asian Tropopause Aerosol Layer (ATAL) Using Satellite Observations, Balloon Measurements and a Chemical Transport Model

Science.gov (United States)

Fairlie, T. D.; Vernier, J.-P.; Liu, H.; Deshler, T.; Natarajan, M.; Bedka, K.; Wegner, T.; Baker, N.; Gadhavi, H.; Ratnam, M. V.;

Data Descriptor : Collocated observations of cloud condensation nuclei, particle size distributions, and chemical composition

NARCIS (Netherlands)

Schmale, Julia; Henning, Silvia; Henzing, Bas; Keskinen, Helmi; Sellegri, Karine; Ovadnevaite, Jurgita; Bougiatioti, Aikaterini; Kalivitis, Nikos; Stavroulas, Iasonas; Jefferson, Anne; Park, Minsu; Schlag, Patrick; Kristensson, Adam; Iwamoto, Yoko; Pringle, Kirsty; Reddington, Carly; Aalto, Pasi; Äijälä, Mikko; Baltensperger, Urs; Bialek, Jakub; Birmili, Wolfram; Bukowiecki, Nicolas; Ehn, Mikael; Fjæraa, Ann Mari; Fiebig, Markus; Frank, Göran; Fröhlich, Roman; Frumau, Arnoud; Furuya, Masaki; Hammer, Emanuel; Heikkinen, Liine; Herrmann, Erik; Holzinger, Rupert; Hyono, Hiroyuki; Kanakidou, Maria; Kiendler-Scharr, Astrid; Kinouchi, Kento; Kos, Gerard P A; Kulmala, Markku; Mihalopoulos, Nikolaos; Motos, Ghislain; Nenes, Athanasios; O'Dowd, Colin; Paramonov, Mikhail; Petäjä, Tuukka; Picard, David; Poulain, Laurent; Prévôt, André Stephan Henry; Slowik, Jay; Sonntag, Andre; Swietlicki, Erik; Svenningsson, Birgitta; Tsurumaru, Hiroshi; Wiedensohler, Alfred; Wittbom, Cerina; Ogren, John A.; Matsuki, Atsushi; Yum, Seong Soo; Myhre, Cathrine Lund; Carslaw, Ken; Stratmann, Frank; Gysel, Martin

2017-01-01

Cloud condensation nuclei (CCN) number concentrations alongside with submicrometer particle number size distributions and particle chemical composition have been measured at atmospheric observatories of the Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS) as well as other

The effect of meteorological and chemical factors on the agreement between observations and predictions of fine aerosol composition in southwestern Ontario during BAQS-Met

Science.gov (United States)

Markovic, M. Z.; Hayden, K. L.; Murphy, J. G.; Makar, P. A.; Ellis, R. A.; Chang, R. Y.-W.; Slowik, J. G.; Mihele, C.; Brook, J.

2011-04-01

The Border Air Quality and Meteorology Study (BAQS-Met) was an intensive, collaborative field campaign during the summer of 2007 that investigated the effects of transboundary pollution, local pollution, and local meteorology on air quality in southwestern Ontario. This analysis focuses on the measurements of the inorganic constituents of particulate matter with diameter of less than 1 μm (PM1), with a specific emphasis on nitrate. We evaluate the ability of AURAMS, Environment Canada's chemical transport model, to represent regional air pollution in SW Ontario by comparing modelled aerosol inorganic chemical composition with measurements from Aerosol Mass Spectrometers (AMS) onboard the National Research Council (NRC) of Canada Twin Otter aircraft and at a ground site in Harrow, ON. The agreement between modelled and measured pNO3- at the ground site (observed mean (Mobs) = 0.50 μg m-3; modelled mean (Mmod) = 0.58 μg m-3; root mean square error (RSME) = 1.27 μg m-3) was better than aloft (Mobs = 0.32 μg m-3; Mmod = 0.09 μg m-3; RSME = 0.48 μg m-3). Possible reasons for discrepancies include errors in (i) emission inventories, (ii) atmospheric chemistry, (iii) predicted meteorological parameters, or (iv) gas/particle thermodynamics in the model framework. Using the inorganic thermodynamics model, ISORROPIA, in an offline mode, we find that the assumption of thermodynamic equilibrium is consistent with observations of gas and particle composition at Harrow. We develop a framework to assess the sensitivity of PM1 nitrate to meteorological and chemical parameters and find that errors in both the predictions of relative humidity and free ammonia (FA ≡ NH3(g) + pNH4+ - 2 · pSO42-) are responsible for the poor agreement between modelled and measured values.

Evaluation of simulated aerosol properties with the aerosol-climate model ECHAM5-HAM using observations from the IMPACT field campaign

NARCIS (Netherlands)

Roelofs, G.-J.; Brink, H. ten; Kiendler-Scharr, A.; Leeuw, G. de; Mensah, A.; Minikin, A.; Otjes, R.

2010-01-01

In May 2008, the measurement campaign IMPACT for observation of atmospheric aerosol and cloud properties was conducted in Cabauw, The Netherlands. With a nudged version of the coupled aerosol-climate model ECHAM5-HAM we simulate the size distribution and chemical composition of the aerosol and the

The impacts of aerosol loading, composition, and water uptake on aerosol extinction variability in the Baltimore–Washington, D.C. region

Directory of Open Access Journals (Sweden)

A. J. Beyersdorf

2016-01-01

Full Text Available In order to utilize satellite-based aerosol measurements for the determination of air quality, the relationship between aerosol optical properties (wavelength-dependent, column-integrated extinction measured by satellites and mass measurements of aerosol loading (PM2.5 used for air quality monitoring must be understood. This connection varies with many factors including those specific to the aerosol type – such as composition, size, and hygroscopicity – and to the surrounding atmosphere, such as temperature, relative humidity (RH, and altitude, all of which can vary spatially and temporally. During the DISCOVER-AQ (Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality project, extensive in situ atmospheric profiling in the Baltimore, MD–Washington, D.C. region was performed during 14 flights in July 2011. Identical flight plans and profile locations throughout the project provide meaningful statistics for determining the variability in and correlations between aerosol loading, composition, optical properties, and meteorological conditions. Measured water-soluble aerosol mass was composed primarily of ammonium sulfate (campaign average of 32 % and organics (57 %. A distinct difference in composition was observed, with high-loading days having a proportionally larger percentage of sulfate due to transport from the Ohio River Valley. This composition shift caused a change in the aerosol water-uptake potential (hygroscopicity such that higher relative contributions of inorganics increased the bulk aerosol hygroscopicity. These days also tended to have higher relative humidity, causing an increase in the water content of the aerosol. Conversely, low-aerosol-loading days had lower sulfate and higher black carbon contributions, causing lower single-scattering albedos (SSAs. The average black carbon concentrations were 240 ng m−3 in the lowest 1 km, decreasing to 35�

Org Areo Boreal Forest Sources, compositions and properties of newly formed and regional organic aerosol in a boreal forest during the Biogenic Aerosol: Effects on Clouds and Climate Campaign

Energy Technology Data Exchange (ETDEWEB)

Thornton, Joel A [Univ. of Washington, Seattle, WA (United States)

2017-12-01

The major goals of this project were to make unique measurements, as part of the DOE sponsored Biogenic Aerosol Effects on Clouds and Climate (BAECC) campaign, of the volatility and molecular composition of organic aerosol, as well as gas-phase concentrations of oxygenated organic compounds that interact and affect organic aerosol. In addition, we aimed to conduct a similar set of measurements as part of a collaborative set of environmental simulation chamber experiments at PNNL, the aim of which was to simulate the atmospheric oxidation of key biogenic volatile organic compounds (BVOC) and study the associated formation and evolution of secondary organic aerosol (SOA). The target BVOC were a set of monoterpenes, isoprene, and related intermediates such as IEPOX. The ultimate goal of such measurements are to develop a more detailed mechanistic understanding of the sensitivity of SOA mass formation and lifetime to precursor and environmental conditions. Molecular composition and direct volatility measurements provide robust tracers of chemical processing and properties. As such, meeting these goals will allow for stronger constraints on the types of processes and their fundamental descriptions needed to simulate aerosol particle number and size, and cloud nucleating ability in regional and global earth system models.

Chemical composition, microstructure, and hygroscopic properties of aerosol particles at the Zotino Tall Tower Observatory (ZOTTO), Siberia, during a summer campaign

Science.gov (United States)

Mikhailov, E. F.; Mironov, G. N.; Pöhlker, C.; Chi, X.; Krüger, M. L.; Shiraiwa, M.; Förster, J.-D.; Pöschl, U.; Vlasenko, S. S.; Ryshkevich, T. I.; Weigand, M.; Kilcoyne, A. L. D.; Andreae, M. O.

2015-08-01

In this study we describe the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the Zotino Tall Tower Observatory (ZOTTO) in central Siberia (61° N, 89° E) from 16 to 21 June 2013. The hygroscopic growth measurements were supplemented with chemical analyses of the samples, including inorganic ions and organic/elemental carbon. In addition, the microstructure and chemical compositions of aerosol particles were analyzed by x-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM). A mass closure analysis indicates that organic carbon accounted for 61 and 38 % of particulate matter (PM) in the accumulation mode and coarse mode, respectively. The water-soluble fraction of organic matter was estimated to be 52 and 8 % of PM in these modes. Sulfate, predominantly in the form of ammoniated sulfate, was the dominant inorganic component in both size modes: ~ 34 % in the accumulation mode vs. ~ 47 % in the coarse mode. The hygroscopic growth measurements were conducted with a filter-based differential hygroscopicity analyzer (FDHA) over the range of 5-99.4 % RH in the hydration and dehydration operation modes. The FDHA study indicates that both accumulation and coarse modes exhibit pronounced water uptake approximately at the same relative humidity (RH), starting at ~ 70 %, while efflorescence occurred at different humidities, i.e., at ~ 35 % RH for submicron particles vs. ~ 50 % RH for supermicron particles. This ~ 15 % RH difference was attributed to higher content of organic material in the submicron particles, which suppresses water release in the dehydration experiments. The kappa mass interaction model (KIM) was applied to characterize and parameterize non-ideal solution behavior and concentration-dependent water uptake by atmospheric aerosol samples in the 5-99.4 % RH range. Based on KIM, the volume-based hygroscopicity parameter, κv, was calculated. The κv,ws value related to the water-soluble (ws

Chemical composition of size-segregated aerosols in Lhasa city, Tibetan Plateau

Science.gov (United States)

Wan, Xin; Kang, Shichang; Xin, Jinyuan; Liu, Bin; Wen, Tianxue; Wang, Pengling; Wang, Yuesi; Cong, Zhiyuan

2016-06-01

To reveal the chemical characteristics of size-segregated aerosols in the high-altitude city of Tibetan Plateau, eight-size aerosol samples were collected in Lhasa from March 2013 to February 2014. The annual mean of online PM2.5 was 25.0 ± 16.0 μg m- 3, which was much lower than Asian cities but similar with some European cities. The annual mean concentrations of organic carbon (OC, 7.92 μg m- 3 in PM2.1 and 12.66 μg m- 3 in PM9.0) and elemental carbon (EC, 1.00 μg m- 3 in PM2.1 and 1.21 μg m- 3 in PM9.0) in Lhasa aerosols were considerably lower than those heavily polluted cities such as Beijing and Xi'an, China and Kathmandu, Nepal. Sulfate, NO3-, NH4+ and Ca2 + were 0.75 ± 0.31, 0.82 ± 0.35, 0.38 ± 0.34 and 0.57 ± 0.29 μg m- 3 in fine particles while in coarse particles they were 0.57 ± 0.37, 0.73 ± 0.23, 0.07 ± 0.03 and 2.52 ± 1.37 μg m- 3, respectively. Secondary water-soluble ions composed 35.8% of the total ionic components in fine particles according to the established electroneutrality, while in coarse particles they took up only 9.3%. Ca2 + (40.6%) was the major component of the coarse particles. For seasonality, the concentrations of OC, EC, SO42 -, NH4+, K+, Ca2 +, Mg2 +, Cl- and Na+ presented higher values during late autumn and winter but were relatively lower in spring and summer. Nevertheless, NO3- was considerably higher in summer and autumn, presumably due to increased tourist-vehicle emissions. During winter and spring, [Ca2 +]/[NO3-+ SO42 -] ratios in coarse particles showed higher values of 7.31 and 6.17, respectively, emphasizing the dust influence. [NO3-]/[SO42 -] ratios in fine particles during spring, summer and autumn exceeding 1 indicated that the currently predominant vehicle exhaust makes a greater contribution to the aerosols. While more stationary sources such as coal and biomass burning existed in winter since the [NO3-]/[SO42 -] ratio was less than 1. Different sources and formation processes lead to a bimodal size

Field characterization of the PM2.5 Aerosol Chemical Speciation Monitor: insights into the composition, sources, and processes of fine particles in eastern China

Directory of Open Access Journals (Sweden)

Y. Zhang

2017-12-01

Full Text Available A PM2.5-capable aerosol chemical speciation monitor (Q-ACSM was deployed in urban Nanjing, China, for the first time to measure in situ non-refractory fine particle (NR-PM2.5 composition from 20 October to 19 November 2015, along with parallel measurements of submicron aerosol (PM1 species by a standard Q-ACSM. Our results show that the NR-PM2.5 species (organics, sulfate, nitrate, and ammonium measured by the PM2.5-Q-ACSM are highly correlated (r2 > 0.9 with those measured by a Sunset Lab OC  /  EC analyzer and a Monitor for AeRosols and GAses (MARGA. The comparisons between the two Q-ACSMs illustrated similar temporal variations in all NR species between PM1 and PM2.5, yet substantial mass fractions of aerosol species were observed in the size range of 1–2.5 µm. On average, NR-PM1−2.5 contributed 53 % of the total NR-PM2.5, with sulfate and secondary organic aerosols (SOAs being the two largest contributors (26 and 27 %, respectively. Positive matrix factorization of organic aerosol showed similar temporal variations in both primary and secondary OAs between PM1 and PM2.5, although the mass spectra were slightly different due to more thermal decomposition on the capture vaporizer of the PM2.5-Q-ACSM. We observed an enhancement of SOA under high relative humidity conditions, which is associated with simultaneous increases in aerosol pH, gas-phase species (NO2, SO2, and NH3 concentrations and aerosol water content driven by secondary inorganic aerosols. These results likely indicate an enhanced reactive uptake of SOA precursors upon aqueous particles. Therefore, reducing anthropogenic NOx, SO2, and NH3 emissions might not only reduce secondary inorganic aerosols but also the SOA burden during haze episodes in China.

Single particle analysis of eastern Mediterranean aerosol particles: Influence of the source region on the chemical composition

Science.gov (United States)

Clemen, Hans-Christian; Schneider, Johannes; Köllner, Franziska; Klimach, Thomas; Pikridas, Michael; Stavroulas, Iasonas; Sciare, Jean; Borrmann, Stephan

2017-04-01

The Mediterranean region is one of the most climatically sensitive areas and is influenced by air masses of different origin. Aerosol particles are one important factor contributing to the Earth's radiative forcing, but knowledge about their composition and sources is still limited. Here, we report on results from the INUIT-BACCHUS-ACTRIS campaign, which was conducted at the Cyprus Atmospheric Observatory (CAO, Agia Marina Xyliatou) in Cyprus in April 2016. Our results show that the chemical composition of the aerosol particles in the eastern Mediterranean is strongly dependent on their source region. The composition of particles in a size range between 150 nm and 3 μm was measured using the Aircraft-based Laser ABlation Aerosol MAss spectrometer (ALABAMA), which is a single particle laser ablation instrument using a bipolar time-of-flight mass spectrometer. The mass spectral information on cations and anions allow for the analysis of different molecular fragments. The information about the source regions results from backward trajectories using HYSPLIT Trajectory Model (Trajectory Ensemble) on hourly basis. To assess the influence of certain source regions on the air masses arriving at CAO, we consider the number of trajectories that crossed the respective source region within defined time steps. For a more detailed picture also the height and the velocity of the air masses during their overpass above the source regions will be considered. During the campaign at CAO in April 2016 three main air mass source regions were observed: 1) Northern Central Europe, likely with an enhanced anthropogenic influence (e.g. sulfate and black carbon from combustion processes, fly ash particles from power plants, characterized by Sr and Ba), 2) Southwest Europe, with a higher influence of the Mediterranean Sea including sea salt particles (characterized by, e.g., NaxCly, NaClxNOy), 3) Northern Africa/Sahara, with air masses that are expected to have a higher load of mineral dust

Source identification and airborne chemical characterisation of aerosol pollution from long-range transport over Greenland during POLARCAT summer campaign 2008

Directory of Open Access Journals (Sweden)

J. Schmale

2011-10-01

Full Text Available We deployed an aerosol mass spectrometer during the POLARCAT (Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate, Chemistry, Aerosols, and Transport summer campaign in Greenland in June/July 2008 on the research aircraft ATR-42. Online size resolved chemical composition data of submicron aerosol were collected up to 7.6 km altitude in the region 60 to 71° N and 40 to 60° W. Biomass burning (BB and fossil fuel combustion (FF plumes originating from North America, Asia, Siberia and Europe were sampled. Transport pathways of detected plumes included advection below 700 hPa, air mass uplifting in warm conveyor belts, and high altitude transport in the upper troposphere. By means of the Lagrangian particle dispersion model FLEXPART, trace gas analysis of O₃ and CO, particle size distributions and aerosol chemical composition 48 pollution events were identified and classified into five chemically distinct categories. Aerosol from North American BB consisted of 22% particulate sulphate, while with increasing anthropogenic and Asian influence aerosol in Asian FF dominated plumes was composed of up to 37% sulphate category mean value. Overall, it was found that the organic matter fraction was larger (85% in pollution plumes than for background conditions (71%. Despite different source regions and emission types the particle oxygen to carbon ratio of all plume classes was around 1 indicating low-volatility highly oxygenated aerosol. The volume size distribution of out-of-plume aerosol showed markedly smaller modes than all other distributions with two Aitken mode diameters of 24 and 43 nm and a geometric standard deviation σ_g of 1.12 and 1.22, respectively, while another very broad mode was found at 490 nm (σ_g = 2.35. Nearly pure BB particles from North America exhibited an Aitken mode at 66 nm (σ_g = 1.46 and an accumulation mode diameter of 392 nm (σ_g = 1

The ToF-ACSM: a portable aerosol chemical speciation monitor with TOFMS detection

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R. Fröhlich

2013-11-01

Full Text Available We present a new instrument for monitoring aerosol composition, the time-of-flight aerosol chemical speciation monitor (ToF-ACSM, combining precision state-of-the-art time-of-flight mass spectrometry with stability, reliability, and easy handling, which are necessities for long-term monitoring operations on the scale of months to years. Based on Aerodyne aerosol mass spectrometer (AMS technology, the ToF-ACSM provides continuous online measurements of chemical composition and mass of non-refractory submicron aerosol particles. In contrast to the larger AMS, the compact-sized and lower-priced ToF-ACSM does not feature particle sizing, similar to the widely-used quadrupole-ACSM (Q-ACSM. Compared to the Q-ACSM, the ToF-ACSM features a better mass resolution of M/ΔM = 600 and better detection limits on the order of −3 for a time resolution of 30 min. With simple upgrades these limits can be brought down by another factor of ~ 8. This allows for operation at higher time resolutions and in low concentration environments. The associated software packages (single packages for integrated operation and calibration and analysis provide a high degree of automation and remote access, minimising the need for trained personnel on site. Intercomparisons with Q-ACSM, C-ToF-AMS, nephelometer and scanning mobility particle sizer (SMPS measurements, performed during a first long-term deployment (> 10 months on the Jungfraujoch mountain ridge (3580 m a.s.l. in the Swiss Alps, agree quantitatively. Additionally, the mass resolution of the ToF-ACSM is sufficient for basic mass defect resolved peak fitting of the recorded spectra, providing a data stream not accessible to the Q-ACSM. This allows for quantification of certain hydrocarbon and oxygenated fragments (e.g. C3H7+ and C2H3O+, both occurring at m/Q = 43 Th, as well as improving inorganic/organic separation.

Application of PIXE technique to studies on global warming/cooling effect of atmospheric aerosols

International Nuclear Information System (INIS)

Kasahara, M.; Hoeller, R.; Tohno, S.; Onishi, Y.; Ma, C.-J.

2002-01-01

During the last decade, the importance of global warming has been recognized worldwide. Atmospheric aerosols play an important role in the global warming/cooling effects. The physicochemical properties of aerosol particles are fundamental to understanding such effects. In this study, the PIXE technique was applied to measure the average chemical properties of aerosols. Micro-PIXE was also applied to investigate the mixing state of the individual aerosol particle. The chemical composition data were used to estimate the optical properties of aerosols. The average values of aerosol radiative forcing were -1.53 w/m 2 in Kyoto and +3.3 w/m 2 in Nagoya, indicating cooling and warming effects respectively. The difference of radiative forcing in the two cities may be caused by the large difference in chemical composition of aerosols

Importance of relative humidity in the oxidative ageing of organic aerosols: case study of the ozonolysis of maleic acid aerosol

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P. J. Gallimore

2011-12-01

Full Text Available Many important atmospheric aerosol processes depend on the chemical composition of the aerosol, e.g. water uptake and particle cloud interactions. Atmospheric ageing processes, such as oxidation reactions, significantly and continuously change the chemical composition of aerosol particles throughout their lifetime. These ageing processes are often poorly understood. In this study we utilize an aerosol flow tube set up and an ultra-high resolution mass spectrometer to explore the effect of relative humidity (RH in the range of <5–90% on the ozonolysis of maleic acid aerosol which is employed as model organic aerosol system. Due to the slow reaction kinetics relatively high ozone concentrations of 160–200 ppm were used to achieve an appreciable degree of oxidation of maleic acid. The effect of oxidative ageing on the hygroscopicity of maleic acid particles is also investigated using an electrodynamic balance and thermodynamic modelling. RH has a profound effect on the oxidation of maleic acid particles. Very little oxidation is observed at RH < 50% and the only observed reaction products are glyoxylic acid and formic acid. In comparison, when RH > 50% there are about 15 oxidation products identified. This increased oxidation was observed even when the particles were exposed to high humidities long after a low RH ozonolysis reaction. This result might have negative implications for the use of water as an extraction solvent for the analysis of oxidized organic aerosols. These humidity-dependent differences in the composition of the ozonolyzed aerosol demonstrate that water is both a key reactant in the oxidation scheme and a determinant of particle phase and hence diffusivity. The measured chemical composition of the processed aerosol is used to model the hygroscopic growth, which compares favourably with water uptake results from the electrodynamic balance measurements. A reaction mechanism is presented which takes into account the RH dependent

Impacts of the mixing state and chemical composition on the cloud condensation nuclei (CCN) activity in Beijing during winter, 2016

Science.gov (United States)

Ren, J.; Zhang, F.

2017-12-01

Abstract.Understanding aerosol chemical composition and mixing state on CCN activity in polluted urban area is crucial to determine NCCN accurately and thus to quantify aerosol indirect effects. Aerosol hrgroscopicity, size-resolved cloud condensation nuclei (CCN) concentration and chemical composition are measured under polluted and background conditions in Beijing based on the Air Pollution and Human Health (APHH) field campaign in winter 2016. The CCN number concentration (NCCN) is predicted by using κ-Köhler theory from the PNSD and five simplified of the mixing state and chemical composition. The assumption of EIS (sulfate, nitrate and SOA internally mixed, and POA and BC externally mixed with size-resolved chemical composition) shows the best closure to predict NCCN with the ratio of predicted to measured NCCN of 0.96-1.12 both in POL and BG conditions. Under BG conditions, IB (internal mixture with bulk chemical composition) scheme achieves the best CCN closure during any periods of a day. In polluted days, EIS and IS (internal mixture with size-resolved chemical composition) scheme may achieve better closure than IB scheme due to the heterogeneity in particles composition across different size. ES (external mixture with size-resolved chemical composition) and EB (external mixture with bulk chemical composition) scheme markedly underestimate the NCCN with the ratio of predicted to measured NCCN of 0.6-0.8. In addition, we note that assumptions of size-resolved composition (IS or ES) show very limited promotes by comparing with the assumptions of bulk composition (IB or EB), furthermore, the prediction becomes worse by using size-resolved assumption in clean days. The predicted NCCN during eve-rush periods shows the most sensitivity to the five different assumptions, with ratios of the predicted and measured NCCN ranging from 0.5 to 1.4, reflecting great impacts from evening traffic and cooking sources. The result from the sensitivity examination of predict

Nature, Origin, Potential Composition, and Climate Impact of the Asian Tropopause Aerosol Layer (ATAL)

Science.gov (United States)

Fairlie, T. D.; Vernier, J.-P.; Thomason, L. W.; Natarajan, M.; Bedka, K.; Wienhold, F.; Bian J.; Martinsson, B.

2015-01-01

Satellite observations from SAGE II and CALIPSO indicate that summertime aerosol extinction has more than doubled in the Asian Tropopause Aerosol Layer (ATAL) since the late 1990s. Here we show remote and in-situ observations, together with results from a chemical transport model (CTM), to explore the likely composition, origin, and radiative forcing of the ATAL. We show in-situ balloon measurements of aerosol backscatter, which support the high levels observed by CALIPSO since 2006. We also show in situ measurements from aircraft, which indicate a predominant carbonaceous contribution to the ATAL (Carbon/Sulfur ratios of 2- 10), which is supported by the CTM results. We show that the peak in ATAL aerosol lags by 1 month the peak in CO from MLS, associated with deep convection over Asia during the summer monsoon. This suggests that secondary formation and growth of aerosols in the upper troposphere on monthly timescales make a significant contribution to ATAL. Back trajectory calculations initialized from CALIPSO observations provide evidence that deep convection over India is a significant source for ATAL through the vertical transport of pollution to the upper troposphere.

Characterization of biogenic secondary organic aerosols using statistical methods; Charakterisierung Biogener Sekundaerer Organischer Aerosole mit Statistischen Methoden

Energy Technology Data Exchange (ETDEWEB)

Spindler, Christian

2010-07-01

Atmospheric aerosols have important influence on the radiation balance of the Earth, on visibility and human health. Secondary organic aerosol is formed from gas-to-particle conversion of oxidized volatile organic compounds. A dominant fraction of the gases originates from plant emissions, making biogenic secondary organic aerosol (BSOA) an especially important constituent of the atmosphere. Knowing the chemical composition of BSOA particles is crucial for a thorough understanding of aerosol processes in the environment. In this work, the chemical composition of BSOA particles was measured with aerosol mass spectrometry and analyzed with statistical methods. The experimental part of the work comprises process studies of the formation and aging of biogenic aerosols in simulation chambers. Using a plant chamber, real tree emissions were used to produce particles in a way close to conditions in forest environments. In the outdoor chamber SAPHIR, OH-radicals were produced from the photooxidation of ozone under illumination with natural sunlight. Here, BSOA was produced from defined mixtures of mono- and sesquiterpenes that represent boreal forest emissions. A third kind of experiments was performed in the indoor chamber AIDA. Here, particles were produced from ozonolysis of single monoterpenes and aged by condensing OH-oxidation products. Two aerosol mass spectrometers (AMS) were used to measure the chemical composition of the particles. One of the instruments is equipped with a quadrupole mass spectrometer providing unit mass resolution. The second instrument contains a time-of-flight mass spectrometer and provides mass resolution sufficient to distinguish different fragments with the same nominal mass. Aerosol mass spectra obtained with these instruments are strongly fragmented due to electron impact ionization of the evaporated molecules. In addition, typical BSOA mass spectra are very similar to each other. In order to get a more detailed knowledge about the mass

Investigations on the chemical composition of the organic fraction of tropospheric aerosols. Final report; Untersuchungen zur chemischen Zusammensetzung der organischen Komponente des troposphaerischen Aerosols. AFS-Abschlussbericht

Energy Technology Data Exchange (ETDEWEB)

Hoffmann, T.; Warscheid, B.

2000-07-01

Although the knowledge about the significance of airborne particulate matter for the radiation balance of the atmosphere has increased during the last few years, several important aerosol formation mechanisms are still poorly understood. This is especially true for aerosols which are formed from volatile organic precursors from natural or anthropogenic sources (secondary organic aerosols). Therefore, the research project aimed on the development of a mass spectrometric real-time technique for the qualitative and quantitative investigations of the chemical composition of secondary organic aerosols, especially from the ozonolysis of monoterpenes (e.g. {alpha}-pinene, {beta}-pinene, sabinene, {delta}{sup 3}-carene, limonene). Using a modified atmospheric pressure chemical ionisation source (APCI), the formation of gas and particle phase products could be observed with a time resolution of about 1 second. The detection limit of the developed technique is about 100 ppt(v/v) in the positive ion mode. Based on the development of standard addition techniques, selected products were quantified in the gas and particle phase. Using isotopically labelled water also certain underlying reaction mechanisms were investigated. Another part of the project focused on the identification of low volatile reaction products by MS/MS-studies. These studies showed that the particle phase is mainly composed of several multifunctional carboxylic acids (dicarboxylic acids, oxo-carboxylic acids, hydroxy-carboxylic acids etc.). Finally, the APCI-studies gave robust evidences on the presence of strong intermolecular interactions between the different products. Since the experiments also showed a correlation between the intensity of product interactions (adduct formation) by hydrogen-bonding and new particle formation potential, the results of the project can be considered to provide an important contribution for an better understanding of nucleation events above forested areas. (orig.) [German

Physical and chemical characterization of urban winter-time aerosols by mobile measurements in Helsinki, Finland

Science.gov (United States)

Pirjola, Liisa; Niemi, Jarkko V.; Saarikoski, Sanna; Aurela, Minna; Enroth, Joonas; Carbone, Samara; Saarnio, Karri; Kuuluvainen, Heino; Kousa, Anu; Rönkkö, Topi; Hillamo, Risto

2017-06-01

A two-week measurement campaign by a mobile laboratory van was performed in urban environments in the Helsinki metropolitan area, Finland, in winter 2012, to obtain a comprehensive view on aerosol properties and sources. The abundances and physico-chemical properties of particles varied strongly in time and space, depending on the main sources of aerosols. Four major types of winter aerosol were recognized: 1) clean background aerosol with low particle number (Ntot) and lung deposited surface area (LDSA) concentrations due to marine air flows from the Atlantic Ocean; 2) long-range transported (LRT) pollution aerosol due to air flows from eastern Europe where the particles were characterized by the high contribution of oxygenated organic aerosol (OOA) and inorganic species, particularly sulphate, but low BC contribution, and their size distribution possessed an additional accumulation mode; 3) fresh smoke plumes from residential wood combustion in suburban small houses, these particles were characterized by high biomass burning organic aerosol (BBOA) and black carbon (BC) concentrations; and 4) fresh emissions from traffic while driving on busy streets in the city centre and on the highways during morning rush hours. This aerosol was characterized by high concentration of Ntot, LDSA, small particles in the nucleation mode, as well as high hydrocarbon-like organic aerosol (HOA) and BC concentrations. In general, secondary components (OOA, NO3, NH4, and SO4) dominated the PM1 chemical composition during the LRT episode accounting for 70-80% of the PM1 mass, whereas fresh primary emissions (BC, HOA and BBOA) dominated the local traffic and wood burning emissions. The major individual particle types observed with electron microscopy analysis (TEM/EDX) were mainly related to residential wood combustion (K/S/C-rich, soot, other C-rich particles), traffic (soot, Si/Al-rich, Fe-rich), heavy fuel oil combustion in heat plants or ships (S with V-Ni-Fe), LRT pollutants (S

Correlations between Optical, Chemical and Physical Properties ofBiomass Burn Aerosols

Energy Technology Data Exchange (ETDEWEB)

Hopkins, Rebecca J.; Lewis, K.; Desyaterik, Yury; Wang, Z.; Tivanski, Alexei V.; Arnott, W.P.; Laskin, Alexander; Gilles, M.K.

2008-01-29

Aerosols generated from burning different plant fuels were characterized to determine relationships between chemical, optical and physical properties. Single scattering albedo ({omega}) and Angstrom absorption coefficients ({alpha}{sub ap}) were measured using a photoacoustic technique combined with a reciprocal nephelometer. Carbon-to-oxygen atomic ratios, sp{sup 2} hybridization, elemental composition and morphology of individual particles were measured using scanning transmission X-ray microscopy coupled with near-edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS) and scanning electron microscopy with energy dispersion of X-rays (SEM/EDX). Particles were grouped into three categories based on sp2 hybridization and chemical composition. Measured {omega} (0.4-1.0 at 405 nm) and {alpha}{sub ap} (1.0-3.5) values displayed a fuel dependence. The category with sp{sup 2} hybridization >80% had values of {omega} (<0.5) and {alpha}{sub ap} ({approx}1.25) characteristic of light absorbing soot. Other categories with lower sp2 hybridization (20 to 60%) exhibited higher {omega} (>0.8) and {alpha}{sub ap} (1.0 to 3.5) values, indicating increased absorption spectral selectivity.

The physico-chemical evolution of atmospheric aerosols and the gas-particle partitioning of inorganic aerosol during KORUS-AQ

Science.gov (United States)

Lee, T.; Park, T.; Lee, J. B.; Lim, Y. J.; Ahn, J.; Park, J. S.; Soo, C. J.; Desyaterik, Y.; Collett, J. L., Jr.

2017-12-01

Aerosols influence climate change directly by scattering and absorption and indirectly by acting as cloud condensation nuclei and some of the effects of aerosols are reduction in visibility, deterioration of human health, and deposition of pollutants to ecosystems. Urban area is large source of aerosols and aerosol precursors. Aerosol sources are both local and from long-range transport. Long-range transport processed aerosol are often dominant sources of aerosol pollution in Korea. To improve our knowledge of aerosol chemistry, Korea and U.S-Air Quality (KORUS-AQ) of Aircraft-based aerosol measurement took place in and around Seoul, Korea during May and June 2016. KORUS-AQ campaigns were conducted to study the chemical characterization and processes of pollutants in the Seoul Metropolitan area to regional scales of Korean peninsula. Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed on aircraft platforms on-board DC-8 (NASA) aircraft. We characterized aerosol chemical properties and mass concentrations of sulfate, nitrate, ammonium and organics in polluted air plumes and investigate the spatial and vertical distribution of the species. The results of studies show that organics is predominant in Aerosol and a significant fraction of the organics is oxygenated organic aerosol (OOA) at the high altitude. Both Nitrate and sulfate can partition between the gas and particle phases. The ratios for HNO3/(N(V) (=gaseous HNO3 + particulate Nitrate) and SO2/(SO2+Sulfate) were found to exhibit quite different distributions between the particles and gas phase for the locations during KORUS-AQ campaign, representing potential for formation of additional particulate nitrate and sulfate. The results of those studies can provide highly resolved temporal and spatial air pollutant, which are valuable for air quality model input parameters for aerosol behaviour.

Fourteen months of on-line measurements of the non-refractory submicron aerosol at the Jungfraujoch (3580 m a.s.l.) - chemical composition, origins and organic aerosol sources

Science.gov (United States)

Fröhlich, R.; Cubison, M. J.; Slowik, J. G.; Bukowiecki, N.; Canonaco, F.; Croteau, P. L.; Gysel, M.; Henne, S.; Herrmann, E.; Jayne, J. T.; Steinbacher, M.; Worsnop, D. R.; Baltensperger, U.; Prévôt, A. S. H.

2015-10-01

Chemically resolved (organic, nitrate, sulfate, ammonium) data of non-refractory submicron (NR-PM1) aerosol from the first long-term deployment (27 July 2012 to 02 October 2013) of a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) at the Swiss high-altitude site Jungfraujoch (JFJ; 3580 m a.s.l.) are presented. Besides total mass loadings, diurnal variations and relative species contributions during the different meteorological seasons, geographical origin and sources of organic aerosol (OA) are discussed. Backward transport simulations show that the highest (especially sulfate) concentrations of NR-PM1 were measured in air masses advected to the station from regions south of the JFJ, while lowest concentrations were seen from western regions. OA source apportionment for each season was performed using the Source Finder (SoFi) interface for the multilinear engine (ME-2). OA was dominated in all seasons by oxygenated OA (OOA, 71-88 %), with lesser contributions from local tourism-related activities (7-12 %) and hydrocarbon-like OA related to regional vertical transport (3-9 %). In summer the OOA can be separated into a background low-volatility OA (LV-OOA I, possibly associated with long-range transport) and a slightly less oxidised low-volatility OA (LV-OOA II) associated with regional vertical transport. Wood burning-related OA associated with regional transport was detected during the whole winter 2012/2013 and during rare events in summer 2013, in the latter case attributed to small-scale transport for the surrounding valleys. Additionally, the data were divided into periods with free tropospheric (FT) conditions and periods with planetary boundary layer (PBL) influence, enabling the assessment of the composition for each. Most nitrate and part of the OA are injected from the regional PBL, while sulfate is mainly produced in the FT. The south/north gradient of sulfate is also pronounced in FT air masses (sulfate mass fraction from the south: 45

Sources and composition of submicron organic mass in marine aerosol particles

Science.gov (United States)

Frossard, Amanda A.; Russell, Lynn M.; Burrows, Susannah M.; Elliott, Scott M.; Bates, Timothy S.; Quinn, Patricia K.

2014-11-01

The sources and composition of atmospheric marine aerosol particles (aMA) have been investigated with a range of physical and chemical measurements from open-ocean research cruises. This study uses the characteristic functional group composition (from Fourier transform infrared spectroscopy) of aMA from five ocean regions to show the following: (i) The organic functional group composition of aMA that can be identified as mainly atmospheric primary marine (ocean derived) aerosol particles (aPMA) is 65 ± 12% hydroxyl, 21 ± 9% alkane, 6 ± 6% amine, and 7 ± 8% carboxylic acid functional groups. Contributions from photochemical reactions add carboxylic acid groups (15%-25%), shipping effluent in seawater and ship emissions add additional alkane groups (up to 70%), and coastal or continental emissions mix in alkane and carboxylic acid groups. (ii) The organic composition of aPMA is nearly identical to model-generated primary marine aerosol particles from bubbled seawater (gPMA, which has 55 ± 14% hydroxyl, 32 ± 14% alkane, and 13 ± 3% amine functional groups), indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. (iii) While the seawater organic functional group composition was nearly invariant across all three ocean regions studied and the ratio of organic carbon to sodium (OC/Na+) in the gPMA remained nearly constant over a broad range of chlorophyll a concentrations, the gPMA alkane group fraction appeared to increase with chlorophyll a concentrations (r = 0.66). gPMA from productive seawater had a larger fraction of alkane functional groups (42 ± 9%) compared to gPMA from nonproductive seawater (22 ± 10%), perhaps due to the presence of surfactants in productive seawater that stabilize the bubble film and lead to preferential drainage of the more soluble (lower alkane group fraction) organic components. gPMA has a hydroxyl group absorption peak location characteristic of

Aerosol composition and properties variation at the ground and over the column under different air masses advection in South Italy.

Science.gov (United States)

Pavese, G; Lettino, A; Calvello, M; Esposito, F; Fiore, S

2016-04-01

Aerosol composition and properties variation under the advection of different air masses were investigated, as case studies, by contemporary measurements over the atmospheric column and at the ground in a semi-rural site in South Italy. The absence of local strong sources in this area allowed to characterize background aerosol and to compare particle mixing effects under various atmospheric circulation conditions. Aerosol optical depth (AOD) and Ǻngström parameters from radiometric measurements allowed the detection and identification of polluted, dust, and volcanic atmospheric conditions. AODs were the input for a suitable model to evaluate the columnar aerosol composition, according to six main atmospheric components (water-soluble, soot, sea salt accumulation, sea salt coarse, mineral dus,t and biological). Scanning electron microscope (SEM) analysis of particulate sampled with a 13-stage impactor at the ground showed not only fingerprints typical of the different air masses but also the effects of transport and aging on atmospheric particles, suggesting processes that changed their chemical and optical properties. Background columnar aerosol was characterized by 72% of water-soluble and soot, in agreement with ground-based findings that highlighted 60% of contribution from anthropogenic carbonate particles and soot. In general, a good agreement between ground-based and columnar results was observed. Under the advection of trans-boundary air masses, water-soluble and soot were always present in columnar aerosol, whereas, in variable percentages, sea salt and mineral particles characterized both dust and volcanic conditions. At the ground, sulfates characterized the amorphous matrix produced in finer stages by the evaporation of solutions of organic and inorganic aerosols. Sulfates were also one of the key players involved in heterogeneous chemical reactions, producing complex secondary aerosol, as such clay-sulfate internally mixed particle externally mixed

A Study of Summer and Winter Highly Time-resolved Submicron Aerosol Composition Measured at a Suburban Site in Prague

Czech Academy of Sciences Publication Activity Database

Kubelová, Lucie; Vodička, Petr; Schwarz, Jaroslav; Cusack, Michael; Makeš, Otakar; Ondráček, Jakub; Ždímal, Vladimír

2015-01-01

Roč. 118, OCT 2015 (2015), s. 45-57 ISSN 1352-2310 R&D Projects: GA ČR GAP209/11/1342 Institutional support: RVO:67985858 Keywords : atmospheric aerosol * chemical composition * size distribution Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 3.459, year: 2015

The Effect of Aerosol Hygroscopicity and Volatility on Aerosol Optical Properties During Southern Oxidant and Aerosol Study

Science.gov (United States)

Khlystov, A.; Grieshop, A. P.; Saha, P.; Subramanian, R.

2014-12-01

Secondary organic aerosol (SOA) from biogenic sources can influence optical properties of ambient aerosol by altering its hygroscopicity and contributing to light absorption directly via formation of brown carbon and indirectly by enhancing light absorption by black carbon ("lensing effect"). The magnitude of these effects remains highly uncertain. A set of state-of-the-art instruments was deployed at the SEARCH site near Centerville, AL during the Southern Oxidant and Aerosol Study (SOAS) campaign in summer 2013 to measure the effect of relative humidity and temperature on aerosol size distribution, composition and optical properties. Light scattering and absorption by temperature- and humidity-conditioned aerosols was measured using three photo-acoustic extinctiometers (PAX) at three wavelengths (405 nm, 532 nm, and 870 nm). The sample-conditioning system provided measurements at ambient RH, 10%RH ("dry"), 85%RH ("wet"), and 200 C ("TD"). In parallel to these measurements, a long residence time temperature-stepping thermodenuder (TD) and a variable residence time constant temperature TD in combination with three SMPS systems and an Aerosol Chemical Speciation Monitor (ACSM) were used to assess aerosol volatility and kinetics of aerosol evaporation. We will present results of the on-going analysis of the collected data set. We will show that both temperature and relative humidity have a strong effect on aerosol optical properties. SOA appears to increase aerosol light absorption by about 10%. TD measurements suggest that aerosol equilibrated fairly quickly, within 2 s. Evaporation varied substantially with ambient aerosol loading and composition and meteorology.

Composite study of aerosol export events from East Asia and North America

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Y. Luan

2013-02-01

Full Text Available We use satellite observations of aerosol optical depth (AOD from the Moderate Resolution Imaging Spectrometer (MODIS together with the GEOS-Chem global chemical transport model to contrast export of aerosols from East Asia and North America during 2004–2010. The GEOS-Chem model reproduces the spatial distribution and temporal variations of Asian aerosol outflow generally well, although a low bias (−30% is found in the model fine mode AOD, particularly during summer. We use the model to identify 244 aerosol pollution export events from E. Asia and 251 export events from N. America over our 7-year study period. When these events are composited by season, we find that the AOD in the outflow is enhanced by 50–100% relative to seasonal mean values. The composite Asian plume splits into one branch going poleward to the Arctic in 3–4 days, with the other crossing the Pacific Ocean in 6–8 days. A fraction of the aerosols is trapped in the subtropical Pacific High during spring and summer. The N. American plume travels to the northeast Atlantic, reaching Europe after 4–5 days. Part of the composite plume turns anticyclonically in the Azores High, where it slowly decays. Both the Asian and N. American export events are favored by a dipole structure in sea-level pressure anomalies, associated with mid-latitude cyclone activity over the respective source regions. This dipole structure during outflow events is a strong feature for all seasons except summer, when convection becomes more important. The observed AOD in the E. Asian outflow exhibits stronger seasonality, with a spring maximum, than the N. American outflow, with a broad spring/summer maximum. The large spring AOD in the Asian outflow is the result of enhanced sulfate and dust aerosol concentrations, but is also due to a larger export efficiency of sulfate and SO₂ from the Asian boundary layer relative to the N. American boundary layer. While the N. American sulfate outflow

Chemical properties and morphology of Marine Aerosol in the Mediterranean atmosphere: a mesocosm study

Science.gov (United States)

D'Anna, Barbara; Sellegri, Karine; Charrière, Bruno; Sempéré, Richard; Mas, Sébastien; Marchand, Nicolas; George, Christian; Même, Aurèlie; R'mili, Badr; Delmont, Anne; Schwier, Allison; Rose, Clémence; Colomb, Aurèlie; Pey, Jorge; Langley Dewitt, Helen

2014-05-01

The Mediterranean Sea is a special marine environment characterized by low biological activity and high anthropogenic pressure. It is often difficult to discriminate the contribution of Primary Sea Salt Aerosol formed at the sea surface from background level of the aerosol. An alternative tool to study the sea-air exchanges in a controlled environment is provided by the mesocosms, which represent an important link between field studies and laboratory experiments. The sea-air transfer of particles and gases was investigated in relation to water chemical composition and biological activity during a mesocosm experiment within the SAM project (Sources of marine Aerosol in the Mediterranean) at the Oceanographic and Marine Station STARESO in Western Corsica (May 2013). Three 2 m mesocosms were filled with screened (sensors and received different treatments: one was left unchanged as control and two were enriched by addition of nitrates and phosphates respecting Redfield ratio (N:P = 16). The evolution of the three systems was followed for 20 days. The set of sensors in each mesocosm was allowed to monitor, at high frequency (every 10 min), the water temperature, conductivity, pH, incident light, fluorescence of chlorophyll a and dissolved oxygen concentration. The mesocosm seawaters were daily sampled for chemical (colored dissolved organic matter, particulate matter and related polar compounds, transparent polysaccharides and nutrients concentration) and biological (chlorophyll a, virus, phytoplankton and zooplankton) analyses. Both dissolved and gaseous VOCs were also analyzed. In addition, few liters of seawater from each mesocosm were daily and immediately collected and transferred to a bubble-bursting apparatus to simulate nascent sea spray aerosol. On-line chemical analysis of the sub-micrometer fraction was performed by a TOF-AMS (Aerodyne). Off-line analysis included TEM-EDX for morphology and size distribution studies and a hybrid quadrupole-orbitrap mass

Proof of the chemical composition of environmental aerosols with aid of spectroscopic methods and neutron activation

International Nuclear Information System (INIS)

Rettenmoser, T.

1999-01-01

Comparing the results obtained at the three sites, the following conclusions can be drawn: The total mass concentration is significantly enhanced in the city of Salzburg. Moreover, it is higher in the rural area than in the small town; this is caused by the existence of relatively large biogenic aerosols in ambient air. However, the mass concentration distribution is greater in the small town than in the countryside, because the above mentioned aerosols of biological origin may be too big to be registered by the used instruments. Here the biggest values were again found in the city. The total activity concentration is approximately the same in the city and the small town (provided that climatic conditions were similar). Unfortunately, no corresponding measurements were made in the rural area. The activity concentration distributions are again comparable in the city and the small town. In the rural area, on the other hand, the measured values are slightly higher due to geological reasons. Finally the particle concentration distributions are similar in the small town and the rural area, while the corresponding value is slightly higher in the city. It should be noted, however, that the measuring device used in this study is slightly inaccurate in the range of the small size fractions (which are of particular importance for anthropogenic aerosols). Because of the difficulties described in the measurement section, no comparison of the elemental composition of the ambient aerosols could be made. (author)

Aerosol chemistry in Titan's ionosphere: simultaneous growth and etching processes

Science.gov (United States)

Carrasco, Nathalie; Cernogora, Guy; Jomard, François; Etcheberry, Arnaud; Vigneron, Jackie

2016-10-01

Since the Cassini-CAPS measurements, organic aerosols are known to be present and formed at high altitudes in the diluted and partially ionized medium that is Titan's ionosphere [1]. This unexpected chemistry can be further investigated in the laboratory with plasma experiments simulating the complex ion-neutral chemistry starting from N2-CH4 [2]. Two sorts of solid organic samples can be produced in laboratory experiments simulating Titan's atmospheric reactivity: grains in the volume and thin films on the reactor walls. We expect that grains are more representative of Titan's atmospheric aerosols, but films are used to provide optical indices for radiative models of Titan's atmosphere.The aim of the present study is to address if these two sorts of analogues are chemically equivalent or not, when produced in the same N2-CH4 plasma discharge. The chemical compositions of both these materials are measured by using elemental analysis, XPS analysis and Secondary Ion Mass Spectrometry. We find that films are homogeneous but significantly less rich in nitrogen and hydrogen than grains produced in the same experimental conditions. This surprising difference in their chemical compositions is explained by the efficient etching occurring on the films, which stay in the discharge during the whole plasma duration, whereas the grains are ejected after a few minutes [3]. The impact for our understanding of Titan's aerosols chemical composition is important. Our study shows that chemical growth and etching process are simultaneously at stake in Titan's ionosphere. The more the aerosols stay in the ionosphere, the more graphitized they get through etching process. In order to infer Titan's aerosols composition, our work highlights a need for constraints on the residence time of aerosols in Titan's ionosphere. [1] Waite et al. (2009) Science , 316, p. 870[2] Szopa et al. (2006) PSS, 54, p. 394[3] Carrasco et al. (2016) PSS, 128, p. 52

COBRA: A Computational Brewing Application for Predicting the Molecular Composition of Organic Aerosols

Energy Technology Data Exchange (ETDEWEB)

Fooshee, David R.; Nguyen, Tran B.; Nizkorodov, Sergey A.; Laskin, Julia; Laskin, Alexander; Baldi, Pierre

2012-05-08

Atmospheric organic aerosols (OA) represent a significant fraction of airborne particulate matter and can impact climate, visibility, and human health. These mixtures are difficult to characterize experimentally due to the enormous complexity and dynamic nature of their chemical composition. We introduce a novel Computational Brewing Application (COBRA) and apply it to modeling oligomerization chemistry stemming from condensation and addition reactions of monomers pertinent to secondary organic aerosol (SOA) formed by photooxidation of isoprene. COBRA uses two lists as input: a list of chemical structures comprising the molecular starting pool, and a list of rules defining potential reactions between molecules. Reactions are performed iteratively, with products of all previous iterations serving as reactants for the next one. The simulation generated thousands of molecular structures in the mass range of 120-500 Da, and correctly predicted ~70% of the individual SOA constituents observed by high-resolution mass spectrometry (HR-MS). Selected predicted structures were confirmed with tandem mass spectrometry. Esterification and hemiacetal formation reactions were shown to play the most significant role in oligomer formation, whereas aldol condensation was shown to be insignificant. COBRA is not limited to atmospheric aerosol chemistry, but is broadly applicable to the prediction of reaction products in other complex mixtures for which reasonable reaction mechanisms and seed molecules can be supplied by experimental or theoretical methods.

A European Aerosol Phenomenology - 3: Physical and Chemical 2 Characteristics of Particulate Matter from 60 Rural, Urban, and Kerbside Sites Across Europe

Czech Academy of Sciences Publication Activity Database

Putaud, J.-P.; Van Dingenen, R.; Alastuey, A.; Bauer, H.; Birmili, W.; Cyrys, J.; Flentje, H.; Fuzzi, S.; Gehrig, R.; Harrison, R. M.; Hansson, H.C.; Herrmann, H.; Hitzenberger, R.; Hüglin, C.; Jones, A.M.; Kasper-Giebl, A.; Kiss, G.; Kousa, A.; Kuhlbusch, T.A.J.; Löschau, G.; Maenhaut, W.; Molnar, A.; Moreno, T.; Pekkanen, J.; Perrino, C.; Pitz, M.; Puxbaum, H.; Querol, X.; Rodriguez, S.; Salma, I.; Schwarz, Jaroslav; Smolík, Jiří; Schneider, J.; Spindler, G.; ten Brink, H.; Tursic, J.; Viana, M.; Wiedensohler, A.; Raes, F.

2010-01-01

Roč. 44, č. 10 (2010), s. 1308-1320 ISSN 1352-2310 Institutional research plan: CEZ:AV0Z40720504 Keywords : aerosol * chemical composition * number concentration Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 3.226, year: 2010

Role of organic aerosols in CCN activation and closure over a rural background site in Western Ghats, India

Science.gov (United States)

Singla, V.; Mukherjee, S.; Safai, P. D.; Meena, G. S.; Dani, K. K.; Pandithurai, G.

2017-06-01

The cloud condensation nuclei (CCN) closure study was performed to exemplify the effect of aerosol chemical composition on the CCN activity of aerosols at Mahabaleshwar, a high altitude background site in the Western Ghats, India. For this, collocated aerosol, CCN, Elemental Carbon (EC), Organic Carbon (OC), sub-micron aerosol chemical speciation for the period from 3rd June to 19th June 2015 was used. The chemical composition of non-refractory particulate matter (theory on the basis of measured aerosol particle number size distribution, size independent NR-PM1 chemical composition and calculated hygroscopicity. The CCN closure study was evaluated for 3 scenarios, B-I (all soluble inorganics), B-IO (all soluble organics and inorganics) and B-IOOA (all soluble inorganic and soluble oxygenated organic aerosol, OOA). OOA component was derived from the positive matrix factorization (PMF) analysis of organic aerosol mass spectra. Considering the bulk composition as internal mixture, CCN closure study was underestimated by 16-39% for B-I and overestimated by 47-62% for B-IO. The CCN closure result was appreciably improved for B-IOOA where the knowledge of OOA fraction was introduced and uncertainty reduced to within 8-10%.

Desorption atmospheric pressure photoionization high-resolution mass spectrometry: a complementary approach for the chemical analysis of atmospheric aerosols.

Science.gov (United States)

Parshintsev, Jevgeni; Vaikkinen, Anu; Lipponen, Katriina; Vrkoslav, Vladimir; Cvačka, Josef; Kostiainen, Risto; Kotiaho, Tapio; Hartonen, Kari; Riekkola, Marja-Liisa; Kauppila, Tiina J

2015-07-15

On-line chemical characterization methods of atmospheric aerosols are essential to increase our understanding of physicochemical processes in the atmosphere, and to study biosphere-atmosphere interactions. Several techniques, including aerosol mass spectrometry, are nowadays available, but they all suffer from some disadvantages. In this research, desorption atmospheric pressure photoionization high-resolution (Orbitrap) mass spectrometry (DAPPI-HRMS) is introduced as a complementary technique for the fast analysis of aerosol chemical composition without the need for sample preparation. Atmospheric aerosols from city air were collected on a filter, desorbed in a DAPPI source with a hot stream of toluene and nitrogen, and ionized using a vacuum ultraviolet lamp at atmospheric pressure. To study the applicability of the technique for ambient aerosol analysis, several samples were collected onto filters and analyzed, with the focus being on selected organic acids. To compare the DAPPI-HRMS data with results obtained by an established method, each filter sample was divided into two equal parts, and the second half of the filter was extracted and analyzed by liquid chromatography/mass spectrometry (LC/MS). The DAPPI results agreed with the measured aerosol particle number. In addition to the targeted acids, the LC/MS and DAPPI-HRMS methods were found to detect different compounds, thus providing complementary information about the aerosol samples. DAPPI-HRMS showed several important oxidation products of terpenes, and numerous compounds were tentatively identified. Thanks to the soft ionization, high mass resolution, fast analysis, simplicity and on-line applicability, the proposed methodology has high potential in the field of atmospheric research. Copyright © 2015 John Wiley & Sons, Ltd.

Aerosol composition and sources in the central Arctic Ocean during ASCOS

Science.gov (United States)

Chang, R. Y.-W.; Leck, C.; Graus, M.; Müller, M.; Paatero, J.; Burkhart, J. F.; Stohl, A.; Orr, L. H.; Hayden, K.; Li, S.-M.; Hansel, A.; Tjernström, M.; Leaitch, W. R.; Abbatt, J. P. D.

2011-10-01

Measurements of submicron aerosol chemical composition were made over the central Arctic Ocean from 5 August to 8 September 2008 as a part of the Arctic Summer Cloud Ocean Study (ASCOS) using an aerosol mass spectrometer (AMS). The median levels of sulphate and organics for the entire study were 0.051 and 0.055 μ g m-3, respectively. Positive matrix factorisation was performed on the entire mass spectral time series and this enabled marine biogenic and continental sources of particles to be separated. These factors accounted for 33% and 36% of the sampled ambient aerosol mass, respectively, and they were both predominantly composed of sulphate, with 47% of the sulphate apportioned to marine biogenic sources and 48% to continental sources, by mass. Within the marine biogenic factor, the ratio of methane sulphonate to sulphate was 0.25 ± 0.02, consistent with values reported in the literature. The organic component of the continental factor was more oxidised than that of the marine biogenic factor, suggesting that it had a longer photochemical lifetime than the organics in the marine biogenic factor. The remaining ambient aerosol mass was apportioned to an organic-rich factor that could have arisen from a combination of marine and continental sources. In particular, given that the factor does not correlate with common tracers of continental influence, we cannot rule out that the organic factor arises from a primary marine source.

Aged organic aerosol in the Eastern Mediterranean: the Finokalia Aerosol Measurement Experiment – 2008

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L. Hildebrandt

2010-05-01

Full Text Available Aged organic aerosol (OA was measured at a remote coastal site on the island of Crete, Greece during the Finokalia Aerosol Measurement Experiment-2008 (FAME-2008, which was part of the EUCAARI intensive campaign of May 2008. The site at Finokalia is influenced by air masses from different source regions, including long-range transport of pollution from continental Europe. A quadrupole aerosol mass spectrometer (Q-AMS was employed to measure the size-resolved chemical composition of non-refractory submicron aerosol (NR-PM₁, and to estimate the extent of oxidation of the organic aerosol. Factor analysis was used to gain insights into the processes and sources affecting the OA composition. The particles were internally mixed and liquid. The largest fraction of the dry NR-PM₁ sampled was ammonium sulfate and ammonium bisulfate, followed by organics and a small amount of nitrate. The variability in OA composition could be explained with two factors of oxygenated organic aerosol (OOA with differing extents of oxidation but similar volatility. Hydrocarbon-like organic aerosol (HOA was not detected. There was no statistically significant diurnal variation in the bulk composition of NR-PM₁ such as total sulfate or total organic aerosol concentrations. However, the OA composition exhibited statistically significant diurnal variation with more oxidized OA in the afternoon. The organic aerosol was highly oxidized, regardless of the source region. Total OA concentrations also varied little with source region, suggesting that local sources had only a small effect on OA concentrations measured at Finokalia. The aerosol was transported for about one day before arriving at the site, corresponding to an OH exposure of approximately 4×10¹¹ molecules cm⁻³ s. The constant extent of oxidation suggests that atmospheric aging results in a highly oxidized OA at these OH exposures, regardless of the aerosol source.

Aerosol volatility in a boreal forest environment

Science.gov (United States)

Häkkinen, S. A. K.; ńijälä, M.; Lehtipalo, K.; Junninen, H.; Virkkula, A.; Worsnop, D. R.; Kulmala, M.; Petäjä, T.; Riipinen, I.

2012-04-01

Climate and health effects of atmospheric aerosols are determined by their properties such as their chemical composition. Aerosol chemical composition can be studied indirectly by measuring volatility of aerosol particles. The volatility of submicron aerosol particles (20-500 nm) was studied in a boreal forest site at SMEAR II (Station for Measuring Ecosystem-Atmosphere Relations II) station (Vesala et al., 1998) in Hyytiälä, Finland, during 01/2008-05/2010. The instrument used for the measurements was VDMPS (Volatility Differential Mobility Particle Sizer), which consists of two separate instruments: DMPS (Differential Mobility Particle Sizer, Aalto et al., 2001) and TD (Thermodenuder, Wehner et al., 2002). Aerosol evaporation was examined by heating the aerosol and comparing the total aerosol mass before and after heating. In the VDMPS system ambient aerosol sample was heated up to temperatures ranging from 80 °C to 280 °C. The higher the heating temperature was the more aerosol material was evaporated. There was a non-volatile residual present in aerosol particles when heated up to 280 °C. This residual explained (20±8)% of the total aerosol mass. Aerosol non-volatile mass fraction was highest during winter and smallest during summer months. The role of black carbon in the observed non-volatile residual was determined. Black carbon explained 40 to 90% of the non-volatile mass. Especially during colder seasons noticeable amount of non-volatile material, something else than black carbon, was observed. According to Kalberer et al. (2004) some atmospheric organic species can form polymers that have high evaporation temperatures. Also low-volatile organic salts may contribute to the non-volatile aerosol (Smith et al., 2010). Aerosol mass composition measured directly with AMS (Aerosol Mass Spectrometer, Jayne et al., 2000) was analyzed in order to examine the properties of the non-volatile material (other than black carbon). The AMS measurements were performed

Secondary sulfate is internally mixed with sea spray aerosol and organic aerosol in the winter Arctic

Science.gov (United States)

Kirpes, Rachel M.; Bondy, Amy L.; Bonanno, Daniel; Moffet, Ryan C.; Wang, Bingbing; Laskin, Alexander; Ault, Andrew P.; Pratt, Kerri A.

2018-03-01

Few measurements of aerosol chemical composition have been made during the winter-spring transition (following polar sunrise) to constrain Arctic aerosol-cloud-climate feedbacks. Herein, we report the first measurements of individual particle chemical composition near Utqiaġvik (Barrow), Alaska, in winter (seven sample days in January and February 2014). Individual particles were analyzed by computer-controlled scanning electron microscopy with energy dispersive X-ray spectroscopy (CCSEM-EDX, 24 847 particles), Raman microspectroscopy (300 particles), and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS, 290 particles). Sea spray aerosol (SSA) was observed in all samples, with fresh and aged SSA comprising 99 %, by number, of 2.5-7.5 µm diameter particles, 65-95 % from 0.5-2.5 µm, and 50-60 % from 0.1-0.5 µm, indicating SSA is the dominant contributor to accumulation and coarse-mode aerosol during the winter. The aged SSA particles were characterized by reduced chlorine content with 94 %, by number, internally mixed with secondary sulfate (39 %, by number, internally mixed with both nitrate and sulfate), indicative of multiphase aging reactions during transport. There was a large number fraction (40 % of 1.0-4.0 µm diameter particles) of aged SSA during periods when particles were transported from near Prudhoe Bay, consistent with pollutant emissions from the oil fields participating in atmospheric processing of aerosol particles. Organic carbon and sulfate particles were observed in all samples and comprised 40-50 %, by number, of 0.1-0.4 µm diameter particles, indicative of Arctic haze influence. Soot was internally mixed with organic and sulfate components. All sulfate was mixed with organic carbon or SSA particles. Therefore, aerosol sources in the Alaskan Arctic and resulting aerosol chemical mixing states need to be considered when predicting aerosol climate effects, particularly cloud

Chemical characterisation of iron in dust and biomass burning aerosols during AMMA-SOP0/DABEX: implication for iron solubility

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R. Paris

2010-05-01

Full Text Available The chemical composition and the soluble fraction were determined in aerosol samples collected during flights of AMMA-SOP0/DABEX campaign, which were conducted in the West African Sahel during dry season (2006. Two aerosol types are encountered in this period: dust particles (DUST and biomass burning aerosol (BB. Chemical analysis and microscope observations showed that the iron (Fe found in BB samples mainly originates from dust particles mostly internally mixed in the biomass burning layer. Chemical analyses of samples showed that the Fe solubility is lower in African dust samples than in biomass burning aerosols. Our data provide a first idea of the variability of iron dust solubility in the source region (0.1% and 3.4%. We found a relationship between iron solubility/clay content/source which partly confirms that the variability of iron solubility in this source region is related to the character and origin of the aerosols themselves. In the biomass burning samples, no relationship were found between Fe solubility and either the concentrations of acidic species (SO₄²⁻, NO₃⁻ or oxalate or the content of carbon (TC, OC, BC. Therefore, we were unable to determine what processes are involved in this increase of iron solubility. In terms of supply of soluble Fe to oceanic ecosystems on a global scale, the higher solubility observed for Fe in biomass burning could imply an indirect source of Fe to marine ecosystems. But these aerosols are probably not significant because the Sahara is easily the dominant source of Fe to the Atlantic Ocean.

Multisensor analyzer detector (MSAD) for low cost chemical and aerosol detection and pattern fusion

Science.gov (United States)

Swanson, David C.; Merdes, Daniel W.; Lysak, Daniel B., Jr.; Curtis, Richard C.; Lang, Derek C.; Mazzara, Andrew F.; Nicholas, Nicholas C.

2002-08-01

MSAD is being developed as a low-cost point detection chemical and biological sensor system designed around an information fusion inference engine that also allows additional sensors to be included in the detection process. The MSAD concept is based on probable cause detection of hazardous chemical vapors and aerosols of either chemical or biological composition using a small portable unit containing an embedded computer system and several integrated sensors with complementary capabilities. The configuration currently envisioned includes a Surface-Enhanced Raman Spectroscopy (SERS) sensor of chemical vapors and a detector of respirable aerosols based on Fraunhofer diffraction. Additional sensors employing Ion Mobility Spectrometry (IMS), Surface Acoustic Wave (SAW) detection, Flame Photometric Detection (FPD), and other principles are candidates for integration into the device; also, available commercial detectors implementing IMS, SAW, and FPD will be made accessible to the unit through RS232 ports. Both feature and decision level information fusion is supported using a Continuous Inference Network (CINET) of fuzzy logic. Each class of agents has a unique CINET with information inputs from a number of available sensors. Missing or low confidence sensor information is gracefully blended out of the output confidence for the particular agent. This approach constitutes a plug and play arrangement between the sensors and the information pattern recognition algorithms. We are currently doing simulant testing and developing out CINETs for actual agent testing at Edgewood Chemical and Biological Center (ECBC) later this year.

Hygroscopic behavior and chemical composition evolution of internally mixed aerosols composed of oxalic acid and ammonium sulfate

Science.gov (United States)

Wang, Xiaowei; Jing, Bo; Tan, Fang; Ma, Jiabi; Zhang, Yunhong; Ge, Maofa

2017-10-01

Although water uptake of aerosol particles plays an important role in the atmospheric environment, the effects of interactions between components on chemical composition and hygroscopicity of particles are still not well constrained. The hygroscopic properties and phase transformation of oxalic acid (OA) and mixed particles composed of ammonium sulfate (AS) and OA with different organic to inorganic molar ratios (OIRs) have been investigated by using confocal Raman spectroscopy. It is found that OA droplets first crystallize to form OA dihydrate at 71 % relative humidity (RH), and further lose crystalline water to convert into anhydrous OA around 5 % RH during the dehydration process. The deliquescence and efflorescence point for AS is determined to be 80.1 ± 1.5 % RH and 44.3 ± 2.5 % RH, respectively. The observed efflorescence relative humidity (ERH) for mixed OA / AS droplets with OIRs of 1 : 3, 1 : 1 and 3 : 1 is 34.4 ± 2.0, 44.3 ± 2.5 and 64.4 ± 3.0 % RH, respectively, indicating the elevated OA content appears to favor the crystallization of mixed systems at higher RH. However, the deliquescence relative humidity (DRH) of AS in mixed OA / AS particles with OIRs of 1 : 3 and 1 : 1 is observed to occur at 81.1 ± 1.5 and 77 ± 1.0 % RH, respectively. The Raman spectra of mixed OA / AS droplets indicate the formation of ammonium hydrogen oxalate (NH4HC2O4) and ammonium hydrogen sulfate (NH4HSO4) from interactions between OA and AS in aerosols during the dehydration process on the time scale of hours, which considerably influence the subsequent deliquescence behavior of internally mixed particles with different OIRs. The mixed OA / AS particles with an OIR of 3 : 1 exhibit no deliquescence transition over the RH range studied due to the considerable transformation of (NH4)2SO4 into NH4HC2O4 with a high DRH. Although the hygroscopic growth of mixed OA / AS droplets is comparable to that of AS or OA at high RH during the dehydration process, Raman growth

Microbiology and atmospheric processes: biological, physical and chemical characterization of aerosol particles

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D. G. Georgakopoulos

2009-04-01

Full Text Available The interest in bioaerosols has traditionally been linked to health hazards for humans, animals and plants. However, several components of bioaerosols exhibit physical properties of great significance for cloud processes, such as ice nucleation and cloud condensation. To gain a better understanding of their influence on climate, it is therefore important to determine the composition, concentration, seasonal fluctuation, regional diversity and evolution of bioaerosols. In this paper, we will review briefly the existing techniques for detection, quantification, physical and chemical analysis of biological particles, attempting to bridge physical, chemical and biological methods for analysis of biological particles and integrate them with aerosol sampling techniques. We will also explore some emerging spectroscopy techniques for bulk and single-particle analysis that have potential for in-situ physical and chemical analysis. Lastly, we will outline open questions and further desired capabilities (e.g., in-situ, sensitive, both broad and selective, on-line, time-resolved, rapid, versatile, cost-effective techniques required prior to comprehensive understanding of chemical and physical characterization of bioaerosols.

Laboratory studies of the chemical composition and cloud condensation nuclei (CCN activity of secondary organic aerosol (SOA and oxidized primary organic aerosol (OPOA

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A. T. Lambe

2011-09-01

Full Text Available Secondary organic aerosol (SOA and oxidized primary organic aerosol (OPOA were produced in laboratory experiments from the oxidation of fourteen precursors representing atmospherically relevant biogenic and anthropogenic sources. The SOA and OPOA particles were generated via controlled exposure of precursors to OH radicals and/or O₃ in a Potential Aerosol Mass (PAM flow reactor over timescales equivalent to 1–20 days of atmospheric aging. Aerosol mass spectra of SOA and OPOA were measured with an Aerodyne aerosol mass spectrometer (AMS. The fraction of AMS signal at m/z = 43 and m/z = 44 (f₄₃, f₄₄, the hydrogen-to-carbon (H/C ratio, and the oxygen-to-carbon (O/C ratio of the SOA and OPOA were obtained, which are commonly used to characterize the level of oxidation of oxygenated organic aerosol (OOA. The results show that PAM-generated SOA and OPOA can reproduce and extend the observed f₄₄–f₄₃ composition beyond that of ambient OOA as measured by an AMS. Van Krevelen diagrams showing H/C ratio as a function of O/C ratio suggest an oxidation mechanism involving formation of carboxylic acids concurrent with fragmentation of carbon-carbon bonds. Cloud condensation nuclei (CCN activity of PAM-generated SOA and OPOA was measured as a function of OH exposure and characterized as a function of O/C ratio. CCN activity of the SOA and OPOA, which was characterized in the form of the hygroscopicity parameter κ_org, ranged from 8.4×10⁻⁴ to 0.28 over measured O/C ratios ranging from 0.05 to 1.42. This range of κ_org and O/C ratio is significantly wider than has been previously obtained. To first order, the κ_org-to-O/C relationship is well represented by a linear function of the form κ_org = (0.18±0.04 ×O/C + 0.03, suggesting that a simple, semi-empirical parameterization of OOA hygroscopicity and

Nuclear magnetic resonance spectroscopy for determining the functional content of organic aerosols: A review

International Nuclear Information System (INIS)

Chalbot, Marie-Cecile G.; Kavouras, Ilias G.

2014-01-01

The knowledge deficit of organic aerosol (OA) composition has been identified as the most important factor limiting our understanding of the atmospheric fate and implications of aerosol. The efforts to chemically characterize OA include the increasing utilization of nuclear magnetic resonance spectroscopy (NMR). Since 1998, the functional composition of different types, sizes and fractions of OA has been studied with one-dimensional, two-dimensional and solid state proton and carbon-13 NMR. This led to the use of functional group ratios to reconcile the most important sources of OA, including secondary organic aerosol and initial source apportionment using positive matrix factorization. Future research efforts may be directed towards the optimization of experimental parameters, detailed NMR experiments and analysis by pattern recognition methods to identify the chemical components, determination of the NMR fingerprints of OA sources and solid state NMR to study the content of OA as a whole. - Highlights: • Organic aerosol composition by 1 H- and 13 C-NMR spectroscopy. • NMR fingerprints of specific sources, types and sizes of organic aerosol. • Source reconciliation and apportionment using NMR spectroscopy. • Research priorities towards understanding organic aerosol composition and origin. - This review presents the recent advances on the characterization of organic aerosol composition using nuclear magnetic resonance spectroscopy

Eddy covariance measurements with high-resolution time-of-flight aerosol mass spectrometry: a new approach to chemically resolved aerosol fluxes

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D. K. Farmer

2011-06-01

Full Text Available Although laboratory studies show that biogenic volatile organic compounds (VOCs yield substantial secondary organic aerosol (SOA, production of biogenic SOA as indicated by upward fluxes has not been conclusively observed over forests. Further, while aerosols are known to deposit to surfaces, few techniques exist to provide chemically-resolved particle deposition fluxes. To better constrain aerosol sources and sinks, we have developed a new technique to directly measure fluxes of chemically-resolved submicron aerosols using the high-resolution time-of-flight aerosol mass spectrometer (HR-AMS in a new, fast eddy covariance mode. This approach takes advantage of the instrument's ability to quantitatively identify both organic and inorganic components, including ammonium, sulphate and nitrate, at a temporal resolution of several Hz. The new approach has been successfully deployed over a temperate ponderosa pine plantation in California during the BEARPEX-2007 campaign, providing both total and chemically resolved non-refractory (NR PM₁ fluxes. Average deposition velocities for total NR-PM₁ aerosol at noon were 2.05 ± 0.04 mm s⁻¹. Using a high resolution measurement of the NH₂⁺ and NH₃⁺ fragments, we demonstrate the first eddy covariance flux measurements of particulate ammonium, which show a noon-time deposition velocity of 1.9 ± 0.7 mm s⁻¹ and are dominated by deposition of ammonium sulphate.

Molecular corridors and parameterizations of volatility in the chemical evolution of organic aerosols

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Y. Li

2016-03-01

Full Text Available The formation and aging of organic aerosols (OA proceed through multiple steps of chemical reaction and mass transport in the gas and particle phases, which is challenging for the interpretation of field measurements and laboratory experiments as well as accurate representation of OA evolution in atmospheric aerosol models. Based on data from over 30 000 compounds, we show that organic compounds with a wide variety of functional groups fall into molecular corridors, characterized by a tight inverse correlation between molar mass and volatility. We developed parameterizations to predict the saturation mass concentration of organic compounds containing oxygen, nitrogen, and sulfur from the elemental composition that can be measured by soft-ionization high-resolution mass spectrometry. Field measurement data from new particle formation events, biomass burning, cloud/fog processing, and indoor environments were mapped into molecular corridors to characterize the chemical nature of the observed OA components. We found that less-oxidized indoor OA are constrained to a corridor of low molar mass and high volatility, whereas highly oxygenated compounds in atmospheric water extend to high molar mass and low volatility. Among the nitrogen- and sulfur-containing compounds identified in atmospheric aerosols, amines tend to exhibit low molar mass and high volatility, whereas organonitrates and organosulfates follow high O : C corridors extending to high molar mass and low volatility. We suggest that the consideration of molar mass and molecular corridors can help to constrain volatility and particle-phase state in the modeling of OA particularly for nitrogen- and sulfur-containing compounds.

Arctic Aerosols and Sources

DEFF Research Database (Denmark)

Nielsen, Ingeborg Elbæk

2017-01-01

Since the Industrial Revolution, the anthropogenic emission of greenhouse gases has been increasing, leading to a rise in the global temperature. Particularly in the Arctic, climate change is having serious impact where the average temperature has increased almost twice as much as the global during......, ammonium, black carbon, and trace metals. This PhD dissertation studies Arctic aerosols and their sources, with special focus on black carbon, attempting to increase the knowledge about aerosols’ effect on the climate in an Arctic content. The first part of the dissertation examines the diversity...... of aerosol emissions from an important anthropogenic aerosol source: residential wood combustion. The second part, characterizes the chemical and physical composition of aerosols while investigating sources of aerosols in the Arctic. The main instrument used in this research has been the state...

Comparison of three aerosol chemical characterization techniques utilizing PTR-ToF-MS: a study on freshly formed and aged biogenic SOA

Science.gov (United States)

Gkatzelis, Georgios I.; Tillmann, Ralf; Hohaus, Thorsten; Müller, Markus; Eichler, Philipp; Xu, Kang-Ming; Schlag, Patrick; Schmitt, Sebastian H.; Wegener, Robert; Kaminski, Martin; Holzinger, Rupert; Wisthaler, Armin; Kiendler-Scharr, Astrid

2018-03-01

An intercomparison of different aerosol chemical characterization techniques has been performed as part of a chamber study of biogenic secondary organic aerosol (BSOA) formation and aging at the atmosphere simulation chamber SAPHIR (Simulation of Atmospheric PHotochemistry In a large Reaction chamber). Three different aerosol sampling techniques - the aerosol collection module (ACM), the chemical analysis of aerosol online (CHARON) and the collection thermal-desorption unit (TD) were connected to proton transfer reaction time-of-flight mass spectrometers (PTR-ToF-MSs) to provide chemical characterization of the SOA. The techniques were compared among each other and to results from an aerosol mass spectrometer (AMS) and a scanning mobility particle sizer (SMPS). The experiments investigated SOA formation from the ozonolysis of β-pinene, limonene, a β-pinene-limonene mix and real plant emissions from Pinus sylvestris L. (Scots pine). The SOA was subsequently aged by photo-oxidation, except for limonene SOA, which was aged by NO3 oxidation. Despite significant differences in the aerosol collection and desorption methods of the PTR-based techniques, the determined chemical composition, i.e. the same major contributing signals, was found by all instruments for the different chemical systems studied. These signals could be attributed to known products expected from the oxidation of the examined monoterpenes. The sampling and desorption method of ACM and TD provided additional information on the volatility of individual compounds and showed relatively good agreement. Averaged over all experiments, the total aerosol mass recovery compared to an SMPS varied within 80 ± 10, 51 ± 5 and 27 ± 3 % for CHARON, ACM and TD, respectively. Comparison to the oxygen-to-carbon ratios (O : C) obtained by AMS showed that all PTR-based techniques observed lower O : C ratios, indicating a loss of molecular oxygen either during aerosol sampling or detection. The differences in total

Urban aerosol in Oporto, Portugal: Chemical characterization of PM10 and PM2.5

Science.gov (United States)

Custódio, Danilo; Ferreira, Catarina; Alves, Célia; Duarte, Mácio; Nunes, Teresa; Cerqueira, Mário; Pio, Casimiro; Frosini, Daniele; Colombi, Cristina; Gianelle, Vorne; Karanasiou, Angeliki; Querol, Xavier

2014-05-01

Several urban and industrial areas in Southern Europe are not capable of meeting the implemented EU standards for particulate matter. Efficient air quality management is required in order to ensure that the legal limits are not exceeded and that the consequences of poor air quality are controlled and minimized. Many aspects of the direct and indirect effects of suspended particulate matter on climate and public health are not well understood. The temporal variation of the chemical composition is still demanded, since it enables to adopt off-set strategies and to better estimate the magnitude of anthropogenic forcing on climate. This study aims to provide detailed information on concentrations and chemical composition of aerosol from Oporto city, an urban center in Southern Europe. This city is located near the coast line in the North of Portugal, being the country's second largest urban area. Moreover, Oporto city economic prospects depend heavily on a diversified industrial park, which contribute to air quality degradation. Another strong source of air pollution is traffic. The main objectives of this study are: 1) to characterize the chemical composition of PM10 and PM2.5 by setting up an orchestra of aerosol sampling devices in a strategic place in Oporto; 2) to identify the sources of particles exploring parameters such as organic and inorganic markers (e.g. sugars as tracers for biomass burning; metals and elemental carbon for industrial and vehicular emissions); 3) to evaluate long range transport of pollutants using back trajectory analysis. Here we present data obtained between January 2013 and January 2014 in a heavy traffic roadside sampling site located in the city center. Different PM10 and PM2.5 samplers were operated simultaneously in order to collect enough mass on different filter matrixes and to fulfill the requirements of analytical methodologies. More than 100 aerosol samples were collected and then analysed for their mass concentration and

Sources and atmospheric processing of organic aerosol in the Mediterranean: insights from aerosol mass spectrometer factor analysis

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L. Hildebrandt

2011-12-01

Full Text Available Atmospheric particles were measured in the late winter (25 February–26 March 2009 at a remote coastal site on the island of Crete, Greece during the Finokalia Aerosol Measurement Experiment-2009. A quadrupole aerosol mass spectrometer (Q-AMS was employed to quantify the size-resolved chemical composition of non-refractory submicron aerosol, and a thermodenuder was used to analyze the organic aerosol (OA volatility. Complementary measurements included particle size distributions from a scanning mobility particle sizer, inorganic and organic particle composition from filter analysis, air ion concentrations, O₃, NO_x and NO_y concentrations, and meteorological measurements. Factor analysis was performed on the OA mass spectra, and the variability in OA composition could best be explained with three OA components. The oxygenated organic aerosol (OOA was similar in composition and volatility to the summertime OA previously measured at this site and may represent an effective endpoint in particle-phase oxidation of organics. The two other OA components, one associated with amines (Amine-OA and the other probably associated with the burning of olive branches (OB-OA, had very low volatility but were less oxygenated. Hydrocarbon-like organic aerosol (HOA was not detected. The absence of OB-OA and Amine-OA in the summer data may be due to lower emissions and/or photochemical conversion of these components to OOA.

Aircraft-Based measurement of the physico-chemical evolution of atmospheric aerosols in the air pollution plume over a megacity and a remote area

Science.gov (United States)

Park, J. S.; Lee, T.; Park, T.; Lee, J. B.; Lim, Y. J.; Ahn, J.; Kim, J.; Park, S.; Collett, J. L., Jr.

2017-12-01

Aerosols influence climate change directly (scattering and absorption) and indirectly (cloud condensation nuclei), also adverse health effects. The Korean peninsula is a great place to study different sources of the aerosols: urban, rural and marine. In addition, Seoul is one of the large metropolitan areas in the world and has a variety of sources because half of the Korean population lives in Seoul, which comprises only 12% of the country's area. To understand the physico-chemical evolution of atmospheric aerosols in the air pollution plume over a megacity and a remote area, an Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed on an airborne platform (NASA DC-8 and Beechcraft King Air) in June, 2015 and May-June, 2016 during MAPS-Seoul and KORUS-AQ campaigns, respectively, in Korea. The HR-ToF-AMS is capable of measuring non-refractory size resolved chemical composition of submicron particle (NR-PM1). NR-PM1 includes mass concentration of organics, nitrate, sulfate, and ammonium with 10 seconds time resolution. Organics was dominated species in aerosol during all of flights. Organics and nitrate were dominant around energy industrial complex near by Taean, South Korea. The presentation will provide an overview of the composition of NR-PM1 measured in air pollution plumes, and deliver detail information about width, depth and spatial distribution of the pollutant in the air pollution plumes. The results of this study will provide high temporal and spatial resolved details on the air pollution plumes, which are valuable input parameters of aerosol properties for the current air quality models.

Effect of humidity on the composition of isoprene photooxidation secondary organic aerosol

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T. B. Nguyen

2011-07-01

Full Text Available The effect of relative humidity (RH on the composition and concentrations of gas-phase products and secondary organic aerosol (SOA generated from the photooxidation of isoprene under high-NO_x conditions was investigated. Experiments were performed with hydrogen peroxide as the OH precursor and in the absence of seed aerosol. The relative yields of most gas-phase products were the same regardless of initial water vapor concentration with exception of hydroxyacetone and glycolaldehyde, which were considerably affected by RH. A significant change was observed in the SOA composition, with many unique condensed-phase products formed under humid (90 % RH vs. dry (<2 % RH conditions, without any detectable effect on the rate and extent of the SOA mass growth. There is a 40 % reduction in the number and relative abundance of distinct particle-phase nitrogen-containing organic compounds (NOC detected by high resolution mass spectrometry. The suppression of condensation reactions, which produce water as a product, is the most important chemical effect of the increased RH. For example, the total signal from oligomeric esters of 2-methylglyceric acid was reduced by about 60 % under humid conditions and the maximum oligomer chain lengths were reduced by 7–11 carbons. Oligomers formed by addition mechanisms, without direct involvement of water, also decreased at elevated RH but to a much smaller extent. The observed reduction in the extent of condensation-type oligomerization at high RH may have substantial impact on the phase characteristics and hygroscopicity of the isoprene aerosol. The reduction in the amount of organic nitrates in the particle phase has implications for understanding the budget of NOC compounds.

The effect of meteorological and chemical factors on the agreement between observations and predictions of fine aerosol composition in southwestern Ontario during BAQS-Met

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M. Z. Markovic

2011-04-01

Full Text Available The Border Air Quality and Meteorology Study (BAQS-Met was an intensive, collaborative field campaign during the summer of 2007 that investigated the effects of transboundary pollution, local pollution, and local meteorology on air quality in southwestern Ontario. This analysis focuses on the measurements of the inorganic constituents of particulate matter with diameter of less than 1 μm (PM₁, with a specific emphasis on nitrate. We evaluate the ability of AURAMS, Environment Canada's chemical transport model, to represent regional air pollution in SW Ontario by comparing modelled aerosol inorganic chemical composition with measurements from Aerosol Mass Spectrometers (AMS onboard the National Research Council (NRC of Canada Twin Otter aircraft and at a ground site in Harrow, ON. The agreement between modelled and measured pNO₃⁻ at the ground site (observed mean (M_obs = 0.50 μg m⁻³; modelled mean (M_mod = 0.58 μg m⁻³; root mean square error (RSME = 1.27 μg m⁻³ was better than aloft (M_obs = 0.32 μg m⁻³; M_mod = 0.09 μg m⁻³; RSME = 0.48 μg m⁻³. Possible reasons for discrepancies include errors in (i emission inventories, (ii atmospheric chemistry, (iii predicted meteorological parameters, or (iv gas/particle thermodynamics in the model framework. Using the inorganic thermodynamics model, ISORROPIA, in an offline mode, we find that the assumption of thermodynamic equilibrium is consistent with observations of gas and particle composition at Harrow. We develop a framework to assess the sensitivity of PM₁ nitrate to meteorological and chemical parameters and find that errors in both the predictions of relative humidity and free ammonia (FA ≡ NH_3(g + pNH₄⁺ − 2 · pSO₄^2- are responsible for

Microbiology and atmospheric processes: chemical interactions of primary biological aerosols

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L. Deguillaume

2008-07-01

Full Text Available This paper discusses the influence of primary biological aerosols (PBA on atmospheric chemistry and vice versa through microbiological and chemical properties and processes. Several studies have shown that PBA represent a significant fraction of air particulate matter and hence affect the microstructure and water uptake of aerosol particles. Moreover, airborne micro-organisms, namely fungal spores and bacteria, can transform chemical constituents of the atmosphere by metabolic activity. Recent studies have emphasized the viability of bacteria and metabolic degradation of organic substances in cloud water. On the other hand, the viability and metabolic activity of airborne micro-organisms depend strongly on physical and chemical atmospheric parameters such as temperature, pressure, radiation, pH value and nutrient concentrations. In spite of recent advances, however, our knowledge of the microbiological and chemical interactions of PBA in the atmosphere is rather limited. Further targeted investigations combining laboratory experiments, field measurements, and modelling studies will be required to characterize the chemical feedbacks, microbiological activities at the air/snow/water interface supplied to the atmosphere.

Organics, Meteoritic Material, and other Elements in High Altitude Aerosols

Science.gov (United States)

Mahoney, M.; Murphy, D. M.; Thomson, D. S.

1998-01-01

Recent in situ measurements of the chemical composition of single aerosol particles at altitudes up to 19 km have revealed a number of surprising features about ambient particles. Upper tropospheric aerosols in the study region often contained more organic material than sulfate.

New trajectory-driven aerosol and chemical process model Chemical and Aerosol Lagrangian Model (CALM

Directory of Open Access Journals (Sweden)

P. Tunved

2010-11-01

Full Text Available A new Chemical and Aerosol Lagrangian Model (CALM has been developed and tested. The model incorporates all central aerosol dynamical processes, from nucleation, condensation, coagulation and deposition to cloud formation and in-cloud processing. The model is tested and evaluated against observations performed at the SMEAR II station located at Hyytiälä (61° 51' N, 24° 17' E over a time period of two years, 2000–2001. The model shows good agreement with measurements throughout most of the year, but fails in reproducing the aerosol properties during the winter season, resulting in poor agreement between model and measurements especially during December–January. Nevertheless, through the rest of the year both trends and magnitude of modal concentrations show good agreement with observation, as do the monthly average size distribution properties. The model is also shown to capture individual nucleation events to a certain degree. This indicates that nucleation largely is controlled by the availability of nucleating material (as prescribed by the [H₂SO₄], availability of condensing material (in this model 15% of primary reactions of monoterpenes (MT are assumed to produce low volatile species and the properties of the size distribution (more specifically, the condensation sink. This is further demonstrated by the fact that the model captures the annual trend in nuclei mode concentration. The model is also used, alongside sensitivity tests, to examine which processes dominate the aerosol size distribution physical properties. It is shown, in agreement with previous studies, that nucleation governs the number concentration during transport from clean areas. It is also shown that primary number emissions almost exclusively govern the CN concentration when air from Central Europe is advected north over Scandinavia. We also show that biogenic emissions have a large influence on the amount of potential CCN observed

Ambient Aerosol in Southeast Asia: High Resolution Aerosol Mass Spectrometer Measurements Over Oil Palm (Elaeis guineensis)

Science.gov (United States)

Phillips, G.; Dimarco, C.; Misztal, P.; Nemitz, E.; Farmer, D.; Kimmel, J.; Jimenez, J.

2008-12-01

The emission of organic compounds in the troposphere is important factor in the formation of secondary organic aerosol (SOA). A very large proportion of organic material emitted globally is estimated to arise from biogenic sources, with almost half coming from tropical and sub-tropical forests. Preliminary analyses of leave cuvette emission studies suggest that oil palm (Elaeis guineensis) is a significantly larger source of isoprene than tropical forest. Much larger sources of isoprene over oil palm allied with a larger anthropogenic component of local emissions contrast greatly with the remote tropical forest environment and therefore the character of SOA formed may differ significantly. These issues, allied with the high price of palm oil on international markets leading to increased use of land for oil palm production, could give rise to rapidly changing chemical and aerosol regimes in the tropics. It is therefore important to understand the current emissions and composition of organic aerosol over all important land-uses in the tropical environment. This in turn will lead to a greater understanding of the present, and to an improvement in predictive capacity for the future system. To help address these issues, a high resolution time of flight aerosol mass spectrometer (HR-ToF-AMS) was deployed in the Sabahmas (PPB OIL) oil palm plantation near Lahad Datu, in Eastern Sabah, as part of the field component of the Aerosol Coupling in the Earth System (ACES) project, part of the UK NERC APPRAISE program. This project was allied closely with measurements made of similar chemical species and aerosol components at a forest site in the Danum Valley as part of the UK Oxidant and Particle Photochemical Processes above a Southeast Asian tropical rainforest (OP3) project. Measurements of submicron non- refractory aerosol composition are presented along with some preliminary analysis of chemically resolved aerosol fluxes made with a new eddy covariance system, based on the

Aerosol composition and source apportionment in Santiago de Chile

Science.gov (United States)

Artaxo, Paulo; Oyola, Pedro; Martinez, Roberto

1999-04-01

Santiago de Chile, São Paulo and Mexico City are Latin American urban areas that suffer from heavy air pollution. In order to study air pollution in Santiago area, an aerosol source apportionment study was designed to measure ambient aerosol composition and size distribution for two downtown sampling sites in Santiago. The aerosol monitoring stations were operated in Gotuzo and Las Condes during July and August 1996. The study employed stacked filter units (SFU) for aerosol sampling, collecting fine mode aerosol (dpsource apportionment was performed using Absolute Principal Factor Analysis (APFA). Very high aerosol concentrations were observed (up to 400 μg/m 3 PM 10). The main aerosol particle sources in Santiago are resuspended soil dust and traffic emissions. Coarse particles account for 63% of PM 10 aerosol in Gotuzo and 53% in Las Condes. A major part of this component is resuspended soil dust. In the fine fraction, resuspended soil dust accounts for 15% of fine mass, and the aerosols associated with transportation activities account for a high 64% of the fine particle mass. Sulfate particle is an important component of the aerosol in Santiago, mainly originating from gas-to-particle conversion from SO 2. In the Gotuzo site, sulfates are the highest aerosol component, accounting for 64.5% of fine mass. Direct traffic emissions are generally mixed with resuspended soil dust. It is difficult to separate the two components, because the soil dust in downtown Santiago is contaminated with Pb, Br, Cl, and other heavy metals that are also tracers for traffic emissions. Residual oil combustion is observed, with the presence of V, S and Ni. An aerosol components from industrial emissions is also present, with the presence of several heavy metals such as Zn, Cu and others. A factor with molybdenum, arsenic, copper and sulfur was observed frequently, and it results from emissions of copper smelters.

Glyoxal contribution to aerosols over Los Angeles

Science.gov (United States)

Balcerak, Ernie

2012-01-01

Laboratory and field studies have indicated that glyoxal (chemical formula OCHCHO), an atmospheric oxidation product of isoprene and aromatic compounds, may contribute to secondary organic aerosols in the atmosphere, which can block sunlight and affect atmospheric chemistry. Some aerosols are primary aerosols, emitted directly into the atmosphere, while others are secondary, formed through chemical reactions in the atmosphere. Washenfelder et al. describe in situ glyoxal measurements from Pasadena, Calif., near Los Angeles, made during summer 2010. They used three different methods to calculate the contribution of glyoxal to secondary atmospheric aerosol and found that it is responsible for 0-0.2 microgram per cubic meter, or 0-4%, of the secondary organic aerosol mass. The researchers also compared their results to those of a previous study that calculated the glyoxal contribution to aerosol for Mexico City. Mexico City had higher levels of organic aerosol mass from glyoxal. They suggest that the lower contribution of glyoxal to aerosol concentrations for Los Angeles may be due to differences in the composition or water content of the aerosols above the two cities. (Journal of Geophysical Research-Atmospheres, doi:10.1029/2011JD016314, 2011)

The continuous field measurements of soluble aerosol compositions at the Taipei Aerosol Supersite, Taiwan

Science.gov (United States)

Chang, Shih-Yu; Lee, Chung-Te; Chou, Charles C.-K.; Liu, Shaw-Chen; Wen, Tian-Xue

The characteristics of ambient aerosols, affected by solar radiation, relative humidity, wind speed, wind direction, and gas-aerosol interaction, changed rapidly at different spatial and temporal scales. In Taipei Basin, dense traffic emissions and sufficient solar radiation for typical summer days favored the formation of secondary aerosols. In winter, the air quality in Taipei Basin was usually affected by the Asian continental outflows due to the long-range transport of pollutants carried by the winter monsoon. The conventional filter-based method needs a long time for collecting aerosols and analyzing compositions, which cannot provide high time-resolution data to investigate aerosol sources, atmospheric transformation processes, and health effects. In this work, the in situ ion chromatograph (IC) system was developed to provide 15-min time-resolution data of nine soluble inorganic species (Cl -, NO 2-, NO 3-, SO 42-, Na +, NH 4+, K +, Mg 2+ and Ca 2+). Over 89% of all particles larger than approximately 0.056 μm were collected by the in situ IC system. The in situ IC system is estimated to have a limit of detection lower than 0.3 μg m -3 for the various ambient ionic components. Depending on the hourly measurements, the pollutant events with high aerosol concentrations in Taipei Basin were associated with the local traffic emission in rush hour, the accumulation of pollutants in the stagnant atmosphere, the emission of industrial pollutants from the nearby factories, the photochemical secondary aerosol formation, and the long-range transport of pollutants from Asian outflows.

Chemical and isotopic composition of secondary organic aerosol generated by alpha-pinene ozonolysis

NARCIS (Netherlands)

Meusinger, Carl; Dusek, Ulrike; King, Stephanie M.; Holzinger, Rupert; Rosenorn, Thomas; Sperlich, Peter; Julien, Maxime; Remaud, Gerald S.; Bilde, Merete; Rockmann, Thomas; Johnson, Matthew S.

2017-01-01

Secondary organic aerosol (SOA) plays a central role in air pollution and climate. However, the description of the sources and mechanisms leading to SOA is elusive despite decades of research. While stable isotope analysis is increasingly used to constrain sources of ambient aerosol, in many cases

Aerosol composition, chemistry, and source characterization during the 2008 VOCALS Experiment

Energy Technology Data Exchange (ETDEWEB)

Lee, Y.; Springston, S.; Jayne, J.; Wang, J.; Senum, G.; Hubbe, J.; Alexander, L.; Brioude, J.; Spak, S.; Mena-Carrasco, M.; Kleinman, L.; Daum, P.

2010-03-15

Chemical composition of fine aerosol particles over the northern Chilean coastal waters was determined onboard the U.S. DOE G-1 aircraft during the VOCALS (VAMOS Ocean-Cloud-Atmosphere-Land Study) field campaign between October 16 and November 15, 2008. SO42-, NO3-, NH4+, and total organics (Org) were determined using an Aerodyne Aerosol Mass Spectrometer, and SO42-, NO3-, NH4+, Na+, Cl-, CH3SO3-, Mg2+, Ca2+, and K+ were determined using a particle-into-liquid sampler-ion chromatography technique. The results show the marine boundary layer (MBL) aerosol mass was dominated by non- sea-salt SO42- followed by Na+, Cl-, Org, NO3-, and NH4+, in decreasing importance; CH3SO3-, Ca2+, and K+ rarely exceeded their respective limits of detection. The SO42- aerosols were strongly acidic as the equivalent NH4+ to SO42- ratio was only {approx}0.25 on average. NaCl particles, presumably of sea-salt origin, showed chloride deficits but retained Cl- typically more than half the equivalency of Na+, and are externally mixed with the acidic sulfate aerosols. Nitrate was observed only on sea-salt particles, consistent with adsorption of HNO3 on sea-salt aerosols, responsible for the Cl- deficit. Dust particles appeared to play a minor role, judging from the small volume differences between that derived from the observed mass concentrations and that calculated based on particle size distributions. Because SO42- concentrations were substantial ({approx}0.5 - {approx}3 {micro}g/m3) with a strong gradient (highest near the shore), and the ocean-emitted dimethylsulfide and its unique oxidation product, CH3SO3-, were very low (i.e., {le} 40 parts per trillion and <0.05 {micro}g/m3, respectively), the observed SO42- aerosols are believed to be primarily of terrestrial origin. Back trajectory calculations indicate sulfur emissions from smelters and power plants along coastal regions of Peru and Chile are the main sources of these SO4- aerosols. However, compared to observations, model

Elemental composition of aerosol particles from two atmospheric monitoring stations in the Amazon Basin

International Nuclear Information System (INIS)

Artaxo, P.; Gerab, F.; Rabello, M.L.C.

1993-01-01

One key region for the study of processes that are changing the composition of the global atmosphere is the Amazon Basin tropical rain forest. The high rate of deforestation and biomass burning is emitting large amounts of gases and fine-mode aerosol particles to the global atmosphere. Two background monitoring stations are operating continuously measuring aerosol composition, at Cuiaba, and Serra do Navio. Fine- and coarse-mode aerosol particles are being collected using stacked filter units. Particle induced X-ray emission (PIXE) was used to measure concentrations of up to 21 elements: Al, Si, P, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Se, Br, Rb, Sr, Zr, and Pb. The elemental composition was measured at the new PIXE facility from the University of Sao Paulo, using a dedicated 5SDH tandem Pelletron nuclear accelerator. Absolute principal factor analysis (APFA) has derived absolute elemental source profiles. At the Serra do Navio sampling site a very clean background aerosol is being observed. Biogenic aerosol dominates the fine-mode mass concentration, with the presence of K, P, S, Cl, Zn, Br, and FPM. Three components dominate the aerosol composition: Soil dust particles, the natural biogenic release by the forest, and a marine aerosol component. At the Cuiaba site, during the dry season, a strong component of biomass burning is observed. An aerosol mass concentration up to 120 μg/m 3 was measured. APFA showed three components: Soil dust (Al, Ca, Ti, Mn, Fe), biomass burning (soot, FPM, K, Cl) and natural biogenic particles (K, S, Ca, Mn, Zn). The fine-mode biogenic component of both sites shows remarkable similarities, although the two sampling sites are 3000 km apart. Several essential plant nutrients like P, K, S, Ca, Ni and others are transported in the atmosphere as a result of biomass burning processes. (orig.)

Chemical ageing and transformation of diffusivity in semi-solid multi-component organic aerosol particles

Science.gov (United States)

Pfrang, C.; Shiraiwa, M.; Pöschl, U.

2011-07-01

Recent experimental evidence underlines the importance of reduced diffusivity in amorphous semi-solid or glassy atmospheric aerosols. This paper investigates the impact of diffusivity on the ageing of multi-component reactive organic particles approximating atmospheric cooking aerosols. We apply and extend the recently developed KM-SUB model in a study of a 12-component mixture containing oleic and palmitoleic acids. We demonstrate that changes in the diffusivity may explain the evolution of chemical loss rates in ageing semi-solid particles, and we resolve surface and bulk processes under transient reaction conditions considering diffusivities altered by oligomerisation. This new model treatment allows prediction of the ageing of mixed organic multi-component aerosols over atmospherically relevant timescales and conditions. We illustrate the impact of changing diffusivity on the chemical half-life of reactive components in semi-solid particles, and we demonstrate how solidification and crust formation at the particle surface can affect the chemical transformation of organic aerosols.

Chemical ageing and transformation of diffusivity in semi-solid multi-component organic aerosol particles

Directory of Open Access Journals (Sweden)

C. Pfrang

2011-07-01

Full Text Available Recent experimental evidence underlines the importance of reduced diffusivity in amorphous semi-solid or glassy atmospheric aerosols. This paper investigates the impact of diffusivity on the ageing of multi-component reactive organic particles approximating atmospheric cooking aerosols. We apply and extend the recently developed KM-SUB model in a study of a 12-component mixture containing oleic and palmitoleic acids. We demonstrate that changes in the diffusivity may explain the evolution of chemical loss rates in ageing semi-solid particles, and we resolve surface and bulk processes under transient reaction conditions considering diffusivities altered by oligomerisation. This new model treatment allows prediction of the ageing of mixed organic multi-component aerosols over atmospherically relevant timescales and conditions. We illustrate the impact of changing diffusivity on the chemical half-life of reactive components in semi-solid particles, and we demonstrate how solidification and crust formation at the particle surface can affect the chemical transformation of organic aerosols.

Comparison of three aerosol chemical characterization techniques utilizing PTR-ToF-MS: a study on freshly formed and aged biogenic SOA

Directory of Open Access Journals (Sweden)

G. I. Gkatzelis

2018-03-01

Full Text Available An intercomparison of different aerosol chemical characterization techniques has been performed as part of a chamber study of biogenic secondary organic aerosol (BSOA formation and aging at the atmosphere simulation chamber SAPHIR (Simulation of Atmospheric PHotochemistry In a large Reaction chamber. Three different aerosol sampling techniques – the aerosol collection module (ACM, the chemical analysis of aerosol online (CHARON and the collection thermal-desorption unit (TD were connected to proton transfer reaction time-of-flight mass spectrometers (PTR-ToF-MSs to provide chemical characterization of the SOA. The techniques were compared among each other and to results from an aerosol mass spectrometer (AMS and a scanning mobility particle sizer (SMPS. The experiments investigated SOA formation from the ozonolysis of β-pinene, limonene, a β-pinene–limonene mix and real plant emissions from Pinus sylvestris L. (Scots pine. The SOA was subsequently aged by photo-oxidation, except for limonene SOA, which was aged by NO3 oxidation. Despite significant differences in the aerosol collection and desorption methods of the PTR-based techniques, the determined chemical composition, i.e. the same major contributing signals, was found by all instruments for the different chemical systems studied. These signals could be attributed to known products expected from the oxidation of the examined monoterpenes. The sampling and desorption method of ACM and TD provided additional information on the volatility of individual compounds and showed relatively good agreement. Averaged over all experiments, the total aerosol mass recovery compared to an SMPS varied within 80 ± 10, 51 ± 5 and 27 ± 3 % for CHARON, ACM and TD, respectively. Comparison to the oxygen-to-carbon ratios (O : C obtained by AMS showed that all PTR-based techniques observed lower O : C ratios, indicating a loss of molecular oxygen either during aerosol sampling or

Chemical composition and optical properties of aerosols in the lower mixed layer and the free troposphere. Final report of the AFS project; Chemische Zusammensetzung und optische Eigenschaften des Aerosols in der freien Troposphaere. Abschlussbericht zum AFS-Projekt

Energy Technology Data Exchange (ETDEWEB)

Asseng, H. [Freie Univ. Berlin (Germany). Inst. fuer Weltraumwissenschaften]|[Max-Planck-Institut fuer Chemie, Mainz (Germany). Abt. Biogeochemie; Fischer, J. [Freie Univ. Berlin (Germany). Inst. fuer Weltraumwissenschaften; Helas, G. [Max-Planck-Institut fuer Chemie, Mainz (Germany). Abt. Biogeochemie; Weller, M. [Deutscher Wetterdienst, Potsdam (Germany). Meteorologisches Observatorium

2001-08-02

Aerosol radiative forcing is the largest unknown in current climate models and, as a result, in predicting future climate. Accurate vertically-resolved measurements of aerosol optical properties are an important element of improved climate prediction (IPCC). The present project has contributed to this objective. Jets of directly and remotely determined radiation data have been provided suitable to cut down the uncertainty of column- or layer related optical aerosol parameters. In the present case mean values and profiles of spectral scattering - and absorption coefficients have been retrieved from ground based and airborne sky-radiance/solar irradiance measurements. Available analyses of size and chemical composition of sampled particles (adjoined projects) have been also taken into consideration. The retrieved parameters have served as an input for modelling the radiative transfer exactly for the real time of measurements. Closure procedures yielded finally realistic spectral scattering - and absorption coefficients typically for the lower troposphere in a mostly rural Central European region. (orig.) [German] Die ungenuegende Kenntnis strahlungswirksamer, optischer Aerosolparameter ist laut IPCC die groesste Unbekannte bei der Modellierung des Klimas und seiner Veraenderung. Wissenschaft und Technik bemuehen sich in sog. Schliessungsexperimenten aus der Ueberbestimmung direkt und indirekt gemessener Aerosolparameter genaue(re) Kenntnis (Mittelwert/Variation) ueber deren Klimawirksamkeit zu erlangen. Im vorliegenden Projekt wurden aus verschiedenen passiven, spektralen Messungen von Streulicht und Transmission der Atmosphaere in verschiedenen Hoehen sowie aus der Beruecksichtigung von Partikelanalysen Dritter, Streu- und Absorptionskoeffizienten des Aerosols der gesamten Luftsaeule und in vertikaler Aufloesung abgeleitet. Strahlungstransportmodellierungen mit den gewonnenen Aerosolparametern als input engten ueber den Vergleich mit den Messungen deren Grad an

Optical and Chemical Characterization of Aerosols Produced from Cooked Meats

Science.gov (United States)

Niedziela, R. F.; Foreman, E.; Blanc, L. E.

2011-12-01

Cooking processes can release a variety compounds into the air immediately above a cooking surface. The distribution of compounds will largely depend on the type of food that is being processed and the temperatures at which the food is prepared. High temperatures release compounds from foods like meats and carry them away from the preparation surface into cooler regions where condensation into particles can occur. Aerosols formed in this manner can impact air quality, particularly in urban areas where the amount of food preparation is high. Reported here are the results of laboratory experiments designed to optically and chemically characterize aerosols derived from cooking several types of meats including ground beef, salmon, chicken, and pork both in an inert atmosphere and in synthetic air. The laboratory-generated aerosols are studied using a laminar flow cell that is configured to accommodate simultaneous optical characterization in the mid-infrared and collection of particles for subsequent chemical analysis by gas chromatography. Preliminary optical results in the visible and ultra-violet will also be presented.

Characterization of distinct Arctic aerosol accumulation modes and their sources

DEFF Research Database (Denmark)

Lange, R.; Dall'Osto, M.; Skov, H.

2018-01-01

-August). By association to chemical composition, cloud condensation nuclei properties, and meteorological variables, three typical accumulation mode aerosol clusters were identified: Haze (32% of the time), Bimodal (14%) and Aged (6%). In brief: (1) Haze accumulation mode aerosol shows a single mode at 150 nm, peaking...

Importance of aerosol non-sphericity in estimating aerosol radiative forcing in Indo-Gangetic Basin.

Science.gov (United States)

Srivastava, Parul; Dey, Sagnik; Srivastava, Atul Kumar; Singh, Sachchidanand; Mishra, S K; Tiwari, Suresh

2017-12-01

Aerosols are usually presumed spherical in shape while estimating the direct radiative forcing (DRF) using observations or in the models. In the Indo-Gangetic Basin (IGB), a regional aerosol hotspot where dust is a major aerosol species and has been observed to be non-spherical in shape, it is important to test the validity of this assumption. We address this issue using measured chemical composition at megacity Delhi, a representative site of the western IGB. Based on the observation, we choose three non-spherical shapes - spheroid, cylinder and chebyshev, and compute their optical properties. Non-spherical dust enhances aerosol extinction coefficient (β ext ) and single scattering albedo (SSA) at visible wavelengths by >0.05km -1 and >0.04 respectively, while it decreases asymmetry parameter (g) by ~0.1. Accounting non-sphericity leads top-of-the-atmosphere (TOA) dust DRF to more cooling due to enhanced backscattering and increases surface dimming due to enhanced β ext . Outgoing shortwave flux at TOA increases by up to 3.3% for composite aerosols with non-spherical dust externally mixed with other spherical species. Our results show that while non-sphericity needs to be accounted for, choice of shape may not be important in estimating aerosol DRF in the IGB. Copyright © 2017 Elsevier B.V. All rights reserved.

Secondary organic aerosols. Chemical aging, hygroscopicity, and cloud droplet activation

Energy Technology Data Exchange (ETDEWEB)

Buchholz, Angela

2011-07-06

functional groups in this compound was adjusted to reproduce the observed growth curves. However, further information on surface tension and the ratio of the molecular mass and density of the solute is needed to predict activation behavior from hygroscopic growth measurements. A dependence of {kappa} on the ratio of primarily produced OH to initial VOC level was observed. The higher {kappa} values for low precursor concentrations could be attributed to a higher OH/VOC level. The detailed chemical composition of the gas-phase precursors had only little effect on {kappa}. In long term experiments there was no significant effect of the observed chemical aging of the particles on {kappa}. The observed low variability of {kappa} for biogenic SOA particles simplifies their treatment in global models as an average value of {kappa} = 0.1 can be used. (orig.)

Effect of flavoring chemicals on free radical formation in electronic cigarette aerosols.

Science.gov (United States)

Bitzer, Zachary T; Goel, Reema; Reilly, Samantha M; Elias, Ryan J; Silakov, Alexey; Foulds, Jonathan; Muscat, Joshua; Richie, John P

2018-05-20

Flavoring chemicals, or flavorants, have been used in electronic cigarettes (e-cigarettes) since their inception; however, little is known about their toxicological effects. Free radicals present in e-cigarette aerosols have been shown to induce oxidative stress resulting in damage to proliferation, survival, and inflammation pathways in the cell. Aerosols generated from e-liquid solvents alone contain high levels of free radicals but few studies have looked at how these toxins are modulated by flavorants. We investigated the effects of different flavorants on free radical production in e-cigarette aerosols. Free radicals generated from 49 commercially available e-liquid flavors were captured and analyzed using electron paramagnetic resonance (EPR). The flavorant composition of each e-liquid was analyzed by gas chromatography mass spectroscopy (GCMS). Radical production was correlated with flavorant abundance. Ten compounds were identified and analyzed for their impact on free radical generation. Nearly half of the flavors modulated free radical generation. Flavorants with strong correlations included β-damascone, δ-tetradecalactone, γ-decalactone, citral, dipentene, ethyl maltol, ethyl vanillin, ethyl vanillin PG acetal, linalool, and piperonal. Dipentene, ethyl maltol, citral, linalool, and piperonal promoted radical formation in a concentration-dependent manner. Ethyl vanillin inhibited the radical formation in a concentration dependent manner. Free radical production was closely linked with the capacity to oxidize biologically-relevant lipids. Our results suggest that flavoring agents play an important role in either enhancing or inhibiting the production of free radicals in flavored e-cigarette aerosols. This information is important for developing regulatory strategies aimed at reducing potential harm from e-cigarettes. Copyright © 2018 Elsevier Inc. All rights reserved.

A model study of the size and composition distribution of aerosols in an aircraft exhaust

Energy Technology Data Exchange (ETDEWEB)

Sorokin, A.A. [SRC `ECOLEN`, Moscow (Russian Federation)

1997-12-31

A two-dimensional, axisymmetric flow field model which includes water and sulphate aerosol formation represented by moments of the size and composition distribution function is used to calculate the effect of radial turbulent jet mixing on the aerosol size distribution and mean modal composition. (author) 6 refs.

A model study of the size and composition distribution of aerosols in an aircraft exhaust

Energy Technology Data Exchange (ETDEWEB)

Sorokin, A A [SRC ` ECOLEN` , Moscow (Russian Federation)

1998-12-31

A two-dimensional, axisymmetric flow field model which includes water and sulphate aerosol formation represented by moments of the size and composition distribution function is used to calculate the effect of radial turbulent jet mixing on the aerosol size distribution and mean modal composition. (author) 6 refs.

Near Real-Time, Microchip Assay of Aerosol Chemical Composition, Phase I

Data.gov (United States)

National Aeronautics and Space Administration — A compact, autonomous and rugged instrument to measure the concentration of inorganic ions, and possibly organic acids, in atmospheric aerosols is proposed. This...

Single-particle characterization of the high-Arctic summertime aerosol

Science.gov (United States)

Sierau, B.; Chang, R. Y.-W.; Leck, C.; Paatero, J.; Lohmann, U.

2014-07-01

Single-particle mass-spectrometric measurements were carried out in the high Arctic north of 80° during summer 2008. The campaign took place onboard the icebreaker Oden and was part of the Arctic Summer Cloud Ocean Study (ASCOS). The instrument deployed was an aerosol time-of-flight mass spectrometer (ATOFMS) that provides information on the chemical composition of individual particles and their mixing state in real time. Aerosols were sampled in the marine boundary layer at stations in the open ocean, in the marginal ice zone, and in the pack ice region. The largest fraction of particles detected for subsequent analysis in the size range of the ATOFMS between approximately 200 and 3000 nm in diameter showed mass-spectrometric patterns, indicating an internal mixing state and a biomass burning and/or biofuel source. The majority of these particles were connected to an air mass layer of elevated particle concentration mixed into the surface mixed layer from the upper part of the marine boundary layer. The second largest fraction was represented by sea salt particles. The chemical analysis of the over-ice sea salt aerosol revealed tracer compounds that reflect chemical aging of the particles during their long-range advection from the marginal ice zone, or open waters south thereof prior to detection at the ship. From our findings we conclude that long-range transport of particles is one source of aerosols in the high Arctic. To assess the importance of long-range particle sources for aerosol-cloud interactions over the inner Arctic in comparison to local and regional biogenic primary aerosol sources, the chemical composition of the detected particles was analyzed for indicators of marine biological origin. Only a minor fraction showed chemical signatures of potentially ocean-derived primary particles of that kind. However, a chemical bias in the ATOFMS's detection capabilities observed during ASCOS might suggest the presence of a particle type of unknown composition

Single-particle characterization of the High Arctic summertime aerosol

Science.gov (United States)

Sierau, B.; Chang, R. Y.-W.; Leck, C.; Paatero, J.; Lohmann, U.

2014-01-01

Single-particle mass spectrometric measurements were carried out in the High Arctic north of 80° during summer 2008. The campaign took place onboard the icebreaker Oden and was part of the Arctic Summer Cloud Ocean Study (ASCOS). The instrument deployed was an Aerosol Time-of-Flight Mass Spectrometer (ATOFMS) that provides information on the chemical composition of individual particles and their mixing state in real-time. Aerosols were sampled in the marine boundary layer at stations in the open ocean, in the marginal ice zone, and in the pack ice region. The largest fraction of particles detected for subsequent analysis in the size range of the ATOFMS between approximately 200 nm to 3000 nm in diameter showed mass spectrometric patterns indicating an internal mixing state and a biomass burning and/or biofuel source. The majority of these particles were connected to an air mass layer of elevated particle concentration mixed into the surface mixed layer from the upper part of the marine boundary layer. The second largest fraction was represented by sea salt particles. The chemical analysis of the over-ice sea salt aerosol revealed tracer compounds that reflect chemical aging of the particles during their long-range advection from the marginal ice zone, or open waters south thereof prior to detection at the ship. From our findings we conclude that long-range transport of particles is one source of aerosols in the High Arctic. To assess the importance of long-range particle sources for aerosol-cloud interactions over the inner Arctic in comparison to local and regional biogenic primary aerosol sources, the chemical composition of the detected particles was analyzed for indicators of marine biological origin. Only a~minor fraction showed chemical signatures of potentially ocean-derived primary particles of that kind. However, a chemical bias in the ATOFMS's detection capabilities observed during ASCOS might suggest a presence of a particle type of unknown composition

Seasonal characterization of submicron aerosol chemical composition and organic aerosol sources in the southeastern United States: Atlanta, Georgia,and Look Rock, Tennessee

Directory of Open Access Journals (Sweden)

S. H. Budisulistiorini

2016-04-01

Full Text Available A year-long near-real-time characterization of non-refractory submicron aerosol (NR-PM1 was conducted at an urban (Atlanta, Georgia, in 2012 and rural (Look Rock, Tennessee, in 2013 site in the southeastern US using the Aerodyne Aerosol Chemical Speciation Monitor (ACSM collocated with established air-monitoring network measurements. Seasonal variations in organic aerosol (OA and inorganic aerosol species are attributed to meteorological conditions as well as anthropogenic and biogenic emissions in this region. The highest concentrations of NR-PM1 were observed during winter and fall seasons at the urban site and during spring and summer at the rural site. Across all seasons and at both sites, NR-PM1 was composed largely of OA (up to 76 % and sulfate (up to 31 %. Six distinct OA sources were resolved by positive matrix factorization applied to the ACSM organic mass spectral data collected from the two sites over the 1 year of near-continuous measurements at each site: hydrocarbon-like OA (HOA, biomass burning OA (BBOA, semi-volatile oxygenated OA (SV-OOA, low-volatility oxygenated OA (LV-OOA, isoprene-derived epoxydiols (IEPOX OA (IEPOX-OA and 91Fac (a factor dominated by a distinct ion at m∕z 91 fragment ion previously observed in biogenic influenced areas. LV-OOA was observed throughout the year at both sites and contributed up to 66 % of total OA mass. HOA was observed during the entire year only at the urban site (on average 21 % of OA mass. BBOA (15–33 % of OA mass was observed during winter and fall, likely dominated by local residential wood burning emission. Although SV-OOA contributes quite significantly ( ∼  27 %, it was observed only at the urban site during colder seasons. IEPOX-OA was a major component (27–41 % of OA at both sites, particularly in spring and summer. An ion fragment at m∕z 75 is well correlated with the m∕z 82 ion associated with the aerosol mass spectrum of IEPOX

Lidar sprectroscopy instrument (LISSI): An infrastructure facility for chemical aerosol profiling at the University of Hertfordshire

Science.gov (United States)

Tesche, Matthias; Tatarov, Boyan; Noh, Youngmin; Müller, Detlef

2018-04-01

The lidar development at the University of Hertfordshire explores the feasibility of using Raman backscattering for chemical aerosol profiling. This paper provides an overview of the new facility. A high-power Nd:YAG/OPO setup is used to excite Raman backscattering at a wide range of wavelengths. The receiver combines a spectrometer with a 32-channel detector or an ICCD camera to resolve Raman signals of various chemical compounds. The new facility will open new avenues for chemical profiling of aerosol pollution from measurements of Raman scattering by selected chemical compounds, provide data that allow to close the gap between optical and microphysical aerosol profiling with lidar and enables connecting lidar measurements to parameters used in atmospheric modelling.

The effect of varying physical and chemical characteristics of inhaled plutonium aerosols on metabolism and excretion

International Nuclear Information System (INIS)

Mewhinney, J.A.; Muggenburg, B.A.; McClellan, R.O.; Miglio, J.J.

1976-01-01

The effects of different chemical and physical parameters of plutonium aerosols on lung retention, tissue distribution and excretion patterns were evaluated in beagle dogs. Polydisperse aerosols of 239 Pu of different chemical form were produced by heating droplets nebulized from a solution of 239 PuIV in 1M HC1 to temperatures ranging from 325 0 C to 1150 0 C. Droplets containing 238 Pu(OH) 4 were treated at 1150 0 C and the resultant polydisperse aerosol used or separated into monodisperse size groups. Beagle dogs were exposed by inhalation to provide initial lung burdens in the range of 0.75 to 1.0μCi. The aerosols were characterized as to particle size and size distribution, and an in-vitro solubility measurement was made on samples of the aerosol from each animal exposure. Different production temperatures for the 239 Pu aerosols resulted in lung retention half-times that increased as the production temperature increased. The 239 Pu tissue distribution and urinary excretion patterns were correlated with lung retention. Faecal excretion was greater for aerosols produced at lower temperatures. Lung retention half-times for 238 Pu monodisperse aerosols were not greatly different from particle sizes of 0.8 and 1.9μm activity median aerodynamic diameter (AMAD). The third monodisperse aerosol intended to be 3.0μm AMAD had a bimodal particle size distribution and contained a significant fraction of readily soluble material. The 238 Pu polydisperse aerosol had a slightly lower lung retention, increased urinary excretion and translocation to tissues than the comparable 239 Pu polydisperse material. This study serves to emphasize the importance of complete analysis of the aerosol material as well as early excretion data following accidental human exposure to aerosols containing plutonium. The role of chemical form and aerosol particle size in evaluation of such cases is discussed. (author)

Relative humidity impact on aerosol parameters in a Paris suburban area

Directory of Open Access Journals (Sweden)

H. Randriamiarisoa

2006-01-01

Full Text Available Measurements of relative humidity (RH and aerosol parameters (scattering cross section, size distributions and chemical composition, performed in ambient atmospheric conditions, have been used to study the influence of relative humidity on aerosol properties. The data were acquired in a suburban area south of Paris, between 18 and 24 July 2000, in the framework of the 'Etude et Simulation de la Qualité de l'air en Ile-de-France' (ESQUIF program. According to the origin of the air masses arriving over the Paris area, the aerosol hygroscopicity is more or less pronounced. The aerosol chemical composition data were used as input of a thermodynamic model to simulate the variation of the aerosol water mass content with ambient RH and to determine the main inorganic salt compounds. The coupling of observations and modelling reveals the presence of deliquescence processes with hysteresis phenomenon in the hygroscopic growth cycle. Based on the Hänel model, parameterisations of the scattering cross section, the modal radius of the accumulation mode of the size distribution and the aerosol water mass content, as a function of increasing RH, have been assessed. For the first time, a crosscheck of these parameterisations has been performed and shows that the hygroscopic behaviour of the accumulation mode can be coherently characterized by combined optical, size distribution and chemical measurements.

Aerosol composition and source apportionment in the Mexico City Metropolitan Area with PIXE/PESA/STIM and multivariate analysis

OpenAIRE

Johnson , K. S.; De Foy , B.; Zuberi , B.; Molina , L. T.; Molina , M. J.; Xie , Y.; Laskin , A.; Shutthanandan , V.

2006-01-01

Aerosols play an important role in the atmosphere but are poorly characterized, particularly in urban areas like the Mexico City Metropolitan Area (MCMA). The chemical composition of urban particles must be known to assess their effects on the environment, and specific particulate emissions sources should be identified to establish effective pollution control standards. For these reasons, samples of particulate matter ≤2.5 μm (PM_2.5) were collected dur...

Hygroscopic behavior and chemical composition evolution of internally mixed aerosols composed of oxalic acid and ammonium sulfate

Directory of Open Access Journals (Sweden)

X. Wang

2017-10-01

Full Text Available Although water uptake of aerosol particles plays an important role in the atmospheric environment, the effects of interactions between components on chemical composition and hygroscopicity of particles are still not well constrained. The hygroscopic properties and phase transformation of oxalic acid (OA and mixed particles composed of ammonium sulfate (AS and OA with different organic to inorganic molar ratios (OIRs have been investigated by using confocal Raman spectroscopy. It is found that OA droplets first crystallize to form OA dihydrate at 71 % relative humidity (RH, and further lose crystalline water to convert into anhydrous OA around 5 % RH during the dehydration process. The deliquescence and efflorescence point for AS is determined to be 80.1 ± 1.5 % RH and 44.3 ± 2.5 % RH, respectively. The observed efflorescence relative humidity (ERH for mixed OA ∕ AS droplets with OIRs of 1 : 3, 1 : 1 and 3 : 1 is 34.4 ± 2.0, 44.3 ± 2.5 and 64.4 ± 3.0 % RH, respectively, indicating the elevated OA content appears to favor the crystallization of mixed systems at higher RH. However, the deliquescence relative humidity (DRH of AS in mixed OA ∕ AS particles with OIRs of 1 : 3 and 1 : 1 is observed to occur at 81.1 ± 1.5 and 77 ± 1.0 % RH, respectively. The Raman spectra of mixed OA ∕ AS droplets indicate the formation of ammonium hydrogen oxalate (NH4HC2O4 and ammonium hydrogen sulfate (NH4HSO4 from interactions between OA and AS in aerosols during the dehydration process on the time scale of hours, which considerably influence the subsequent deliquescence behavior of internally mixed particles with different OIRs. The mixed OA ∕ AS particles with an OIR of 3 : 1 exhibit no deliquescence transition over the RH range studied due to the considerable transformation of (NH42SO4 into NH4HC2O4 with a high DRH. Although the hygroscopic growth of mixed OA�

Flight-based chemical characterization of biomass burning aerosols within two prescribed burn smoke plumes

Directory of Open Access Journals (Sweden)

K. A. Pratt

2011-12-01

Full Text Available Biomass burning represents a major global source of aerosols impacting direct radiative forcing and cloud properties. Thus, the goal of a number of current studies involves developing a better understanding of how the chemical composition and mixing state of biomass burning aerosols evolve during atmospheric aging processes. During the Ice in Clouds Experiment-Layer Clouds (ICE-L in the fall of 2007, smoke plumes from two small Wyoming Bureau of Land Management prescribed burns were measured by on-line aerosol instrumentation aboard a C-130 aircraft, providing a detailed chemical characterization of the particles. After ~2–4 min of aging, submicron smoke particles, produced primarily from sagebrush combustion, consisted predominantly of organics by mass, but were comprised primarily of internal mixtures of organic carbon, elemental carbon, potassium chloride, and potassium sulfate. Significantly, the fresh biomass burning particles contained minor mass fractions of nitrate and sulfate, suggesting that hygroscopic material is incorporated very near or at the point of emission. The mass fractions of ammonium, sulfate, and nitrate increased with aging up to ~81–88 min and resulted in acidic particles. Decreasing black carbon mass concentrations occurred due to dilution of the plume. Increases in the fraction of oxygenated organic carbon and the presence of dicarboxylic acids, in particular, were observed with aging. Cloud condensation nuclei measurements suggested all particles >100 nm were active at 0.5% water supersaturation in the smoke plumes, confirming the relatively high hygroscopicity of the freshly emitted particles. For immersion/condensation freezing, ice nuclei measurements at −32 °C suggested activation of ~0.03–0.07% of the particles with diameters greater than 500 nm.

Aerosol composition and source apportionment in Santiago de Chile

International Nuclear Information System (INIS)

Artaxo, Paulo; Oyola, Pedro; Martinez, Roberto

1999-01-01

Santiago de Chile, Sao Paulo and Mexico City are Latin American urban areas that suffer from heavy air pollution. In order to study air pollution in Santiago area, an aerosol source apportionment study was designed to measure ambient aerosol composition and size distribution for two downtown sampling sites in Santiago. The aerosol monitoring stations were operated in Gotuzo and Las Condes during July and August 1996. The study employed stacked filter units (SFU) for aerosol sampling, collecting fine mode aerosol (dp 10 mass of particles smaller than 10 μm) and black carbon concentration were also measured. Particle-Induced X-ray Emission (PIXE) was used to measure the concentration of 22 trace elements at levels below 0.5 ng m -3 . Quantitative aerosol source apportionment was performed using Absolute Principal Factor Analysis (APFA). Very high aerosol concentrations were observed (up to 400 μg/m 3 PM 10 ). The main aerosol particle sources in Santiago are resuspended soil dust and traffic emissions. Coarse particles account for 63% of PM 10 aerosol in Gotuzo and 53% in Las Condes. A major part of this component is resuspended soil dust. In the fine fraction, resuspended soil dust accounts for 15% of fine mass, and the aerosols associated with transportation activities account for a high 64% of the fine particle mass. Sulfate particle is an important component of the aerosol in Santiago, mainly originating from gas-to-particle conversion from SO 2 . In the Gotuzo site, sulfates are the highest aerosol component, accounting for 64.5% of fine mass. Direct traffic emissions are generally mixed with resuspended soil dust. It is difficult to separate the two components, because the soil dust in downtown Santiago is contaminated with Pb, Br, Cl, and other heavy metals that are also tracers for traffic emissions. Residual oil combustion is observed, with the presence of V, S and Ni. An aerosol components from industrial emissions is also present, with the presence of

Lidar sprectroscopy instrument (LISSI: An infrastructure facility for chemical aerosol profiling at the University of Hertfordshire

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Tesche Matthias

2018-01-01

The new facility will open new avenues for chemical profiling of aerosol pollution from measurements of Raman scattering by selected chemical compounds, provide data that allow to close the gap between optical and microphysical aerosol profiling with lidar and enables connecting lidar measurements to parameters used in atmospheric modelling.

Chemistry and Microphysics of Lower Stratospheric Aerosols Determined by Satellite Remote Sensing

Science.gov (United States)

Zasetsky, A. Y.; Khalizov, A.; Sloan, J.

2003-12-01

Observations of broadband Infrared satellites such as ILAS-II (Ministry of the Environment, Japan, launched 14 December 2002) and SciSat-1 (Canadian Space Agency, launched 12 August 2003) can provide details of the chemical composition and particle size of atmospheric aerosols by direct inversion without recourse to models. During the past decade, we have developed mathematical methods to achieve this inversion by working with FTIR observations of model atmospheric aerosols in cryogenic flowtubes. More recently, we have converted these to operational algorithms for use in the above missions. In this presentation, we will briefly outline these procedures and illustrate their capabilities using laboratory data. These laboratory results show that the chemical compositions, phases and sizes of ensembles of particles can be obtained simultaneously using these procedures. We will also report chemical and microphysical properties of lower stratospheric clouds and aerosols derived by applying these procedures to observations from space.

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

NARCIS (Netherlands)

Van Beelen, A. J.; Roelofs, G. J H; Hasekamp, O. P.; Henzing, J. S.; Röckmann, T.

2014-01-01

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

Neutralization of Aerosolized Bio-Agents by Filled Nanocomposite Materials through Thermal and Chemical Inactivation Mechanisms

Science.gov (United States)

2016-06-01

Bio -agents by Filled Nanocomposite Materials through Thermal and Chemical Inactivation Mechanisms Distribution Statement A. Approved for public...of Cincinnati Project Title: Neutralization of Aerosolized Bio -agents by Filled Nanocomposite Materials through Thermal and Chemical Inactivation...fire ball, where they will not effectively interact with any viable bio -aerosol. 1.1.4. Conclusions Cryo-milling is necessary to achieve a

PM2.5 Chemical Compositions and Aerosol Optical Properties in Beijing during the Late Fall

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Huanbo Wang

2015-01-01

Full Text Available Daily PM2.5 mass concentrations and chemical compositions together with the aerosol optical properties were measured from 8–28 November 2011 in Beijing. PM2.5 mass concentration varied from 15.6–237.5 μg∙m−3 and showed a mean value of 111.2 ± 73.4 μg∙m−3. Organic matter, NH4NO3 and (NH42SO4 were the major constituents of PM2.5, accounting for 39.4%, 15.4%, and 14.9% of the total mass, respectively, while fine soil, chloride salt, and elemental carbon together accounted for 27.7%. Daily scattering and absorption coefficients (σsc and σap were in the range of 31.1–667 Mm−1 and 8.24–158.0 Mm−1, with mean values of 270 ± 200 Mm−1 and 74.3 ± 43.4 Mm−1. Significant increases in σsc and σap were observed during the pollution accumulation episodes. The revised IMPROVE algorithm was applied to estimate the extinction coefficient (bext. On average, organic matter was the largest contributor, accounting for 44.6% of bext, while (NH42SO4, NH4NO3, elemental carbon, and fine soil accounted for 16.3% 18.0%, 18.6%, and 2.34% of bext, respectively. Nevertheless, the contributions of (NH42SO4 and NH4NO3 were significantly higher during the heavy pollution periods than those on clean days. Typical pollution episodes were also explored, and it has been characterized that secondary formation of inorganic compounds is more important than carbonaceous pollution for visibility impairment in Beijing.

Photochemical aging of aerosol particles in different air masses arriving at Baengnyeong Island, Korea

Science.gov (United States)

Kang, Eunha; Lee, Meehye; Brune, William H.; Lee, Taehyoung; Park, Taehyun; Ahn, Joonyoung; Shang, Xiaona

2018-05-01

Atmospheric aerosol particles are a serious health risk, especially in regions like East Asia. We investigated the photochemical aging of ambient aerosols using a potential aerosol mass (PAM) reactor at Baengnyeong Island in the Yellow Sea during 4-12 August 2011. The size distributions and chemical compositions of aerosol particles were measured alternately every 6 min from the ambient air or through the highly oxidizing environment of a potential aerosol mass (PAM) reactor. Particle size and chemical composition were measured by using the combination of a scanning mobility particle sizer (SMPS) and a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). Inside the PAM reactor, O3 and OH levels were equivalent to 4.6 days of integrated OH exposure at typical atmospheric conditions. Two types of air masses were distinguished on the basis of the chemical composition and the degree of aging: air transported from China, which was more aged with a higher sulfate concentration and O : C ratio, and the air transported across the Korean Peninsula, which was less aged with more organics than sulfate and a lower O : C ratio. For both episodes, the particulate sulfate mass concentration increased in the 200-400 nm size range when sampled through the PAM reactor. A decrease in organics was responsible for the loss of mass concentration in 100-200 nm particles when sampled through the PAM reactor for the organics-dominated episode. This loss was especially evident for the m/z 43 component, which represents less oxidized organics. The m/z 44 component, which represents further oxidized organics, increased with a shift toward larger sizes for both episodes. It is not possible to quantify the maximum possible organic mass concentration for either episode because only one OH exposure of 4.6 days was used, but it is clear that SO2 was a primary precursor of secondary aerosol in northeast Asia, especially during long-range transport from China. In addition

Chemical composition of individual aerosol particles from working areas in a nickel refinery.

Science.gov (United States)

Höflich, B L; Wentzel, M; Ortner, H M; Weinbruch, S; Skogstad, A; Hetland, S; Thomassen, Y; Chaschin, V P; Nieboer, E

2000-06-01

Individual aerosol particles (n = 1170) collected at work stations in a nickel refinery were analyzed by wavelength-dispersive electron-probe microanalysis. By placing arbitrary restrictions on the contents of sulfur and silicon, the particles could be divided into four main groups. Scanning electron images indicated that most of the particles examined were relatively small (refinery intermediates. The implications of the findings for aerosol speciation measurements, toxicological studies and interpretation of adverse health effects are explored.

Aerosol composition and source apportionment in the Mexico City Metropolitan Area with PIXE/PESA/STIM and multivariate analysis

OpenAIRE

K. S. Johnson; B. de Foy; B. de Foy; B. Zuberi; B. Zuberi; L. T. Molina; L. T. Molina; M. J. Molina; M. J. Molina; Y. Xie; A. Laskin; V. Shutthanandan

2006-01-01

Aerosols play an important role in the atmosphere but are poorly characterized, particularly in urban areas like the Mexico City Metropolitan Area (MCMA). The chemical composition of urban particles must be known to assess their effects on the environment, and specific particulate emissions sources should be identified to establish effective pollution control standards. For these reasons, samples of particulate matter ≤2.5 μm (PM2.5) were collected during the MCMA-2003 Field Campaign f...

THE INFLUENCE OF BENZENE AS A TRACE REACTANT IN TITAN AEROSOL ANALOGS

Energy Technology Data Exchange (ETDEWEB)

Trainer, Melissa G. [Planetary Environments Laboratory, Code 699, NASA Goddard Space Flight Center, Greenbelt, MD 20771 (United States); Sebree, Joshua A. [NASA Postdoctoral Program Fellow, Code 699, Goddard Space Flight Center, Greenbelt, MD 20771 (United States); Heidi Yoon, Y.; Tolbert, Margaret A., E-mail: melissa.trainer@nasa.gov [Cooperative Institute for Research in Environmental Sciences, University of Colorado at Boulder, Box 216 UCB, Boulder, CO 80309 (United States)

2013-03-20

Benzene has been detected in Titan's atmosphere by Cassini instruments, with concentrations ranging from sub-ppb in the stratosphere to ppm in the ionosphere. Sustained levels of benzene in the haze formation region could signify that it is an important reactant in the formation of Titan's organic aerosol. To date, there have not been laboratory investigations to assess the influence of benzene on aerosol properties. We report a laboratory study on the chemical composition of organic aerosol formed from C{sub 6}H{sub 6}/CH{sub 4}/N{sub 2} via far ultraviolet irradiation (120-200 nm). The compositional results are compared to those from aerosol generated by a more ''traditional Titan'' mixture of CH{sub 4}/N{sub 2}. Our results show that even a trace amount of C{sub 6}H{sub 6} (10 ppm) has significant impact on the chemical composition and production rates of organic aerosol. There are several pathways by which photolyzed benzene may react to form larger molecules, both with and without the presence of CH{sub 4}, but many of these reaction mechanisms are only beginning to be explored for the conditions at Titan. Continued work investigating the influence of benzene in aerosol growth will advance understanding of this previously unstudied reaction system.

Effect of Morphology and Composition on the Hygroscopicity of Soot Aerosols

Science.gov (United States)

Williams, L.; Slowik, J.; Davidovits, P.; Jayne, J.; Kolb, C.; Worsnop, D.; Rudich, Y.

2003-12-01

Freshly generated soot aerosols are initially hydrophobic and unlikely to act as cloud condensation nuclei (CCN). However, during combustion many low vapor pressure gas products are formed that may then condense on existing soot aerosols. Additionally, soot particles may acquire coatings as they age, such as acids, salts, and oxygenated organics. An understanding of this aging process and its effect on soot hygroscopicity is necessary to address the potential of soot to act as a CCN. The transformation of soot from hydrophobic to hydrophilic is the focus of this work. An aim here is to determine the minimum coating required for hygroscopic growth. Soot particles produced by combustion of mixtures of fuel and air are size selected by a Differential Mobility Analyzer (DMA) and entrained in a laminar flow passing through a flow tube. The size selected soot particles are mixed with a controlled amount of the gas phase precursors to produce the coatings to be studied. Initial studies are focused on coatings of H2SO4, NH4NO3, and selected organics. The number of particles per unit volume of air is counted by a Condensation Particle Counter (CPC) and the particles are isokinetically sampled into an Aerosol Mass Spectrometer (AMS). Two distinct types of soot aerosols have been observed depending on the type of fuel and air mixture. With soot produced by the combustion of propane and air, the AMS shows a polydisperse particle size distribution with aerodynamic diameters ranging from 100 nm to 400 nm. The aerodynamic diameter is linearly related to the DMA-determined mobility diameter with the product density x shape factor = 1.2. The organic molecules in this soot are mostly PAH compounds. However, when kerosene is added to the propane flame, the soot particle morphology and composition is strikingly altered. While the DMA shows an essentially unchanged mobility diameter distribution, in the range 100 nm to 400, aerodynamic particle diameter is constant at about 100 nm

Single-particle characterization of the high-Arctic summertime aerosol

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B. Sierau

2014-07-01

Full Text Available Single-particle mass-spectrometric measurements were carried out in the high Arctic north of 80° during summer 2008. The campaign took place onboard the icebreaker Oden and was part of the Arctic Summer Cloud Ocean Study (ASCOS. The instrument deployed was an aerosol time-of-flight mass spectrometer (ATOFMS that provides information on the chemical composition of individual particles and their mixing state in real time. Aerosols were sampled in the marine boundary layer at stations in the open ocean, in the marginal ice zone, and in the pack ice region. The largest fraction of particles detected for subsequent analysis in the size range of the ATOFMS between approximately 200 and 3000 nm in diameter showed mass-spectrometric patterns, indicating an internal mixing state and a biomass burning and/or biofuel source. The majority of these particles were connected to an air mass layer of elevated particle concentration mixed into the surface mixed layer from the upper part of the marine boundary layer. The second largest fraction was represented by sea salt particles. The chemical analysis of the over-ice sea salt aerosol revealed tracer compounds that reflect chemical aging of the particles during their long-range advection from the marginal ice zone, or open waters south thereof prior to detection at the ship. From our findings we conclude that long-range transport of particles is one source of aerosols in the high Arctic. To assess the importance of long-range particle sources for aerosol–cloud interactions over the inner Arctic in comparison to local and regional biogenic primary aerosol sources, the chemical composition of the detected particles was analyzed for indicators of marine biological origin. Only a minor fraction showed chemical signatures of potentially ocean-derived primary particles of that kind. However, a chemical bias in the ATOFMS's detection capabilities observed during ASCOS might suggest the presence of a particle type of

Functional group composition of ambient and source organic aerosols determined by tandem mass spectrometry

Energy Technology Data Exchange (ETDEWEB)

Dron, J.; El Haddad, I.; Temime-Roussel, B.; Wortham, H.; Marchand, N. [Univ Aix Marseille, CNRS, Lab Chim Provence, Equipe Instrumentat and React Atmospher, UMR 6264, F-13331 Marseille 3 (France); Jaffrezo, J.L. [Univ Grenoble 1, CNRS, UMR 5183, Lab Glaciol and Geophys Environm, F-38402 St Martin Dheres (France)

2010-07-01

The functional group composition of various organic aerosols (OA) is investigated using a recently developed analytical approach based on atmospheric pressure chemical ionisation-tandem mass spectrometry (APCIMS/MS). The determinations of three functional groups contents are performed quantitatively by neutral loss (carboxylic and carbonyl groups, R-COOH and R-CO-R' respectively) and precursor ion (nitro groups, R-NO{sub 2}) scanning modes of a tandem mass spectrometer. Major organic aerosol sources are studied: vehicular emission and wood combustion for primary aerosol sources; and a secondary organic aerosol (SOA) produced through photooxidation of o-xylene. The results reveal significant differences in the functional group contents of these source aerosols. The laboratory generated SOA is dominated by carbonyls while carboxylics are preponderate in the wood combustion particles. On the other hand, vehicular emissions are characterised by a strong nitro content. The total amount of the three functional groups accounts for 1.7% (vehicular) to 13.5% (o-xylene photooxidation) of the organic carbon. Diagnostic functional group ratios are then used to tentatively discriminate sources of particles collected in an urban background environment located in an Alpine valley (Chamonix, France) during a strong winter pollution event. The three functional groups under study account for a total functionalization rate of 2.2 to 3.8% of the organic carbon in this ambient aerosol, which is also dominated by carboxylic moieties. In this particular case study of a deep alpine valley during winter, we show that the nitro- and carbonyl-to-carboxylic diagnostic ratios can be a useful tool to discriminate sources. In these conditions, the total OA concentrations are highly dominated by wood combustion OA. This result is confirmed by an organic markers source apportionment approach which assess a wood burning organic carbon contribution of about 60%. Finally, examples of functional

Functional group composition of ambient and source organic aerosols determined by tandem mass spectrometry

Directory of Open Access Journals (Sweden)

J. Dron

2010-08-01

Full Text Available The functional group composition of various organic aerosols (OA is investigated using a recently developed analytical approach based on atmospheric pressure chemical ionisation-tandem mass spectrometry (APCI-MS/MS. The determinations of three functional groups contents are performed quantitatively by neutral loss (carboxylic and carbonyl groups, R-COOH and R-CO-R´ respectively and precursor ion (nitro groups, R-NO₂ scanning modes of a tandem mass spectrometer. Major organic aerosol sources are studied: vehicular emission and wood combustion for primary aerosol sources; and a secondary organic aerosol (SOA produced through photooxidation of o-xylene. The results reveal significant differences in the functional group contents of these source aerosols. The laboratory generated SOA is dominated by carbonyls while carboxylics are preponderate in the wood combustion particles. On the other hand, vehicular emissions are characterised by a strong nitro content. The total amount of the three functional groups accounts for 1.7% (vehicular to 13.5% (o-xylene photooxidation of the organic carbon. Diagnostic functional group ratios are then used to tentatively discriminate sources of particles collected in an urban background environment located in an Alpine valley (Chamonix, France during a strong winter pollution event. The three functional groups under study account for a total functionalisation rate of 2.2 to 3.8% of the organic carbon in this ambient aerosol, which is also dominated by carboxylic moieties. In this particular case study of a deep alpine valley during winter, we show that the nitro- and carbonyl-to-carboxylic diagnostic ratios can be a useful tool to discriminate sources. In these conditions, the total OA concentrations are highly dominated by wood combustion OA. This result is confirmed by an organic markers source apportionment approach which assess a wood burning organic carbon contribution of about 60

Creating Aerosol Types from CHemistry (CATCH): A New Algorithm to Extend the Link Between Remote Sensing and Models

Science.gov (United States)

Dawson, K. W.; Meskhidze, N.; Burton, S. P.; Johnson, M. S.; Kacenelenbogen, M. S.; Hostetler, C. A.; Hu, Y.

2017-11-01

Current remote sensing methods can identify aerosol types within an atmospheric column, presenting an opportunity to incrementally bridge the gap between remote sensing and models. Here a new algorithm was designed for Creating Aerosol Types from CHemistry (CATCH). CATCH-derived aerosol types—dusty mix, maritime, urban, smoke, and fresh smoke—are based on first-generation airborne High Spectral Resolution Lidar (HSRL-1) retrievals during the Ship-Aircraft Bio-Optical Research (SABOR) campaign, July/August 2014. CATCH is designed to derive aerosol types from model output of chemical composition. CATCH-derived aerosol types are determined by multivariate clustering of model-calculated variables that have been trained using retrievals of aerosol types from HSRL-1. CATCH-derived aerosol types (with the exception of smoke) compare well with HSRL-1 retrievals during SABOR with an average difference in aerosol optical depth (AOD) methods. In the future, spaceborne HSRL-1 and CATCH can be used to gain insight into chemical composition of aerosol types, reducing uncertainties in estimates of aerosol radiative forcing.

Elemental and iron isotopic composition of aerosols collected in a parking structure

International Nuclear Information System (INIS)

Majestic, Brian J.; Anbar, Ariel D.; Herckes, Pierre

2009-01-01

The trace metal contents and iron isotope composition of size-resolved aerosols were determined in a parking structure in Tempe, AZ, USA. Particulate matter (PM) 2.5 μm were collected. Several air toxics (e.g., arsenic, cadmium, and antimony) were enriched above the crustal average, implicating automobiles as an important source. Extremely high levels of fine copper (up to 1000 ng m -3 ) were also observed in the parking garage, likely from brake wear. The iron isotope composition of the aerosols were found to be + 0.15 ± 0.03 per mille and + 0.18 ± 0.03 per mille for the PM 2.5 μm fractions, respectively. The similarity of isotope composition indicates a common source for each size fraction. To better understand the source of iron in the parking garage, the elemental composition in four brake pads (two semi-metallic and two ceramic), two tire tread samples, and two waste oil samples were determined. Striking differences in the metallic and ceramic brake pads were observed. The ceramic brake pads contained 10-20% copper by mass, while the metallic brake pads contained about 70% iron, with very little copper. Both waste oil samples contained significant amounts of calcium, phosphorous, and zinc, consistent with the composition of some engine oil additives. Differences in iron isotope composition were observed between the source materials; most notably between the tire tread (average = + 0.02 per mille ) and the ceramic brake linings (average = + 0.65 per mille ). Differences in isotopic composition were also observed between the metallic (average = + 0.18 per mille ) and ceramic brake pads, implying that iron isotope composition may be used to resolve these sources. The iron isotope composition of the metallic brake pads was found to be identical to the aerosols, implying that brake dust is the dominant source of iron in a parking garage.

Unraveling different chemical fingerprints between a champagne wine and its aerosols.

Science.gov (United States)

Liger-Belair, Gérard; Cilindre, Clara; Gougeon, Régis D; Lucio, Marianna; Gebefügi, Istvan; Jeandet, Philippe; Schmitt-Kopplin, Philippe

2009-09-29

As champagne or sparkling wine is poured into a glass, the myriad of ascending bubbles collapse and radiate a multitude of tiny droplets above the free surface into the form of very characteristic and refreshing aerosols. Ultrahigh-resolution MS was used as a nontargeted approach to discriminate hundreds of surface active compounds that are preferentially partitioning in champagne aerosols; thus, unraveling different chemical fingerprints between the champagne bulk and its aerosols. Based on accurate exact mass analysis and database search, tens of these compounds overconcentrating in champagne aerosols were unambiguously discriminated and assigned to compounds showing organoleptic interest or being aromas precursors. By drawing a parallel between the fizz of the ocean and the fizz in Champagne wines, our results closely link bursting bubbles and flavor release; thus, supporting the idea that rising and collapsing bubbles act as a continuous paternoster lift for aromas in every glass of champagne.

Primary and Secondary Organic Marine Aerosol and Oceanic Biological Activity: Recent Results and New Perspectives for Future Studies

Directory of Open Access Journals (Sweden)

Matteo Rinaldi

2010-01-01

Full Text Available One of the most important natural aerosol systems at the global level is marine aerosol that comprises both organic and inorganic components of primary and secondary origin. The present paper reviews some new results on primary and secondary organic marine aerosol, achieved during the EU project MAP (Marine Aerosol Production, comparing them with those reported in the recent literature. Marine aerosol samples collected at the coastal site of Mace Head, Ireland, show a chemical composition trend that is influenced by the oceanic biological activity cycle, in agreement with other observations. Laboratory experiments show that sea-spray aerosol from biologically active sea water can be highly enriched in organics, and the authors highlight the need for further studies on the atmospheric fate of such primary organics. With regard to the secondary fraction of organic aerosol, the average chemical composition and molecular tracer (methanesulfonic-acid, amines distribution could be successfully characterized by adopting a multitechnique analytical approach.

Chemical aging of single and multicomponent biomass burning aerosol surrogate particles by OH: implications for cloud condensation nucleus activity

Directory of Open Access Journals (Sweden)

J. H. Slade

2015-09-01

Full Text Available Multiphase OH and O3 oxidation reactions with atmospheric organic aerosol (OA can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low-soluble single-component OA by OH and O3 can increase their water solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA surrogate particles exposed to OH and O3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH and O3 exposure applying a CCN counter (CCNc coupled to an aerosol flow reactor (AFR. Levoglucosan (LEV, 4-methyl-5-nitrocatechol (MNC, and potassium sulfate (KS serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O3 exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~ 0.1, indicating that chemically aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH-exposed MNC-coated KS particles is similar to the OH unexposed atomized 1 : 1 by mass MNC : KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC or inorganic ions

Insights into Submicron Aerosol Composition and Sources from the WINTER Aircraft Campaign Over the Eastern US.

Science.gov (United States)

Schroder, J. C.; Campuzano Jost, P.; Day, D. A.; Fibiger, D. L.; McDuffie, E. E.; Blake, N. J.; Hills, A. J.; Hornbrook, R. S.; Apel, E. C.; Weinheimer, A. J.; Campos, T. L.; Brown, S. S.; Jimenez, J. L.

2015-12-01

The WINTER aircraft campaign was a recent field experiment to probe the sources and evolution of gas pollutants and aerosols in Northeast US urban and industrial plumes during the winter. A highly customized Aerodyne aerosol mass spectrometer (AMS) was flown on the NCAR C-130 to characterize submicron aerosol composition and evolution. Thirteen research flights were conducted covering a wide range of conditions, including rural, urban, and marine environments during day and night. Organic aerosol (OA) was a large component of the submicron aerosol in the boundary layer. The fraction of OA (fOA) was smaller (35-40%) than in recent US summer campaigns (~60-70%). Biomass burning was observed to be an important source of OA in the boundary layer, which is consistent with recent wintertime studies that show a substantial contribution of residential wood burning to the OA loadings. OA oxygenation (O/C ratio) shows a broad distribution with a substantial fraction of smaller O/C ratios when compared to previous summertime campaigns. Since measurements were rarely made very close to primary sources (i.e. directly above urban areas), this is consistent with oxidative chemistry being slower during winter. SOA formation and aging in the NYC plume was observed during several flights and compared with summertime results from LA (CalNex) and Mexico City (MILAGRO). Additionally, an oxidation flow reactor (OFR) capable of oxidizing ambient air up to several equivalent days of oxidation was deployed for the first time in an aircraft platform. The aerosol outflow of the OFR was sampled with the AMS to provide real-time snapshots of the potential for aerosol formation and aging. For example, a case study of a flight through the Ohio River valley showed evidence of oxidation of SO2 to sulfate. The measured sulfate enhancements were in good agreement with our OFR chemical model. OFR results for SOA will be discussed.

Effect of Heterogeneous Chemical Reactions on the Köhler Activation of Aqueous Organic Aerosols.

Science.gov (United States)

Djikaev, Yuri S; Ruckenstein, Eli

2018-05-03

We study some thermodynamic aspects of the activation of aqueous organic aerosols into cloud droplets considering the aerosols to consist of liquid solution of water and hydrophilic and hydrophobic organic compounds, taking into account the presence of reactive species in the air. The hydrophobic (surfactant) organic molecules on the surface of such an aerosol can be processed by chemical reactions with some atmospheric species; this affects the hygroscopicity of the aerosol and hence its ability to become a cloud droplet either via nucleation or via Köhler activation. The most probable pathway of such processing involves atmospheric hydroxyl radicals that abstract hydrogen atoms from hydrophobic organic molecules located on the aerosol surface (first step), the resulting radicals being quickly oxidized by ubiquitous atmospheric oxygen molecules to produce surface-bound peroxyl radicals (second step). These two reactions play a crucial role in the enhancement of the Köhler activation of the aerosol and its evolution into a cloud droplet. Taking them and a third reaction (next in the multistep chain of relevant heterogeneous reactions) into account, one can derive an explicit expression for the free energy of formation of a four-component aqueous droplet on a ternary aqueous organic aerosol as a function of four independent variables of state of a droplet. The results of numerical calculations suggest that the formation of cloud droplets on such (aqueous hydrophilic/hydrophobic organic) aerosols is most likely to occur as a Köhler activation-like process rather than via nucleation. The model allows one to determine the threshold parameters of the system necessary for the Köhler activation of such aerosols, which are predicted to be very sensitive to the equilibrium constant of the chain of three heterogeneous reactions involved in the chemical aging of aerosols.

Uncertainty in Predicting CCN Activity of Aged and Primary Aerosols

Science.gov (United States)

Zhang, Fang; Wang, Yuying; Peng, Jianfei; Ren, Jingye; Collins, Don; Zhang, Renyi; Sun, Yele; Yang, Xin; Li, Zhanqing

2017-11-01

Understanding particle CCN activity in diverse atmospheres is crucial when evaluating aerosol indirect effects. Here aerosols measured at three sites in China were categorized as different types for attributing uncertainties in CCN prediction in terms of a comprehensive data set including size-resolved CCN activity, size-resolved hygroscopic growth factor, and chemical composition. We show that CCN activity for aged aerosols is unexpectedly underestimated 22% at a supersaturation (S) of 0.2% when using κ-Kohler theory with an assumption of an internal mixture with measured bulk composition that has typically resulted in an overestimate of the CCN activity in previous studies. We conclude that the underestimation stems from neglect of the effect of aging/coating on particle hygroscopicity, which is not considered properly in most current models. This effect enhanced the hygroscopicity parameter (κ) by between 11% (polluted conditions) and 30% (clean days), as indicated in diurnal cycles of κ based on measurements by different instruments. In the urban Beijing atmosphere heavily influenced by fresh emissions, the CCN activity was overestimated by 45% at S = 0.2%, likely because of inaccurate assumptions of particle mixing state and because of variability of chemical composition over the particle size range. For both fresh and aged aerosols, CCN prediction exhibits very limited sensitivity to κSOA, implying a critical role of other factors like mixing of aerosol components within and between particles in regulating CCN activity. Our findings could help improving CCN parameterization in climate models.

Functional group analysis by H NMR/chemical derivatization for the characterization of organic aerosol from the SMOCC field campaign

Directory of Open Access Journals (Sweden)

E. Tagliavini

2006-01-01

Full Text Available Water soluble organic compounds (WSOC in aerosol samples collected in the Amazon Basin in a period encompassing the middle/late dry season and the beginning of the wet season, were investigated by H NMR spectroscopy. HiVol filter samples (PM2.5 and PM>2.5 and size-segregated samples from multistage impactor were subjected to H NMR characterization. The H NMR methodology, recently developed for the analysis of organic aerosol samples, has been improved by exploiting chemical methylation of carboxylic groups with diazomethane, which allows the direct determination of the carboxylic acid content of WSOC. The content of carboxylic carbons for the different periods and sizes ranged from 12% to 20% of total measured carbon depending on the season and aerosol size, with higher contents for the fine particles in the transition and wet periods with respect to the dry period. A comprehensive picture is presented of WSOC functional groups in aerosol samples representative of the biomass burning period, as well as of transition and semi-clean atmospheric conditions. A difference in composition between fine (PM2.5 and coarse (PM>2.5 size fractions emerged from the NMR data, the former showing higher alkylic content, the latter being largely dominated by R-O-H (or R-O-R' functional groups. Very small particles (<0.14 μm, however, present higher alkyl-chain content and less oxygenated carbons than larger fine particles (0.42–1.2 μm. More limited variations were found between the average compositions in the different periods of the campaign.

Atmospheric Aerosol Emissions Related to the Mediterranean Seawater Biogeochemistry

Science.gov (United States)

Sellegri, K.; Schwier, A.; Rose, C.; Gazeau, F. P. H.; Guieu, C.; D'anna, B.; Ebling, A. M.; Pey, J.; Marchand, N.; Charriere, B.; Sempéré, R.; Mas, S.

2016-02-01

Marine aerosols contribute significantly to the global aerosol load and consequently has an important impact on the Earth's climate. Different factors influence the way they are produced at the air/seawater interface. The sea state (whitecap coverage, temperature, etc. ) influence the size and concentration of primarily produced particles but also biogeochemical characteristics of the seawater influence both the physical and chemical primary fluxes to the atmosphere. An additional aerosol source of marine aerosol to the atmosphere is the formation of new particles by gaz-to-particle conversion, i.e. nucleation. How the seawater and surface microlayer biogeochemical compositions influences the aerosol emissions is still a large debate. In order to study marine emissions, one approach is to use semi-controlled environments such as mesocosms. Within the MedSea and SAM projects, we characterize the primary Sea Spray Aerosol (SSA) during mesocosms experiments performed during different seasons in the Mediteranean Sea. Mesocosms were either left unchanged as control or enriched by addition of nutriments in order to create different levels of phytoplanctonic activities. The mesocosms waters were daily analyzed for their chemical and biological composition (DOC, CDOM, TEP, Chl-a, virus, bacteria, phytoplankton and zooplankton concentrations). SSA production by bubble bursting was daily simulated in a dedicated set-up. The size segregated SSA number fluxes, cloud condensation nuclei (CCN) properties, and chemical composition were determined as a function of the seawater characteristics. We show that the SSA organic content was clearly correlated to the seawater Chl-a level, provided that the mesocosm was not enriched to create an artificial phytoplanctonic bloom. In our experiments, the enrichment of the seawater with natural surface microlayer did not impact the SSA organic content nor its CCN properties. At last, nucleation of secondary particles were observed to occur in

A GCM study of organic matter in marine aerosol and its potential contribution to cloud drop activation

NARCIS (Netherlands)

Roelofs, G.J.H.

2007-01-01

With the global aerosol-climate model ECHAM5-HAM we investigate the potential influence of organic aerosol originating from the ocean on aerosol mass and chemical composition and the droplet concentration and size of marine clouds. We present sensitivity simulations in which the uptake of organic

Seasonal variations in aerosol particle composition at the puy-de-Dôme research station in France

Directory of Open Access Journals (Sweden)

E. J. Freney

2011-12-01

Full Text Available Detailed investigations of the chemical and microphysical properties of atmospheric aerosol particles were performed at the puy-de-Dôme (pdD research station (1465 m in autumn (September and October 2008, winter (February and March 2009, and summer (June 2010 using a compact Time-of-Flight Aerosol Mass Spectrometer (cToF-AMS. Over the three campaigns, the average mass concentrations of the non-refractory submicron particles ranged from 10 μg m⁻³ up to 27 μg m⁻³. Highest nitrate and ammonium mass concentrations were measured during the winter and during periods when marine modified airmasses were arriving at the site, whereas highest concentrations of organic particles were measured during the summer and during periods when continental airmasses arrived at the site. The measurements reported in this paper show that atmospheric particle composition is strongly influenced by both the season and the origin of the airmass. The total organic mass spectra were analysed using positive matrix factorisation to separate individual organic components contributing to the overall organic particle mass concentrations. These organic components include a low volatility oxygenated organic aerosol particle (LV-OOA and a semi-volatile organic aerosol particle (SV-OOA. Correlations of the LV-OOA components with fragments of m/z 60 and m/z 73 (mass spectral markers of wood burning during the winter campaign suggest that wintertime LV-OOA are related to aged biomass burning emissions, whereas organic aerosol particles measured during the summer are likely linked to biogenic sources. Equivalent potential temperature calculations, gas-phase, and LIDAR measurements define whether the research site is in the planetary boundary layer (PBL or in the free troposphere (FT/residual layer (RL. We observe that SV-OOA and nitrate particles are associated with air masses arriving from the PBL where as particle composition measured from RL

Inorganic Salt Interference on CO2+ in Aerodyne AMS and ACSM Organic Aerosol Composition Studies.

Science.gov (United States)

Pieber, Simone M; El Haddad, Imad; Slowik, Jay G; Canagaratna, Manjula R; Jayne, John T; Platt, Stephen M; Bozzetti, Carlo; Daellenbach, Kaspar R; Fröhlich, Roman; Vlachou, Athanasia; Klein, Felix; Dommen, Josef; Miljevic, Branka; Jiménez, José L; Worsnop, Douglas R; Baltensperger, Urs; Prévôt, André S H

2016-10-04

Aerodyne aerosol mass spectrometer (AMS) and Aerodyne aerosol chemical speciation monitor (ACSM) mass spectra are widely used to quantify organic aerosol (OA) elemental composition, oxidation state, and major environmental sources. The OA CO 2 + fragment is among the most important measurements for such analyses. Here, we show that a non-OA CO 2 + signal can arise from reactions on the particle vaporizer, ion chamber, or both, induced by thermal decomposition products of inorganic salts. In our tests (eight instruments, n = 29), ammonium nitrate (NH 4 NO 3 ) causes a median CO 2 + interference signal of +3.4% relative to nitrate. This interference is highly variable between instruments and with measurement history (percentiles P 10-90 = +0.4 to +10.2%). Other semi-refractory nitrate salts showed 2-10 times enhanced interference compared to that of NH 4 NO 3 , while the ammonium sulfate ((NH 4 ) 2 SO 4 ) induced interference was 3-10 times lower. Propagation of the CO 2 + interference to other ions during standard AMS and ACSM data analysis affects the calculated OA mass, mass spectra, molecular oxygen-to-carbon ratio (O/C), and f 44 . The resulting bias may be trivial for most ambient data sets but can be significant for aerosol with higher inorganic fractions (>50%), e.g., for low ambient temperatures, or laboratory experiments. The large variation between instruments makes it imperative to regularly quantify this effect on individual AMS and ACSM systems.

Secondary organic aerosol in the global aerosol – chemical transport model Oslo CTM2

Directory of Open Access Journals (Sweden)

I. S. A. Isaksen

2007-11-01

Full Text Available The global chemical transport model Oslo CTM2 has been extended to include the formation, transport and deposition of secondary organic aerosol (SOA. Precursor hydrocarbons which are oxidised to form condensible species include both biogenic species such as terpenes and isoprene, as well as species emitted predominantly by anthropogenic activities (toluene, m-xylene, methylbenzene and other aromatics. A model simulation for 2004 gives an annual global SOA production of approximately 55 Tg. Of this total, 2.5 Tg is found to consist of the oxidation products of anthropogenically emitted hydrocarbons, and about 15 Tg is formed by the oxidation products of isoprene. The global production of SOA is increased to about 69 Tg yr−1 by allowing semi-volatile species to partition to ammonium sulphate aerosol. This brings modelled organic aerosol values closer to those observed, however observations in Europe remain significantly underestimated. Allowing SOA to partition into ammonium sulphate aerosol increases the contribution of anthropogenic SOA from about 4.5% to 9.4% of the total production. Total modelled organic aerosol (OA values are found to represent a lower fraction of the measured values in winter (when primary organic aerosol (POA is the dominant OA component than in summer, which may be an indication that estimates of POA emissions are too low. Additionally, for measurement stations where the summer OA values are higher than in winter, the model generally underestimates the increase in summertime OA. In order to correctly model the observed increase in OA in summer, additional SOA sources or formation mechanisms may be necessary. The importance of NO3 as an oxidant of SOA precursors is found to vary regionally, causing up to 50%–60% of the total amount of SOA near the surface in polluted regions and less than 25% in more remote areas, if the yield of condensible oxidation products for β-pinene is used for NO3 oxidation of all terpenes

Development and Characterization of a Thermodenuder for Aerosol Volatility Measurements

Energy Technology Data Exchange (ETDEWEB)

Dr. Timothy Onasch

2009-09-09

This SBIR Phase I project addressed the critical need for improved characterization of carbonaceous aerosol species in the atmosphere. The proposed work focused on the development of a thermodenuder (TD) system capable of systematically measuring volatility profiles of primary and secondary organic aerosol species and providing insight into the effects of absorbing and nonabsorbing organic coatings on particle absorption properties. This work provided the fundamental framework for the generation of essential information needed for improved predictions of ambient aerosol loadings and radiative properties by atmospheric chemistry models. As part of this work, Aerodyne Research, Inc. (ARI) continued to develop and test, with the final objective of commercialization, an improved thermodenuder system that can be used in series with any aerosol instrument or suite of instruments (e.g., aerosol mass spectrometers-AMS, scanning mobility particle sizers-SMPS, photoacoustic absorption spectrometers-PAS, etc.) to obtain aerosol chemical, physical, and optical properties as a function of particle volatility. In particular, we provided the proof of concept for the direct coupling of our improved TD design with a full microphysical model to obtain volatility profiles for different organic aerosol components and to allow for meaningful comparisons between different TD-derived aerosol measurements. In a TD, particles are passed through a heated zone and a denuding (activated charcoal) zone to remove semi-volatile material. Changes in particle size, number concentration, optical absorption, and chemical composition are subsequently detected with aerosol instrumentation. The aerosol volatility profiles provided by the TD will strengthen organic aerosol emission inventories, provide further insight into secondary aerosol formation mechanisms, and provide an important measure of particle absorption (including brown carbon contributions and identification, and absorption enhancements

Relating hygroscopicity and composition of organic aerosol particulate matter

CERN Document Server

Duplissy, J; Prevot, A S H; Barmpadimos, I; Jimenez, J L; Gysel, M; Worsnop, D R; Aiken, A C; Tritscher, T; Canagaratna, M R; Collins, D R; Alfarra, M R; Metzger, A; Tomlinson, J; DeCarlo, P F; Weingartner, E; Baltensperger, U

2011-01-01

A hygroscopicity tandem differential mobility analyzer (HTDMA) was used to measure the water uptake (hygroscopicity) of secondary organic aerosol (SOA) formed during the chemical and photochemical oxidation of several organic precursors in a smog chamber. Electron ionization mass spectra of the non-refractory submicron aerosol were simultaneously determined with an aerosol mass spectrometer (AMS), and correlations between the two different signals were investigated. SOA hygroscopicity was found to strongly correlate with the relative abundance of the ion signal m/z 44 expressed as a fraction of total organic signal (f(44)). m/z 44 is due mostly to the ion fragment CO(2)(+) for all types of SOA systems studied, and has been previously shown to strongly correlate with organic O/C for ambient and chamber OA. The analysis was also performed on ambient OA from two field experiments at the remote site Jungfrau-joch, and the megacity Mexico City, where similar results were found. A simple empirical linear relation b...

The impact of aerosol composition on the particle to gas partitioning of reactive mercury.

Science.gov (United States)

Rutter, Andrew P; Schauer, James J

2007-06-01

A laboratory system was developed to study the gas-particle partitioning of reactive mercury (RM) as a function of aerosol composition in synthetic atmospheric particulate matter. The collection of RM was achieved by filter- and sorbent-based methods. Analyses of the RM collected on the filters and sorbents were performed using thermal extraction combined with cold vapor atomic fluorescence spectroscopy (CVAFS), allowing direct measurement of the RM load on the substrates. Laboratory measurements of the gas-particle partitioning coefficients of RM to atmospheric aerosol particles revealed a strong dependence on aerosol composition, with partitioning coefficients that varied by orders of magnitude depending on the composition of the particles. Particles of sodium nitrate and the chlorides of potassium and sodium had high partitioning coefficients, shifting the RM partitioning toward the particle phase, while ammonium sulfate, levoglucosan, and adipic acid caused the RM to partition toward the gas phase and, therefore, had partitioning coefficients that were lower by orders of magnitude.

Linking variations in sea spray aerosol particle hygroscopicity to composition during two microcosm experiments

Directory of Open Access Journals (Sweden)

S. D. Forestieri

2016-07-01

Full Text Available The extent to which water uptake influences the light scattering ability of marine sea spray aerosol (SSA particles depends critically on SSA chemical composition. The organic fraction of SSA can increase during phytoplankton blooms, decreasing the salt content and therefore the hygroscopicity of the particles. In this study, subsaturated hygroscopic growth factors at 85 % relative humidity (GF(85 % of predominately submicron SSA particles were quantified during two induced phytoplankton blooms in marine aerosol reference tanks (MARTs. One MART was illuminated with fluorescent lights and the other was illuminated with sunlight, referred to as the "indoor" and "outdoor" MARTs, respectively. Optically weighted GF(85 % values for SSA particles were derived from measurements of light scattering and particle size distributions. The mean optically weighted SSA diameters were 530 and 570 nm for the indoor and outdoor MARTs, respectively. The GF(85 % measurements were made concurrently with online particle composition measurements, including bulk composition (using an Aerodyne high-resolution aerosol mass spectrometer and single particle (using an aerosol time-of-flight mass spectrometer measurement, and a variety of water-composition measurements. During both microcosm experiments, the observed optically weighted GF(85 % values were depressed substantially relative to pure inorganic sea salt by 5 to 15 %. There was also a time lag between GF(85 % depression and the peak chlorophyll a (Chl a concentrations by either 1 (indoor MART or 3-to-6 (outdoor MART days. The fraction of organic matter in the SSA particles generally increased after the Chl a peaked, also with a time lag, and ranged from about 0.25 to 0.5 by volume. The observed depression in the GF(85 % values (relative to pure sea salt is consistent with the large observed volume fractions of non-refractory organic matter (NR-OM comprising the SSA. The GF(85 % values

Chemical compositions, sources and evolution processes of the submicron aerosols in Nanjing, China during wintertime

Science.gov (United States)

Wu, Y.; He, Y.; Ge, X.; Wang, J.; Yu, H.; Chen, M.

2016-12-01

Elevated atmospheric particulate matter pollution is one of the most significant environmental issues in the Yangtze River Delta (YRD), China. Thus it is important to unravel the characteristics, sources and evolution processes of the ambient aerosols in order to improve the air quality. In this study, we report the real-time monitoring results on submicron aerosol particles (PM1) in suburban Nanjing during wintertime of 2015, using an Aerodyne soot particle aerosol mass spectrometer (SP-AMS). This instrument allows the fast measurement of refractory black carbon simultaneously with other aerosol components. Results show that organics was on average the most abundant species of PM1 (25.9%), but other inorganic species, such as nitrate (23.7%) and sulfate (23.3%) also comprised large mass fractions. As the sampling site is heavily influenced by various sources including industrial, traffic and other anthropogenic emissions, etc., six organic aerosol (OA) factors were identified from Positive matrix factorization (PMF) analysis of the SP-AMS OA mass spectra. These factors include three primary OA factors - a hydrocarbon-like OA, an industry-related OA (IOA) and a cooking OA (COA), and three secondary OA factors, i.e., a local OOA (LSOA), a semi-volatile OOA (SV-OOA) and a low-volatility OOA (LV-OOA). Overall, the primary organic aerosol (POA) (HOA, IOA and COA) dominated the total OA mass. Behaviors and evolution processes of these OA factors will be discussed in combining with the other supporting data.

Temperature effect on physical and chemical properties of secondary organic aerosol from m-xylene photooxidation

Directory of Open Access Journals (Sweden)

D. R. Cocker III

2010-04-01

Full Text Available The chemical and physical differences of secondary organic aerosol (SOA formed at select isothermal temperatures (278 K, 300 K, and 313 K are explored with respect to density, particle volatility, particle hygroscopicity, and elemental chemical composition. A transition point in SOA density, volatility, hygroscopicity and elemental composition is observed near 290–292 K as SOA within an environmental chamber is heated from 278 K to 313 K, indicating the presence of a thermally labile compound. No such transition points are observed for SOA produced at 313 K or 300 K and subsequently cooled to 278 K. The SOA formed at the lowest temperatures (278 K is more than double the SOA formed at 313 K. SOA formed at 278 K is less hydrophilic and oxygenated while more volatile and dense than SOA formed at 300 K or 313 K. The properties of SOA formed at 300 K and 313 K when reduced to 278 K did not match the properties of SOA initially formed at 278 K. This study demonstrates that it is insufficient to utilize the enthalpy of vaporization when predicting SOA temperature dependence.

Cloud-Driven Changes in Aerosol Optical Properties - Final Technical Report

Energy Technology Data Exchange (ETDEWEB)

Ogren, John A.; Sheridan, Patrick S.; Andrews, Elisabeth

2007-09-30

The optical properties of aerosol particles are the controlling factors in determining direct aerosol radiative forcing. These optical properties depend on the chemical composition and size distribution of the aerosol particles, which can change due to various processes during the particles’ lifetime in the atmosphere. Over the course of this project we have studied how cloud processing of atmospheric aerosol changes the aerosol optical properties. A counterflow virtual impactor was used to separate cloud drops from interstitial aerosol and parallel aerosol systems were used to measure the optical properties of the interstitial and cloud-scavenged aerosol. Specifically, aerosol light scattering, back-scattering and absorption were measured and used to derive radiatively significant parameters such as aerosol single scattering albedo and backscatter fraction for cloud-scavenged and interstitial aerosol. This data allows us to demonstrate that the radiative properties of cloud-processed aerosol can be quite different than pre-cloud aerosol. These differences can be used to improve the parameterization of aerosol forcing in climate models.

Enhancing non-refractory aerosol apportionment from an urban industrial site through receptor modeling of complete high time-resolution aerosol mass spectra

Science.gov (United States)

McGuire, M. L.; Chang, R. Y.-W.; Slowik, J. G.; Jeong, C.-H.; Healy, R. M.; Lu, G.; Mihele, C.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

2014-08-01

Receptor modeling was performed on quadrupole unit mass resolution aerosol mass spectrometer (Q-AMS) sub-micron particulate matter (PM) chemical speciation measurements from Windsor, Ontario, an industrial city situated across the Detroit River from Detroit, Michigan. Aerosol and trace gas measurements were collected on board Environment Canada's Canadian Regional and Urban Investigation System for Environmental Research (CRUISER) mobile laboratory. Positive matrix factorization (PMF) was performed on the AMS full particle-phase mass spectrum (PMFFull MS) encompassing both organic and inorganic components. This approach compared to the more common method of analyzing only the organic mass spectra (PMFOrg MS). PMF of the full mass spectrum revealed that variability in the non-refractory sub-micron aerosol concentration and composition was best explained by six factors: an amine-containing factor (Amine); an ammonium sulfate- and oxygenated organic aerosol-containing factor (Sulfate-OA); an ammonium nitrate- and oxygenated organic aerosol-containing factor (Nitrate-OA); an ammonium chloride-containing factor (Chloride); a hydrocarbon-like organic aerosol (HOA) factor; and a moderately oxygenated organic aerosol factor (OOA). PMF of the organic mass spectrum revealed three factors of similar composition to some of those revealed through PMFFull MS: Amine, HOA and OOA. Including both the inorganic and organic mass proved to be a beneficial approach to analyzing the unit mass resolution AMS data for several reasons. First, it provided a method for potentially calculating more accurate sub-micron PM mass concentrations, particularly when unusual factors are present, in this case the Amine factor. As this method does not rely on a priori knowledge of chemical species, it circumvents the need for any adjustments to the traditional AMS species fragmentation patterns to account for atypical species, and can thus lead to more complete factor profiles. It is expected that this

Enhancing non-refractory aerosol apportionment from an urban industrial site through receptor modelling of complete high time-resolution aerosol mass spectra

Science.gov (United States)

McGuire, M. L.; Chang, R. Y.-W.; Slowik, J. G.; Jeong, C.-H.; Healy, R. M.; Lu, G.; Mihele, C.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

2014-02-01

Receptor modelling was performed on quadrupole unit mass resolution aerosol mass spectrometer (Q-AMS) sub-micron particulate matter (PM) chemical speciation measurements from Windsor, Ontario, an industrial city situated across the Detroit River from Detroit, Michigan. Aerosol and trace gas measurements were collected on board Environment Canada's CRUISER mobile laboratory. Positive matrix factorization (PMF) was performed on the AMS full particle-phase mass spectrum (PMFFull MS) encompassing both organic and inorganic components. This approach was compared to the more common method of analysing only the organic mass spectra (PMFOrg MS). PMF of the full mass spectrum revealed that variability in the non-refractory sub-micron aerosol concentration and composition was best explained by six factors: an amine-containing factor (Amine); an ammonium sulphate and oxygenated organic aerosol containing factor (Sulphate-OA); an ammonium nitrate and oxygenated organic aerosol containing factor (Nitrate-OA); an ammonium chloride containing factor (Chloride); a hydrocarbon-like organic aerosol (HOA) factor; and a moderately oxygenated organic aerosol factor (OOA). PMF of the organic mass spectrum revealed three factors of similar composition to some of those revealed through PMFFull MS: Amine, HOA and OOA. Including both the inorganic and organic mass proved to be a beneficial approach to analysing the unit mass resolution AMS data for several reasons. First, it provided a method for potentially calculating more accurate sub-micron PM mass concentrations, particularly when unusual factors are present, in this case, an Amine factor. As this method does not rely on a priori knowledge of chemical species, it circumvents the need for any adjustments to the traditional AMS species fragmentation patterns to account for atypical species, and can thus lead to more complete factor profiles. It is expected that this method would be even more useful for HR-ToF-AMS data, due to the ability

Stratospheric aerosols and precursor gases

Science.gov (United States)

1982-01-01

Measurements were made of the aerosol size, height and geographical distribution, their composition and optical properties, and their temporal variation with season and following large volcanic eruptions. Sulfur-bearing gases were measured in situ in the stratosphere, and studied of the chemical and physical processes which control gas-to-particle conversion were carried out in the laboratory.

Small scale studies of production of fissium aerosols

International Nuclear Information System (INIS)

Lindqvist, O.; Rydberg, J.

1983-02-01

A small scale study concerning the production and analysis of fission product aerosols formed at various temperatures as a function of the chemical composition of the fissium/corium mixture at the source is presented. CsOH, CsJ and Te are the main aerosol components to be expected. The thermodynamic characterization of occuring Te-iodides and other phases is of great importance for reactor core meltdown chemistry and for the evaluation of the aerosol transport tests. Elemental iodine seems not to be released in significant amounts in reducing atmosphere. Analysis data concerning elements, phases, themral analysis and gases are presented. (G.B.)

Marine Emissions and Atmospheric Processing Influence Aerosol Mixing States in the Bering Strait and Chukchi Sea

Science.gov (United States)

Kirpes, R.; Rodriguez, B.; Kim, S.; Park, K.; China, S.; Laskin, A.; Pratt, K.

2017-12-01

The Arctic region is rapidly changing due to sea ice loss and increasing oil/gas development and shipping activity. These changes influence aerosol sources and composition, resulting in complex aerosol-cloud-climate feedbacks. Atmospheric particles were collected aboard the R/V Araon in July-August 2016 in the Alaskan Arctic along the Bering Strait and Chukchi Sea. Offline analysis of individual particles by microscopic and spectroscopic techniques provided information on particle size, morphology, and chemical composition. Sea spray aerosol (SSA) and organic aerosol (OA) particles were the most commonly observed particle types, and sulfate was internally mixed with both SSA and OA. Evidence of multiphase sea spray aerosol reactions was observed, with varying degrees of chlorine depletion observed along the cruise. Notably, atmospherically processed SSA, completely depleted in chlorine, and internally mixed organic and sulfate particles, were observed in samples influenced by the central Arctic Ocean. Changes in particle composition due to fog processing were also investigated. Due to the changing aerosol sources and atmospheric processes in the Arctic region, it is crucial to understand aerosol composition in order to predict climate impacts.

A GCM study of organic matter in marine aerosol and its potential contribution to cloud drop activation

Directory of Open Access Journals (Sweden)

G. J. Roelofs

2008-02-01

Full Text Available With the global aerosol-climate model ECHAM5-HAM we investigate the potential influence of organic aerosol originating from the ocean on aerosol mass and chemical composition and the droplet concentration and size of marine clouds. We present sensitivity simulations in which the uptake of organic matter in the marine aerosol is prescribed for each aerosol mode with varying organic mass and mixing state, and with a geographical distribution and seasonality similar to the oceanic emission of dimethyl sulfide. Measurements of aerosol mass, aerosol chemical composition and cloud drop effective radius are used to assess the representativity of the model initializations. Good agreement with the measurements is obtained when organic matter is added to the Aitken, accumulation and coarse modes simultaneously. Representing marine organics in the model leads to higher cloud drop number concentrations and thus smaller cloud drop effective radii, and this improves the agreement with measurements. The mixing state of the organics and the other aerosol matter, i.e. internal or external depending on the formation process of aerosol organics, is an important factor for this. We estimate that globally about 75 Tg C yr⁻¹ of organic matter from marine origin enters the aerosol phase, with comparable contributions from primary emissions and secondary organic aerosol formation.

Chemical interactions between aerosols and vapors in the primary circuit of an LWR during a severe accident

International Nuclear Information System (INIS)

Wheatley, C.J.

1988-01-01

Aerosol formation, agglomeration, convection and deposition within the primary circuit of an LWR during a severe accident significantly affect the transport of fission products, even though they may compose only a small fraction of the aerosol material. Intra-particle and vapor chemical interactions are important to this through mass transfer between the aerosol and vapor. The authors will describe a model that attempts to account for these processes and of the two-way coupling that exists with the thermal hydraulics. They will discuss what agglomeration and deposition mechanisms must be included, alternatives for treating intra-particle chemical interactions, mechanisms of aerosol formation, and methods for solving the resulting equations. Results will be presented that illustrate the importance of treating the two-way coupling and the extent to which disequilibrium between the aerosol and vapor affects fission product behavior

Can Condensing Organic Aerosols Lead to Less Cloud Particles?

Science.gov (United States)

Gao, C. Y.; Tsigaridis, K.; Bauer, S.

2017-12-01

We examined the impact of condensing organic aerosols on activated cloud number concentration in a new aerosol microphysics box model, MATRIX-VBS. The model includes the volatility-basis set (VBS) framework in an aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state) that resolves aerosol mass and number concentrations and aerosol mixing state. Preliminary results show that by including the condensation of organic aerosols, the new model (MATRIX-VBS) has less activated particles compared to the original model (MATRIX), which treats organic aerosols as non-volatile. Parameters such as aerosol chemical composition, mass and number concentrations, and particle sizes which affect activated cloud number concentration are thoroughly evaluated via a suite of Monte-Carlo simulations. The Monte-Carlo simulations also provide information on which climate-relevant parameters play a critical role in the aerosol evolution in the atmosphere. This study also helps simplifying the newly developed box model which will soon be implemented in the global model GISS ModelE as a module.

Aerosol activation and cloud processing in the global aerosol-climate model ECHAM5-HAM

Directory of Open Access Journals (Sweden)

G. J. Roelofs

2006-01-01

Full Text Available A parameterization for cloud processing is presented that calculates activation of aerosol particles to cloud drops, cloud drop size, and pH-dependent aqueous phase sulfur chemistry. The parameterization is implemented in the global aerosol-climate model ECHAM5-HAM. The cloud processing parameterization uses updraft speed, temperature, and aerosol size and chemical parameters simulated by ECHAM5-HAM to estimate the maximum supersaturation at the cloud base, and subsequently the cloud drop number concentration (CDNC due to activation. In-cloud sulfate production occurs through oxidation of dissolved SO2 by ozone and hydrogen peroxide. The model simulates realistic distributions for annually averaged CDNC although it is underestimated especially in remote marine regions. On average, CDNC is dominated by cloud droplets growing on particles from the accumulation mode, with smaller contributions from the Aitken and coarse modes. The simulations indicate that in-cloud sulfate production is a potentially important source of accumulation mode sized cloud condensation nuclei, due to chemical growth of activated Aitken particles and to enhanced coalescence of processed particles. The strength of this source depends on the distribution of produced sulfate over the activated modes. This distribution is affected by uncertainties in many parameters that play a direct role in particle activation, such as the updraft velocity, the aerosol chemical composition and the organic solubility, and the simulated CDNC is found to be relatively sensitive to these uncertainties.

Seasonal variations in high time-resolved chemical compositions, sources, and evolution of atmospheric submicron aerosols in the megacity Beijing

Science.gov (United States)

Hu, Wei; Hu, Min; Hu, Wei-Wei; Zheng, Jing; Chen, Chen; Wu, Yusheng; Guo, Song

2017-08-01

A severe regional haze problem in the megacity Beijing and surrounding areas, caused by fast formation and growth of fine particles, has attracted much attention in recent years. In order to investigate the secondary formation and aging process of urban aerosols, four intensive campaigns were conducted in four seasons between March 2012 and March 2013 at an urban site in Beijing (116.31° E, 37.99° N). An Aerodyne high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS) was deployed to measure non-refractory chemical components of submicron particulate matter (NR-PM1). The average mass concentrations of PM1 (NR-PM1+black carbon) were 45.1 ± 45.8, 37.5 ± 31.0, 41.3 ± 42.7, and 81.7 ± 72.4 µg m-3 in spring, summer, autumn, and winter, respectively. Organic aerosol (OA) was the most abundant component in PM1, accounting for 31, 33, 44, and 36 % seasonally, and secondary inorganic aerosol (SNA, sum of sulfate, nitrate, and ammonium) accounted for 59, 57, 43, and 55 % of PM1 correspondingly. Based on the application of positive matrix factorization (PMF), the sources of OA were obtained, including the primary ones of hydrocarbon-like (HOA), cooking (COA), biomass burning OA (BBOA) and coal combustion OA (CCOA), and secondary component oxygenated OA (OOA). OOA, which can be split into more-oxidized (MO-OOA) and less-oxidized OOA (LO-OOA), accounted for 49, 69, 47, and 50 % in four seasons, respectively. Totally, the fraction of secondary components (OOA+SNA) contributed about 60-80 % to PM1, suggesting that secondary formation played an important role in the PM pollution in Beijing, and primary sources were also non-negligible. The evolution process of OA in different seasons was investigated with multiple metrics and tools. The average carbon oxidation states and other metrics show that the oxidation state of OA was the highest in summer, probably due to both strong photochemical and aqueous-phase oxidations. It was indicated by the good correlations

Variation in global chemical composition of PM2.5: emerging results from SPARTAN

Science.gov (United States)

Snider, Graydon; Weagle, Crystal L.; Murdymootoo, Kalaivani K.; Ring, Amanda; Ritchie, Yvonne; Stone, Emily; Walsh, Ainsley; Akoshile, Clement; Anh, Nguyen Xuan; Balasubramanian, Rajasekhar; Brook, Jeff; Qonitan, Fatimah D.; Dong, Jinlu; Griffith, Derek; He, Kebin; Holben, Brent N.; Kahn, Ralph; Lagrosas, Nofel; Lestari, Puji; Ma, Zongwei; Misra, Amit; Norford, Leslie K.; Quel, Eduardo J.; Salam, Abdus; Schichtel, Bret; Segev, Lior; Tripathi, Sachchida; Wang, Chien; Yu, Chao; Zhang, Qiang; Zhang, Yuxuan; Brauer, Michael; Cohen, Aaron; Gibson, Mark D.; Liu, Yang; Vanderlei Martins, J.; Rudich, Yinon; Martin, Randall V.

2016-08-01

The Surface PARTiculate mAtter Network (SPARTAN) is a long-term project that includes characterization of chemical and physical attributes of aerosols from filter samples collected worldwide. This paper discusses the ongoing efforts of SPARTAN to define and quantify major ions and trace metals found in fine particulate matter (PM2.5). Our methods infer the spatial and temporal variability of PM2.5 in a cost-effective manner. Gravimetrically weighed filters represent multi-day averages of PM2.5, with a collocated nephelometer sampling air continuously. SPARTAN instruments are paired with AErosol RObotic NETwork (AERONET) sun photometers to better understand the relationship between ground-level PM2.5 and columnar aerosol optical depth (AOD).We have examined the chemical composition of PM2.5 at 12 globally dispersed, densely populated urban locations and a site at Mammoth Cave (US) National Park used as a background comparison. So far, each SPARTAN location has been active between the years 2013 and 2016 over periods of 2-26 months, with an average period of 12 months per site. These sites have collectively gathered over 10 years of quality aerosol data. The major PM2.5 constituents across all sites (relative contribution ± SD) are ammoniated sulfate (20 % ± 11 %), crustal material (13.4 % ± 9.9 %), equivalent black carbon (11.9 % ± 8.4 %), ammonium nitrate (4.7 % ± 3.0 %), sea salt (2.3 % ± 1.6 %), trace element oxides (1.0 % ± 1.1 %), water (7.2 % ± 3.3 %) at 35 % RH, and residual matter (40 % ± 24 %).Analysis of filter samples reveals that several PM2.5 chemical components varied by more than an order of magnitude between sites. Ammoniated sulfate ranges from 1.1 µg m-3 (Buenos Aires, Argentina) to 17 µg m-3 (Kanpur, India in the dry season). Ammonium nitrate ranged from 0.2 µg m-3 (Mammoth Cave, in summer) to 6.8 µg m-3 (Kanpur, dry season). Equivalent black carbon ranged from 0.7 µg m-3 (Mammoth Cave) to over 8 µg m-3 (Dhaka, Bangladesh and Kanpur

Tropospheric Aerosols

Science.gov (United States)

Buseck, P. R.; Schwartz, S. E.

2003-12-01

uncertainties by "the I-beams". Only an uncertainty range rather than a best estimate is presented for direct aerosol forcing by mineral dust and for indirect aerosol forcing. An assessment of the present level of scientific understanding is indicated at the bottom of the figure (reproduced by permission of Intergovernmental Panel on Climate Change). The importance of atmospheric aerosols to issues of societal concern has motivated much research intended to describe their loading, distribution, and properties and to develop understanding of the controlling processes to address such issues as air pollution, acid deposition, and climate influences of aerosols. However, description based wholly on measurements will inevitably be limited in its spatial and temporal coverage and in the limited characterization of aerosol properties. These limitations are even more serious for predictions of future emissions and provide motivation for concurrent theoretical studies and development of model-based description of atmospheric aerosols.An important long-range goal, which has already been partly realized, is to develop quantitative understanding of the processes that control aerosol loading, composition, and microphysical properties as well as the resultant optical and cloud-nucleating properties. An objective is to incorporate these results into chemical transport models that can be used for predictions. Such models are required, for example, to design approaches to achieve air quality standards and to assess and predict aerosol influences on climate change. Much current research is directed toward enhancing this understanding and to evaluating it by comparison of model results and observations. However, compared to gases, models involving particles are far more complex because of the need to specify additional parameters such as particle sizes and size distributions, compositions as a function of size, particle shapes, and temporal and spatial variations, including reactions that occur

Sources and composition of urban aerosol particles

Science.gov (United States)

Vogt, M.; Johansson, C.; Mårtensson, M.; Struthers, H.; Ahlm, L.; Nilsson, D.

2011-09-01

From May 2008 to March 2009 aerosol emissions were measured using the eddy covariance method covering the size range 0.25 to 2.5 μm diameter (Dp) from a 105 m tower, in central Stockholm, Sweden. Supporting chemical aerosol data were collected at roof and street level. Results show that the inorganic fraction of sulfate, nitrate, ammonium and sea salt accounts for approximately 15% of the total aerosol mass removed at 0.6 μm Dp. Further heating to 300 °C caused very little additional losses road traffic (as inferred from the ratio of the incremental concentrations of nitrogen oxides (NOx) and BC measured on a densely trafficked street) and the fluxes of non-volatile material at tower level are in close agreement, suggesting a traffic source of BC. We have estimated the emission factors (EFs) for non-volatile particles <0.6 μm Dp to be 2.4±1.4 mg veh-1 km-1 based on either CO2 fluxes or traffic activity data. Light (LDV) and heavy duty vehicle (HDV) EFs were estimated using multiple linear regression and reveal that for non-volatile particulate matter in the 0.25 to 0.6 μm Dp range, the EFHDV is approximately twice as high as the EFLDV, the difference not being statistically significant.

Measured Mass-Normalized Optical Cross Sections For Aerosolized Organophosphorus Chemical Warfare Simulants

National Research Council Canada - National Science Library

Gurton, Kristan P; Felton, Melvin; Dahmani, Rachid; Ligon, David

2007-01-01

We present newly measured results of an ongoing experimental program established to measure optical cross sections in the mid and long wave infrared for a variety of chemical and biologically based aerosols...

Variations of aerosol size distribution, chemical composition and optical properties from roadside to ambient environment: A case study in Hong Kong, China

Science.gov (United States)

Zhang, Qian; Ning, Zhi; Shen, Zhenxing; Li, Guoliang; Zhang, Junke; Lei, Yali; Xu, Hongmei; Sun, Jian; Zhang, Leiming; Westerdahl, Dane; Gali, Nirmal Kumar; Gong, Xuesong

2017-10-01

This study investigated the ;roadside-to-ambient; evolution of particle physicochemical and optical properties in typical urban atmospheres of Hong Kong through collection of chemically-resolved PM2.5 data and PM2.5 size distribution at a roadside and an ambient site. Roadside particle size distribution showed typical peaks in the nuclei mode (30-40 nm) while ambient measurements peaked in the Aitken mode (50-70 nm), revealing possible condensation and coagulation growth of freshly emitted particles during aging processes. Much higher levels of anthropogenic chemical components, i.e. nitrate, sulfate, ammonium, organic carbon (OC) and elemental carbon (EC), but lower levels of OC/EC and secondary inorganic aerosols (SIA)/EC ratios appeared in roadside than ambient particles. The high OC/EC and SIA/EC ratios in ambient particles implied high contributions from secondary aerosols. Black carbon (BC), a strong light absorbing material, showed large variations in optical properties when mixed with other inorganic and organic components. Particle-bound polycyclic aromatic hydrocarbons (p-PAHs), an indicator of brown carbon (BrC), showed significant UV-absorbing ability. The average BC and p-PAHs concentrations were 3.8 and 87.6 ng m-3, respectively, at the roadside, but were only 1.5 and 18.1 ng m-3 at the ambient site, suggesting BC and p-PAHs concentrations heavily driven by traffic emissions. In contrast, PM2.5 UV light absorption coefficients (babs-BrC,370nm) at the ambient site (4.2 Mm-1) and at the roadside site (4.1 Mm-1) were similar, emphasizing that particle aging processes enhanced UV light-absorbing properties, a conclusion that was also supported by the finding that the Absorption Ångström coefficient (AAC) value at UV wavelengths (AAC_UV band) at the ambient site were ∼1.7 times higher than that at the roadside. Both aqueous reaction and photochemically produced secondary organic aerosol (SOA) for ambient aerosols contributed to the peak values of babs

Contribution of anthropogenic aerosols in direct radiative forcing and atmospheric heating rate over Delhi in the Indo-Gangetic Basin.

Science.gov (United States)

Srivastava, Atul K; Singh, Sachchidanand; Tiwari, S; Bisht, D S

2012-05-01

The present work is aimed to understand direct radiation effects due to aerosols over Delhi in the Indo-Gangetic Basin (IGB) region, using detailed chemical analysis of surface measured aerosols during the year 2007. An optically equivalent aerosol model was formulated on the basis of measured aerosol chemical compositions along with the ambient meteorological parameters to derive radiatively important aerosol optical parameters. The derived aerosol parameters were then used to estimate the aerosol direct radiative forcing at the top of the atmosphere, surface, and in the atmosphere. The anthropogenic components measured at Delhi were found to be contributing ∼ 72% to the composite aerosol optical depth (AOD(0.5) ∼ 0.84). The estimated mean surface and atmospheric forcing for composite aerosols over Delhi were found to be about -69, -85, and -78 W m(-2) and about +78, +98, and +79 W m(-2) during the winter, summer, and post-monsoon periods, respectively. The anthropogenic aerosols contribute ∼ 90%, 53%, and 84% to the total aerosol surface forcing and ∼ 93%, 54%, and 88% to the total aerosol atmospheric forcing during the above respective periods. The mean (± SD) surface and atmospheric forcing for composite aerosols was about -79 (± 15) and +87 (± 26) W m(-2) over Delhi with respective anthropogenic contributions of ∼ 71% and 75% during the overall period of observation. Aerosol induced large surface cooling, which was relatively higher during summer as compared to the winter suggesting an increase in dust loading over the station. The total atmospheric heating rate at Delhi averaged during the observation was found to be 2.42  ±  0.72 K day(-1), of which the anthropogenic fraction contributed as much as ∼ 73%.

Methods of analysis for complex organic aerosol mixtures from urban emission sources of particulate carbon

International Nuclear Information System (INIS)

Mazurek, M.A.; Hildemann, L.M.; Simoneit, B.R.T.

1990-10-01

Organic aerosols comprise approximately 30% by mass of the total fine particulate matter present in urban atmospheres. The chemical composition of such aerosols is complex and reflects input from multiple sources of primary emissions to the atmosphere, as well as from secondary production of carbonaceous aerosol species via photochemical reactions. To identify discrete sources of fine carbonaceous particles in urban atmospheres, analytical methods must reconcile both bulk chemical and molecular properties of the total carbonaceous aerosol fraction. This paper presents an overview of the analytical protocol developed and used in a study of the major sources of fine carbon particles emitted to an urban atmosphere. 23 refs., 1 fig., 2 tabs

Enviro-HIRLAM/ HARMONIE Studies in ECMWF HPC EnviroAerosols Project

Science.gov (United States)

Hansen Sass, Bent; Mahura, Alexander; Nuterman, Roman; Baklanov, Alexander; Palamarchuk, Julia; Ivanov, Serguei; Pagh Nielsen, Kristian; Penenko, Alexey; Edvardsson, Nellie; Stysiak, Aleksander Andrzej; Bostanbekov, Kairat; Amstrup, Bjarne; Yang, Xiaohua; Ruban, Igor; Bergen Jensen, Marina; Penenko, Vladimir; Nurseitov, Daniyar; Zakarin, Edige

2017-04-01

The EnviroAerosols on ECMWF HPC project (2015-2017) "Enviro-HIRLAM/ HARMONIE model research and development for online integrated meteorology-chemistry-aerosols feedbacks and interactions in weather and atmospheric composition forecasting" is aimed at analysis of importance of the meteorology-chemistry/aerosols interactions and to provide a way for development of efficient techniques for on-line coupling of numerical weather prediction and atmospheric chemical transport via process-oriented parameterizations and feedback algorithms, which will improve both the numerical weather prediction and atmospheric composition forecasts. Two main application areas of the on-line integrated modelling are considered: (i) improved numerical weather prediction with short-term feedbacks of aerosols and chemistry on formation and development of meteorological variables, and (ii) improved atmospheric composition forecasting with on-line integrated meteorological forecast and two-way feedbacks between aerosols/chemistry and meteorology. During 2015-2016 several research projects were realized. At first, the study on "On-line Meteorology-Chemistry/Aerosols Modelling and Integration for Risk Assessment: Case Studies" focused on assessment of scenarios with accidental and continuous emissions of sulphur dioxide for case studies for Atyrau (Kazakhstan) near the northern part of the Caspian Sea and metallurgical enterprises on the Kola Peninsula (Russia), with GIS integration of modelling results into the RANDOM (Risk Assessment of Nature Detriment due to Oil spill Migration) system. At second, the studies on "The sensitivity of precipitation simulations to the soot aerosol presence" & "The precipitation forecast sensitivity to data assimilation on a very high resolution domain" focused on sensitivity and changes in precipitation life-cycle under black carbon polluted conditions over Scandinavia. At third, studies on "Aerosol effects over China investigated with a high resolution

Persistence of urban organic aerosols composition: Decoding their structural complexity and seasonal variability.

Science.gov (United States)

Matos, João T V; Duarte, Regina M B O; Lopes, Sónia P; Silva, Artur M S; Duarte, Armando C

2017-12-01

Organic Aerosols (OAs) are typically defined as highly complex matrices whose composition changes in time and space. Focusing on time vector, this work uses two-dimensional nuclear magnetic resonance (2D NMR) techniques to examine the structural features of water-soluble (WSOM) and alkaline-soluble organic matter (ASOM) sequentially extracted from fine atmospheric aerosols collected in an urban setting during cold and warm seasons. This study reveals molecular signatures not previously decoded in NMR-related studies of OAs as meaningful source markers. Although the ASOM is less hydrophilic and structurally diverse than its WSOM counterpart, both fractions feature a core with heteroatom-rich branched aliphatics from both primary (natural and anthropogenic) and secondary origin, aromatic secondary organics originated from anthropogenic aromatic precursors, as well as primary saccharides and amino sugar derivatives from biogenic emissions. These common structures represent those 2D NMR spectral signatures that are present in both seasons and can thus be seen as an "annual background" profile of the structural composition of OAs at the urban location. Lignin-derived structures, nitroaromatics, disaccharides, and anhydrosaccharides signatures were also identified in the WSOM samples only from periods identified as smoke impacted, which reflects the influence of biomass-burning sources. The NMR dataset on the H-C molecules backbone was also used to propose a semi-quantitative structural model of urban WSOM, which will aid efforts for more realistic studies relating the chemical properties of OAs with their atmospheric behavior. Copyright © 2017 Elsevier Ltd. All rights reserved.

The Two-Column Aerosol Project: Phase I - Overview and Impact of Elevated Aerosol Layers on Aerosol Optical Depth

Science.gov (United States)

Berg, Larry K.; Fast, Jerome D.; Barnard, James C.; Burton, Sharon P.; Cairns, Brian; Chand, Duli; Comstock, Jennifer M.; Dunagan, Stephen; Ferrare, Richard A.; Flynn, Connor J.;

The Two-Column Aerosol Project: Phase I—Overview and impact of elevated aerosol layers on aerosol optical depth

Science.gov (United States)

Berg, Larry K.; Fast, Jerome D.; Barnard, James C.; Burton, Sharon P.; Cairns, Brian; Chand, Duli; Comstock, Jennifer M.; Dunagan, Stephen; Ferrare, Richard A.; Flynn, Connor J.; Hair, Johnathan W.; Hostetler, Chris A.; Hubbe, John; Jefferson, Anne; Johnson, Roy; Kassianov, Evgueni I.; Kluzek, Celine D.; Kollias, Pavlos; Lamer, Katia; Lantz, Kathleen; Mei, Fan; Miller, Mark A.; Michalsky, Joseph; Ortega, Ivan; Pekour, Mikhail; Rogers, Ray R.; Russell, Philip B.; Redemann, Jens; Sedlacek, Arthur J.; Segal-Rosenheimer, Michal; Schmid, Beat; Shilling, John E.; Shinozuka, Yohei; Springston, Stephen R.; Tomlinson, Jason M.; Tyrrell, Megan; Wilson, Jacqueline M.; Volkamer, Rainer; Zelenyuk, Alla; Berkowitz, Carl M.

2016-01-01

The Two-Column Aerosol Project (TCAP), conducted from June 2012 through June 2013, was a unique study designed to provide a comprehensive data set that can be used to investigate a number of important climate science questions, including those related to aerosol mixing state and aerosol radiative forcing. The study was designed to sample the atmosphere between and within two atmospheric columns; one fixed near the coast of North America (over Cape Cod, MA) and a second moveable column over the Atlantic Ocean several hundred kilometers from the coast. The U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF) was deployed at the base of the Cape Cod column, and the ARM Aerial Facility was utilized for the summer and winter intensive observation periods. One important finding from TCAP is that four of six nearly cloud-free flight days had aerosol layers aloft in both the Cape Cod and maritime columns that were detected using the nadir pointing second-generation NASA high-spectral resolution lidar (HSRL-2). These layers contributed up to 60% of the total observed aerosol optical depth (AOD). Many of these layers were also intercepted by the aircraft configured for in situ sampling, and the aerosol in the layers was found to have increased amounts of biomass burning material and nitrate compared to aerosol found near the surface. In addition, while there was a great deal of spatial and day-to-day variability in the aerosol chemical composition and optical properties, no systematic differences between the two columns were observed.

Geochemical perspectives from a new aerosol chemical mass closure

Directory of Open Access Journals (Sweden)

B. Guinot

2007-01-01

Full Text Available The aerosol chemical mass closure is revisited and a simple and inexpensive methodology is proposed. This methodology relies on data obtained for aerosol mass, and concentration of the major ions and the two main carbon components, the organic carbon (OC and the black carbon (BC. Atmospheric particles are separated into coarse (AD>2 μm and fine (AD<2 μm fractions and are treated separately. For the coarse fraction the carbonaceous component is minor and assumption is made for the conversion factor k of OC-to-POM (Particulate Organic Matter which is fixed to the value of 1.8 accounting for secondary species. The coarse soluble calcium is shown to display a correlation (regression coefficient f, y axis intercept b with the missing mass. Conversely, the fine fraction is dominated by organic species and assumption is made for dust which is assumed to have the same f factor as the coarse mode dust. The fine mode mass obtained from chemical analyses is then adjusted to the actual weighed mass by tuning the k conversion factor. The k coefficient is kept different in the two modes due to the expected different origins of the organic particles. Using the f and k coefficient obtained from the data set, the mass closure is reached for each individual sample with an undetermined fraction less than 10%. The procedure has been applied to different urban and peri-urban environments in Europe and in Beijing and its efficiency and uncertainties on f and k values are discussed. The f and k coefficients are shown to offer consistent geochemical indications on aerosol origin and transformations. f allows to retrieve dust mass and its value accounting for Ca abundance in dust at the site of investigation may serve as an indicator of dust origin and aerosol interactions with anthropogenic acids. f values were found to vary in the 0.08–0.12 range in European urban areas, and a broader range in Beijing (0.01–0.16. As expected, k appears to be a relevant proxy for

Bioaerosol detection by aerosol TOF-mass spectrometry: Application of matrix assisted laser desorption/ionisation

NARCIS (Netherlands)

Wuijckhuijse, A.L. van; Stowers, M.A.; Kientz, Ch.E.; Marijnissen, J.C.M.; Scarlett, B.

2000-01-01

In previous publications the use of an aerosol time of flight mass spectrometer was reported for the on-line measurements of aerosols (Weiss 1997, Kievit 1995). The apparatus is capable of measuring the size as well as the chemical composition, by the use of Laser Desorption/Ionisation (LDI), of an

Characterizing and Understanding Aerosol Optical Properties: CARES - Final Report

Energy Technology Data Exchange (ETDEWEB)

Cappa, Christopher D [Univ. of California, Davis, CA (United States); Atkinson, Dean B [Portland State Univ., Portland, OR (United States)

2017-12-17

The scientific focus of this study was to use ambient measurements to develop new insights into the understanding of the direct radiative forcing by atmospheric aerosol particles. The study used data collected by the PI’s and others as part of both the 2010 U.S. Department of Energy (DOE) sponsored Carbonaceous Aerosols and Radiative Effects Study (CARES), which took place in and around Sacramento, CA, and the 2012 Clean Air for London (ClearfLo) study. We focus on measurements that were made of aerosol particle optical properties, namely the wavelength-dependent light absorption, scattering and extinction. Interpretation of these optical property measurements is facilitated through consideration of complementary measurements of the aerosol particle chemical composition and size distributions. With these measurements, we addressed the following general scientific questions: 1. How does light scattering and extinction by atmospheric aerosol particles depend on particle composition, water uptake, and size? 2. To what extent is light absorption by aerosol particles enhanced through the mixing of black carbon with other particulate components? 3. What relationships exist between intensive aerosol particle optical properties, and how do these depend on particle source and photochemical aging? 4. How well do spectral deconvolution methods, which are commonly used in remote sensing, retrieve information about particle size distributions?

Growth of BaTiO3-PVDF composite thick films by using aerosol deposition

Science.gov (United States)

Cho, Sung Hwan; Yoon, Young Joon

2016-01-01

Barium titanate (BaTiO3)-polyvinylidene fluoride (PVDF) composite thick films were grown by using aerosol deposition at room temperature with BaTiO3 and PVDF powders. To produce a uniform composition in ceramic and polymer composite films, which show a substantial difference in specific gravity, we used PVDF-coated BaTiO3 powders as the starting materials. An examination of the microstructure confirmed that the BaTiO3 were well distributed in the PVDF matrix in the form of a 0 - 3 compound. The crystallite size in the BaTiO3-PVDF composite thick films was 5 ˜ 50 times higher than that in pure BaTiO3 thick films. PVDF plays a role in suppressing the fragmentation of BaTiO3 powder during the aerosol deposition process and in controlling the relative permittivity.

Elemental composition of the particulate matter present in the atmospheric aerosols of Sete Lagoas, MG

International Nuclear Information System (INIS)

Queiroz, Paula Guimaraes Moura; Jacomino, Vanusa Maria Feliciano; Menezes, Maria Angela de Barros Correia

2007-01-01

The main objective of this study was the identification of sources generating particulate matter in the atmospheric aerosols of Sete Lagoas, Minas Gerais. The measurement of the mineral composition was accomplished by X-ray diffractometry and the elemental concentration by neutron activation analysis. The results showed that Al, Cl, Cu, Fe, K, Mg and Na are the predominant chemical elements in the total suspended particles (TPS). The presence of Na, Ba, Cl, Cu, Eu, Fe and Sm in those particles with aerodynamic diameter smaller than 10 μm (PM 10 ), indicates that soil dust and ceramic and pig iron industries are the main sources of air quality degradation in the region. (author)

Seasonal variations in high time-resolved chemical compositions, sources, and evolution of atmospheric submicron aerosols in the megacity Beijing

Directory of Open Access Journals (Sweden)

W. Hu

2017-08-01

Full Text Available A severe regional haze problem in the megacity Beijing and surrounding areas, caused by fast formation and growth of fine particles, has attracted much attention in recent years. In order to investigate the secondary formation and aging process of urban aerosols, four intensive campaigns were conducted in four seasons between March 2012 and March 2013 at an urban site in Beijing (116.31° E, 37.99° N. An Aerodyne high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS was deployed to measure non-refractory chemical components of submicron particulate matter (NR-PM1. The average mass concentrations of PM1 (NR-PM1+black carbon were 45.1 ± 45.8, 37.5 ± 31.0, 41.3 ± 42.7, and 81.7 ± 72.4 µg m−3 in spring, summer, autumn, and winter, respectively. Organic aerosol (OA was the most abundant component in PM1, accounting for 31, 33, 44, and 36 % seasonally, and secondary inorganic aerosol (SNA, sum of sulfate, nitrate, and ammonium accounted for 59, 57, 43, and 55 % of PM1 correspondingly. Based on the application of positive matrix factorization (PMF, the sources of OA were obtained, including the primary ones of hydrocarbon-like (HOA, cooking (COA, biomass burning OA (BBOA and coal combustion OA (CCOA, and secondary component oxygenated OA (OOA. OOA, which can be split into more-oxidized (MO-OOA and less-oxidized OOA (LO-OOA, accounted for 49, 69, 47, and 50 % in four seasons, respectively. Totally, the fraction of secondary components (OOA+SNA contributed about 60–80 % to PM1, suggesting that secondary formation played an important role in the PM pollution in Beijing, and primary sources were also non-negligible. The evolution process of OA in different seasons was investigated with multiple metrics and tools. The average carbon oxidation states and other metrics show that the oxidation state of OA was the highest in summer, probably due to both strong photochemical and aqueous-phase oxidations

Connecting Organic Aerosol Climate-Relevant Properties to Chemical Mechanisms of Sources and Processing

Energy Technology Data Exchange (ETDEWEB)

Thornton, Joel [Univ. of Washington, Seattle, WA (United States)

2015-01-26

The research conducted on this project aimed to improve our understanding of secondary organic aerosol (SOA) formation in the atmosphere, and how the properties of the SOA impact climate through its size, phase state, and optical properties. The goal of this project was to demonstrate that the use of molecular composition information to mechanistically connect source apportionment and climate properties can improve the physical basis for simulation of SOA formation and properties in climate models. The research involved developing and improving methods to provide online measurements of the molecular composition of SOA under atmospherically relevant conditions and to apply this technology to controlled simulation chamber experiments and field measurements. The science we have completed with the methodology will impact the simulation of aerosol particles in climate models.

Enhancement of the aerosol direct radiative effect by semi-volatile aerosol components: airborne measurements in North-Western Europe

Directory of Open Access Journals (Sweden)

W. T. Morgan

2010-09-01

Full Text Available A case study of atmospheric aerosol measurements exploring the impact of the vertical distribution of aerosol chemical composition upon the radiative budget in North-Western Europe is presented. Sub-micron aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS on both an airborne platform and a ground-based site at Cabauw in the Netherlands. The examined period in May 2008 was characterised by enhanced pollution loadings in North-Western Europe and was dominated by ammonium nitrate and Organic Matter (OM. Both ammonium nitrate and OM were observed to increase with altitude in the atmospheric boundary layer. This is primarily attributed to partitioning of semi-volatile gas phase species to the particle phase at reduced temperature and enhanced relative humidity. Increased ammonium nitrate concentrations in particular were found to strongly increase the ambient scattering potential of the aerosol burden, which was a consequence of the large amount of associated water as well as the enhanced mass. During particularly polluted conditions, increases in aerosol optical depth of 50–100% were estimated to occur due to the observed increase in secondary aerosol mass and associated water uptake. Furthermore, the single scattering albedo was also shown to increase with height in the boundary layer. These enhancements combined to increase the negative direct aerosol radiative forcing by close to a factor of two at the median percentile level. Such increases have major ramifications for regional climate predictions as semi-volatile components are often not included in aerosol models.

The results presented here provide an ideal opportunity to test regional and global representations of both the aerosol vertical distribution and subsequent impacts in North-Western Europe. North-Western Europe can be viewed as an analogue for the possible future air quality over other polluted regions of the Northern Hemisphere, where

Complementary online aerosol mass spectrometry and offline FT-IR spectroscopy measurements: Prospects and challenges for the analysis of anthropogenic aerosol particle emissions

Science.gov (United States)

Faber, Peter; Drewnick, Frank; Bierl, Reinhard; Borrmann, Stephan

2017-10-01

The aerosol mass spectrometer (AMS) is well established in investigating highly time-resolved dynamics of submicron aerosol chemical composition including organic aerosol (OA). However, interpretation of mass spectra on molecular level is limited due to strong fragmentation of organic substances and potential reactions inside the AMS ion chamber. Results from complementary filter-based FT-IR absorption measurements were used to explain features in high-resolution AMS mass spectra of different types of OA (e.g. cooking OA, cigarette smoking OA, wood burning OA). Using this approach some AMS fragment ions were validated in this study as appropriate and rather specific markers for a certain class of organic compounds for all particle types under investigation. These markers can therefore be used to get deeper insights in the chemical composition of OA based on AMS mass spectra in upcoming studies. However, the specificity of other fragment ions such as C2H4O2+ (m/z 60.02114) remains ambiguous. In such cases, complementary FT-IR measurements allow the interpretation of highly time-resolved AMS mass spectra at the level of molecular functional groups. Furthermore, this study discusses the challenges in reducing inorganic interferences (e.g. from water and ammonium salts) in FT-IR spectra of atmospheric aerosols to decrease spectral uncertainties for better comparisons and, thus, to get more robust results.

Chemical characteristics of ambient aerosols contributed by cooking process at Noorpur village near Delhi (India)

Science.gov (United States)

Singh, Sudha; Kumar, Bablu; Gupta, Gyan Prakash; Kulshrestha, U. C.

2013-05-01

Combustion of fuels such as wood, crop residue and dung cakes etc. is one of the major sources of air pollution in developing countries. These fuels are still used commonly for cooking purpose in rural India. This study investigates the chemical composition of the ambient aerosols during cooking hours at a village called Noorpur (28.470 N, 77.030 E) which lies near Delhi city. Aerosol sampling was carried out during August 2011-May 2012 by using handy sampler (Envirotech model APM 821) installed at the terrace of a building (˜6m). The samples were collected on 8 hourly basis using Teflon filters. The water extract of these filters was analyzed for major anions (F-, Cl-, NO3-, SO42-) and major cations (Na+, NH4+, K+, Ca2+ Mg2+) by ion chromatography (Metrohm 883 Basic IC Plus). Results highlighted that cooking process contributed significant amount of SO42- and K+ṡ. Biomass burning is considered as a potential source of K+ in air. The high concentration of SO42- might be due to oxidation of SO2 contributed by the combustion of dung cakes. Further, the detailed results will be discussed during the conference.

Aerosol composition, oxidation properties, and sources in Beijing: results from the 2014 Asia-Pacific Economic Cooperation summit study

Science.gov (United States)

Xu, W. Q.; Sun, Y. L.; Chen, C.; Du, W.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Zhao, X. J.; Zhou, L. B.; Ji, D. S.; Wang, P. C.; Worsnop, D. R.

2015-12-01

The mitigation of air pollution in megacities remains a great challenge because of the complex sources and formation mechanisms of aerosol particles. The 2014 Asia-Pacific Economic Cooperation (APEC) summit in Beijing serves as a unique experiment to study the impacts of emission controls on aerosol composition, size distributions, and oxidation properties. Herein, a high-resolution time-of-flight aerosol mass spectrometer was deployed in urban Beijing for real-time measurements of size-resolved non-refractory submicron aerosol (NR-PM1) species from 14 October to 12 November 2014, along with a range of collocated measurements. The average (±σ) PM1 was 41.6 (±38.9) μg m-3 during APEC, which was decreased by 53 % compared with that before APEC. The aerosol composition showed substantial changes owing to emission controls during APEC. Secondary inorganic aerosol (SIA: sulfate + nitrate + ammonium) showed significant reductions of 62-69 %, whereas organics presented much smaller decreases (35 %). The results from the positive matrix factorization of organic aerosol (OA) indicated that highly oxidized secondary organic aerosol (SOA) showed decreases similar to those of SIA during APEC. However, primary organic aerosol (POA) from cooking, traffic, and biomass-burning sources were comparable to those before APEC, indicating the presence of strong local source emissions. The oxidation properties showed corresponding changes in response to OA composition. The average oxygen-to-carbon level during APEC was 0.36 (±0.10), which is lower than the 0.43 (±0.13) measured before APEC, demonstrating a decrease in the OA oxidation degree. The changes in size distributions of primary and secondary species varied during APEC. SIA and SOA showed significant reductions in large accumulation modes with peak diameters shifting from ~ 650 to 400 nm during APEC, whereas those of POA remained relatively unchanged. The changes in aerosol composition, size distributions, and oxidation

The role of iron and black carbon in aerosol light absorption

Directory of Open Access Journals (Sweden)

Y. Derimian

2008-07-01

Full Text Available Iron is a major component of atmospheric aerosols, influencing the light absorption ability of mineral dust, and an important micronutrient that affects oceanic biogeochemistry. The regional distribution of the iron concentration in dust is important for climate studies; however, this is difficult to obtain since it requires in-situ aerosol sampling or simulation of complex natural processes. Simultaneous studies of aerosol chemical composition and radiometric measurements of aerosol optical properties, which were performed in the Negev desert of Israel continuously for about eight years, suggest a potential for deriving a relationship between chemical composition and light absorption properties, in particular the spectral single-scattering albedo.

The two main data sets of the present study were obtained by a sun/sky radiometer and a stacked filter unit sampler that collects particles in coarse and fine size fractions. Analysis of chemical and optical data showed the presence of mixed dust and pollution aerosol in the study area, although their sources appear to be different. Spectral SSA showed an evident response to increased concentrations of iron, black carbon equivalent matter, and their mixing state. A relationship that relates the spectral SSA, the percentage of iron in total particulate mass, and the pollution components was derived. Results calculated, using this relationship, were compared with measurements from dust episodes in several locations around the globe. The comparison showed reasonable agreement between the calculated and the observed iron concentrations, and supported the validity of the suggested approach for the estimation of iron concentrations in mineral dust.

Improved modelling of sodium-spray fires and sodium-combustion aerosol chemical evolution - 15488

International Nuclear Information System (INIS)

Mathe, E.; Kissane, M.; Petitprez, D.

2015-01-01

In the context of the Generation IV Initiative, the consequences of a severe-accident in sodium-cooled fast reactor (SFR) must be studied. Being pyrophoric, sodium will burn upon contact with air in a containment creating toxic aerosols and we must take into account these fire aerosols when assessing the source term. We have developed a numerical simulation named NATRAC to calculate the mass of aerosols produced during a spray fire in a SFR severe accident. The results show that the mass of oxide aerosols can involve more than 60% of the ejected sodium. In a second part we have developed a numerical simulation named STARK based on the Cooper model that models the physico-chemical transformations of the aerosols. However, this model has never been validated and the literature does not permit to do so. In these conditions, we have designed and performed our own experiment ESSTIA to obtain the missing values of the parameters that govern Cooper model. The modified Cooper model we propose with the new parameters reproduces correctly the ESSTIA experimental data. The only parameter that has not yet been measured is the tortuosity of the sodium-fire aerosols surface layers. A dedicated experiment using real sodium-fire aerosols could eliminate any doubts about the uncertainty of the proposed Cooper model

Aerosol characterization over the southeastern United States using high resolution aerosol mass spectrometry: spatial and seasonal variation of aerosol composition, sources, and organic nitrates

Science.gov (United States)

Xu, L.; Suresh, S.; Guo, H.; Weber, R. J.; Ng, N. L.

2015-04-01

We deployed a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and an Aerosol Chemical Speciation Monitor (ACSM) to characterize the chemical composition of submicron non-refractory particles (NR-PM1) in the southeastern US. Measurements were performed in both rural and urban sites in the greater Atlanta area, GA and Centreville, AL for approximately one year, as part of Southeastern Center of Air Pollution and Epidemiology study (SCAPE) and Southern Oxidant and Aerosol Study (SOAS). Organic aerosol (OA) accounts for more than half of NR1 mass concentration regardless of sampling sites and seasons. Positive matrix factorization (PMF) analysis of HR-ToF-AMS measurements identified various OA sources, depending on location and season. Hydrocarbon-like OA (HOA) and cooking OA (COA) have important but not dominant contributions to total OA in urban sites. Biomass burning OA (BBOA) concentration shows a distinct seasonal variation with a larger enhancement in winter than summer. We find a good correlation between BBOA and brown carbon, indicating biomass burning is an important source for brown carbon, although an additional, unidentified brown carbon source is likely present at the rural Yorkville site. Isoprene-derived OA (Isoprene-OA) is only deconvolved in warmer months and contributes 18-36% of total OA. The presence of Isoprene-OA factor in urban sites is more likely from local production in the presence of NOx than transport from rural sites. More-oxidized and less-oxidized oxygenated organic aerosol (MO-OOA and LO-OOA, respectively) are dominant fractions (47-79%) of OA in all sites. MO-OOA correlates well with ozone in summer, but not in winter, indicating MO-OOA sources may vary with seasons. LO-OOA, which reaches a daily maximum at night, correlates better with estimated nitrate functionality from organic nitrates than total nitrates. Based on the HR-ToF-AMS measurements, we estimate that the nitrate functionality from organic nitrates

Titan's organic aerosols: Molecular composition and structure of laboratory analogues inferred from pyrolysis gas chromatography mass spectrometry analysis

Science.gov (United States)

Morisson, Marietta; Szopa, Cyril; Carrasco, Nathalie; Buch, Arnaud; Gautier, Thomas

2016-10-01

Analogues of Titan's aerosols are of primary interest in the understanding of Titan's atmospheric chemistry and climate, and in the development of in situ instrumentation for future space missions. Numerous studies have been carried out to characterize laboratory analogues of Titan aerosols (tholins), but their molecular composition and structure are still poorly known. If pyrolysis gas chromatography mass spectrometry (pyr-GCMS) has been used for years to give clues about their chemical composition, highly disparate results were obtained with this technique. They can be attributed to the variety of analytical conditions used for pyr-GCMS analyses, and/or to differences in the nature of the analogues analyzed, that were produced with different laboratory set-ups under various operating conditions. In order to have a better description of Titan's tholin's molecular composition by pyr-GCMS, we carried out a systematic study with two major objectives: (i) exploring the pyr-GCMS analytical parameters to find the optimal ones for the detection of a wide range of chemical products allowing a characterization of the tholins composition as comprehensive as possible, and (ii) highlighting the role of the CH4 ratio in the gaseous reactive medium on the tholin's molecular structure. We used a radio-frequency plasma discharge to synthetize tholins with different concentrations of CH4 diluted in N2. The samples were pyrolyzed at temperatures covering the 200-700°C range. The extracted gases were then analyzed by GCMS for their molecular identification. The optimal pyrolysis temperature for characterizing the molecular composition of our tholins by GCMS analysis is found to be 600°C. This temperature choice results from the best compromise between the number of compounds released, the quality of the signal and the appearance of pyrolysis artifacts. About a hundred molecules are identified as pyrolysates. A common major chromatographic pattern appears clearly for all the

Investigating the composition of organic aerosol resulting from cyclohexene ozonolysis: low molecular weight and heterogeneous reaction products

Directory of Open Access Journals (Sweden)

J. F. Hamilton

2006-01-01

Full Text Available The composition of organic aerosol formed from the gas phase ozonolysis of cyclohexene has been investigated in a smog chamber experiment. Comprehensive gas chromatography with time of flight mass spectrometric detection was used to determine that dicarboxylic acids and corresponding cyclic anhydrides dominated the small gas phase reaction products found in aerosol sampled during the first hour after initial aerosol formation. Structural analysis of larger more polar molecules was performed using liquid chromatography with ion trap tandem mass spectrometry. This indicated that the majority of identified organic mass was in dimer form, built up from combinations of the most abundant small acid molecules, with frequent indication of the inclusion of adipic acid. Trimers and tetramers potentially formed via similar acid combinations were also observed in lower abundances. Tandem mass spectral data indicated dimers with either acid anhydride or ester functionalities as the linkage between monomers. High-resolution mass spectrometry identified the molecular formulae of the most abundant dimer species to be C10H16O6, C11H18O6, C10H14O8 and C11H16O8 and could be used in some cases to reduce uncertainty in exact chemical structure determination by tandem MS.

The Chemical Composition of Fogs and Clouds in Southern California.

Science.gov (United States)

Munger, James William

Fog and clouds are frequent occurrences in Southern California. Their chemical composition is of interest due to their potential role in the transformation of sulfur and nitrogen oxides to sulfuric and nitric acid and in the subsequent deposition of those acids. In addition, cloud and fog droplets may be involved in the chemistry of low-molecular-weight carboxylic acids and carbonyl compounds. The major inorganic species in cloud and fogwater samples were NH_4^+, H ^+, NO_3^-, and SO_4^{2-}. Concentrations in fogwater samples were 1-10 times 10^ {-3} M; pH values ranged from ~eq2 to 6. Nitrate usually exceeded sulfate. Acidity depended on the availability of of NH_3 from agricultural operations. Stratus cloudwater had somewhat lower concentrations; pH values were in the range 3-4. The major factors accounting for variation in fog- or cloudwater composition were the preexisting aerosol and gas concentrations and variations in liquid water content. Deposition and entrainment or advection of different air masses were also important during extended cloud or fog episodes. The droplet size dependence of cloudwater composition was investigated on one occasion in an intercepted coastal stratus clouds. The observations were consistent with the hypothesis that small droplets form on small secondary aerosol composed of H_2SO _4, HNO_3, and their NH_4^+ salts, while large droplets form on large sea-salt and soil-dust aerosol. Species that can exist in the gas phase, such as HCl and HNO _3, may be found in either droplet-size fraction. Concentrations of S(IV) and CH_2 O in the range 100-1000 μm were observed in fogwater from urban sites in Southern California. Lower concentrations were observed in stratus clouds. The high levels of S(IV) and CH_2 O were attributed to the formation of hydroxymethanesulfonate (HMSA), the S(IV) adduct of CH_2O. Direct measurement of HMSA in fogwater samples from Bakersfield, CA were made by ion-pairing chromatography. Glyoxal and methylglyoxal

Modelled radiative forcing of the direct aerosol effect with multi-observation evaluation

Directory of Open Access Journals (Sweden)

G. Myhre

2009-02-01

Full Text Available A high-resolution global aerosol model (Oslo CTM2 driven by meteorological data and allowing a comparison with a variety of aerosol observations is used to simulate radiative forcing (RF of the direct aerosol effect. The model simulates all main aerosol components, including several secondary components such as nitrate and secondary organic carbon. The model reproduces the main chemical composition and size features observed during large aerosol campaigns. Although the chemical composition compares best with ground-based measurement over land for modelled sulphate, no systematic differences are found for other compounds. The modelled aerosol optical depth (AOD is compared to remote sensed data from AERONET ground and MODIS and MISR satellite retrievals. To gain confidence in the aerosol modelling, we have tested its ability to reproduce daily variability in the aerosol content, and this is performing well in many regions; however, we also identified some locations where model improvements are needed. The annual mean regional pattern of AOD from the aerosol model is broadly similar to the AERONET and the satellite retrievals (mostly within 10–20%. We notice a significant improvement from MODIS Collection 4 to Collection 5 compared to AERONET data. Satellite derived estimates of aerosol radiative effect over ocean for clear sky conditions differs significantly on regional scales (almost up to a factor two, but also in the global mean. The Oslo CTM2 has an aerosol radiative effect close to the mean of the satellite derived estimates. We derive a radiative forcing (RF of the direct aerosol effect of −0.35 Wm⁻² in our base case. Implementation of a simple approach to consider internal black carbon (BC mixture results in a total RF of −0.28 Wm⁻². Our results highlight the importance of carbonaceous particles, producing stronger individual RF than considered in the recent IPCC estimate; however, net RF is less different

Chemical character and probable origin of aerosols at the BARC site, Trombay

International Nuclear Information System (INIS)

Sequeira, R.; Kelkar, D.N.

1975-01-01

Measurements carried out on the dustload and concentration of sodium, potassium, ammonium, calcium, magnesium, iron, aluminium, silicon, chloride and sulphate in atmospheric air at the Bhabha Atomic Research Centre site, Trombay, the period November 1971-April 1972 have been reported. The average dustload is around 200μg/M 3 . About 50 percent of this could be accounted for, by the present analytical estimatioon of the individual chemical constituents : the water-soluble fraction obtained being 20 percent and the water-insoluble fraction accounting for the rest. Marine contribution to aerosol mass, calculated on the basis of water-soluble sodium concentration indicated that the sea is minor source of aerosols contributing 5 percent of the total aerosol mass. It was observed that the organic matter was about 20 percent of the total aerosol mass. If the local soil and fly-ash are the soil contributors to water-insoluble iron and potassium in aerosols, the respective contributions by these two sources were seen to be 13 percent and 48 percents. If all the organics and the non-marine fraction of the water-soluble mass are of industrial origin, the man-made fraction aerosols would constitute a maximum of 80 percent of the dustload in the Trombay air. The remaining 20 percent would be of natural origin, amounting to about 45 μg/M 3 , a value that represents unpolluted atmospheres. (author)

Insights into a dust event transported through Beijing in spring 2012: Morphology, chemical composition and impact on surface aerosols

Energy Technology Data Exchange (ETDEWEB)

Hu, Wei [State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871 (China); Faculty of Environmental and Symbiotic Sciences, Prefectural University of Kumamoto, Kumamoto 862-8502 (Japan); Niu, Hongya [State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871 (China); Key Laboratory of Resource Exploration Research of Hebei Province, Hebei University of Engineering, Handan, Hebei 056038 (China); Zhang, Daizhou [Faculty of Environmental and Symbiotic Sciences, Prefectural University of Kumamoto, Kumamoto 862-8502 (Japan); Wu, Zhijun [State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871 (China); Chen, Chen [State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871 (China); Beijing Municipal Environmental Monitoring Center, Beijing 100044 (China); Wu, Yusheng; Shang, Dongjie [State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871 (China); Hu, Min, E-mail: minhu@pku.edu.cn [State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871 (China)

2016-09-15

Multiple approaches were used to investigate the evolution of surface aerosols in Beijing during the passage of a dust event at high altitude, which was from the Gobi areas of southern Mongolia and covered a wide range of North China. Single particle analysis with electron microscope showed that the majority of coarse particles were mineral ones, and most of them were in the size range of 1–7 μm with a peak of number concentration at about 3.5 μm. Based on elemental composition and morphology, the mineral particles could be classified into several groups, including Si-rich (71%), Ca-rich (15%), Fe-rich (6%), and halite-rich (2%), etc., and they were the main contributors to the aerosol optical depth as the dust occurred. The size distributions of surface aerosols were significantly affected by the dust intrusion. The average number concentration of accumulation mode particles during the event was about 400 cm{sup −3}, which was much lower than that in heavily polluted days (6300 cm{sup −3}). At the stage of floating dust, the number concentration of accumulation mode particles decreased, and coarse particles contributed to total volume concentration of particulate matter as much as 90%. The accumulation mode particles collected in this stage were mostly in the size range of 0.2–0.5 μm, and were rectangular or spherical. They were considered to be particles consisting of ammonium sulfate. New particle formation (NPF) was observed around noon in the three days during the dust event, indicating that the passage of the dust was probably favorable for NPF. - Highlights: • A dust event transported at high altitude through Beijing was investigated. • The dust event caused high variation in surface aerosol number concentrations. • Fine particles in the floating dust period probably consisted of ammonium sulfate. • Passage of the dust induced a favorable condition for new particle formation.

Insights into a dust event transported through Beijing in spring 2012: Morphology, chemical composition and impact on surface aerosols

International Nuclear Information System (INIS)

Hu, Wei; Niu, Hongya; Zhang, Daizhou; Wu, Zhijun; Chen, Chen; Wu, Yusheng; Shang, Dongjie; Hu, Min

2016-01-01

Multiple approaches were used to investigate the evolution of surface aerosols in Beijing during the passage of a dust event at high altitude, which was from the Gobi areas of southern Mongolia and covered a wide range of North China. Single particle analysis with electron microscope showed that the majority of coarse particles were mineral ones, and most of them were in the size range of 1–7 μm with a peak of number concentration at about 3.5 μm. Based on elemental composition and morphology, the mineral particles could be classified into several groups, including Si-rich (71%), Ca-rich (15%), Fe-rich (6%), and halite-rich (2%), etc., and they were the main contributors to the aerosol optical depth as the dust occurred. The size distributions of surface aerosols were significantly affected by the dust intrusion. The average number concentration of accumulation mode particles during the event was about 400 cm"−"3, which was much lower than that in heavily polluted days (6300 cm"−"3). At the stage of floating dust, the number concentration of accumulation mode particles decreased, and coarse particles contributed to total volume concentration of particulate matter as much as 90%. The accumulation mode particles collected in this stage were mostly in the size range of 0.2–0.5 μm, and were rectangular or spherical. They were considered to be particles consisting of ammonium sulfate. New particle formation (NPF) was observed around noon in the three days during the dust event, indicating that the passage of the dust was probably favorable for NPF. - Highlights: • A dust event transported at high altitude through Beijing was investigated. • The dust event caused high variation in surface aerosol number concentrations. • Fine particles in the floating dust period probably consisted of ammonium sulfate. • Passage of the dust induced a favorable condition for new particle formation.

Size-specific composition of aerosols in the El Chichon volcanic cloud

Science.gov (United States)

Woods, D. C.; Chuan, R. L.

1983-01-01

A NASA U-2 research aircraft flew sampling missions in April, May, July, November, and December 1982 aimed at obtaining in situ data in the stratospheric cloud produced from the March-April 1982 El Chichon eruptions. Post flight analyses provided information on the aerosol composition and morphology. The particles ranged in size from smaller than 0.05 m to larger than 20 m diameter and were quite complex in composition. In the April, May, and July samples the aerosol mass was dominated by magmatic and lithic particles larger than about 3 m. The submicron particles consisted largely of sulfuric acid. Halite particles, believed to be related to a salt dome beneath El Chichon, were collected in the stratosphere in April and May. On the July 23 flight, copper-zinc oxide particles were collected. In July, November, and December, in addition to the volcanic ash and acid particles, carbon-rich particles smaller than about 0.1 m aerodynamic diameter were abundant.

Aerosol Emissions from Great Lakes Harmful Algal Blooms

Energy Technology Data Exchange (ETDEWEB)

May, Nathaniel W. [Department; Olson, Nicole E. [Department; Panas, Mark [Department; Axson, Jessica L. [Department; Tirella, Peter S. [Department; Kirpes, Rachel M. [Department; Craig, Rebecca L. [Department; Gunsch, Matthew J. [Department; China, Swarup [William; Laskin, Alexander [William; Ault, Andrew P. [Department; Department; Pratt, Kerri A. [Department; Department

2017-12-20

In freshwater lakes, harmful algal blooms (HABs) of Cyanobacteria (blue-green algae) produce toxins that impact human health. However, little is known about the chemical species present in lake spray aerosol (LSA) produced from wave-breaking in freshwater HABs. In this study, a laboratory LSA generator produced aerosols from freshwater samples collected from Lake Michigan and Lake Erie during HAB and non-bloom conditions. Particles were analyzed for size and chemical composition by single particle mass spectrometry, electron microscopy, and fluorescence microscopy, with three distinct types of LSA identified with varying levels of organic carbon and biological material associated with calcium salts. LSA autofluorescence increases with blue-green algae concentration, showing that organic molecules of biological origin are incorporated in LSA from HABs. The number fraction of LSA with biological mass spectral markers also increases with particle diameter (greater than 0.5 μm), showing that HABs have size-dependent impacts on aerosol composition. The highest number fraction of LSA enriched in organic carbon were observed in particles less than 0.5 μm in diameter. Understanding the transfer of organic and biogenic material from freshwater to the atmosphere via LSA particles is crucial for determining health and climate effects due to HABs.

The influence of the physico-chemical form of the aerosol on the radiological consequences of notional accidental releases of radioactivity from a fast breeder reactor

International Nuclear Information System (INIS)

Kelly, G.N.; Jones, J.A.; Simmonds, J.R.

1979-01-01

The radiological consequences of a wide range of notional accidental releases from a 1300 MW(e) LMFBR (Liquid Metal-cooled Fast Breeder Reactor) were assessed in a study published by the National Radiological Protection Board (NRPB) in 1977. In that study representative values were in general adopted for each of the important parameters while recognising that in reality they could vary considerably. The present study is concerned with the sensitivity of the predicted consequences to the physico-chemical form of the released aerosol. Of particular interest is the importance of a mixed sodium-transuranium element aerosol which may be formed in accidental releases of activity from sodium cooled FBRs. Two significant findings emerge from the study. First the predicted consequences in general are relatively insensitive to the range of physico-chemical forms analysed. For generic assessments therefore it is sufficient to assume the properties of the aerosol adopted in the initial study (1 μm AMAD and each element in the oxide form); the exception concerns the estimation of the incidence of early morbidity, and to a lesser extent early mortality, but only for a limited range of release composition. The second finding is that the radiological consequences are not, contrary to what might have been expected, significantly increased for the release of a mixed sodium-element aerosol

Sampling and chemical analysis by TXRF of size-fractionated ambient aerosols and emissions

International Nuclear Information System (INIS)

John, A.C.; Kuhlbusch, T.A.J.; Fissan, H.; Schmidt, K.-G-; Schmidt, F.; Pfeffer, H.-U.; Gladtke, D.

2000-01-01

Results of recent epidemiological studies led to new European air quality standards which require the monitoring of particles with aerodynamic diameters ≤ 10 μm (PM 10) and ≤ 2.5 μm (PM 2.5) instead of TSP (total suspended particulate matter). As these ambient air limit values will be exceeded most likely at several locations in Europe, so-called 'action plans' have to be set up to reduce particle concentrations, which requires information about sources and processes of PMx aerosols. For chemical characterization of the aerosols, different samplers were used and total reflection x-ray fluorescence analysis (TXRF) was applied beside other methods (elemental and organic carbon analysis, ion chromatography, atomic absorption spectrometry). For TXRF analysis, a specially designed sampling unit was built where the particle size classes 10-2.5 μm and 2.5-1.0 μm were directly impacted on TXRF sample carriers. An electrostatic precipitator (ESP) was used as a back-up filter to collect particles <1 μm directly on a TXRF sample carrier. The sampling unit was calibrated in the laboratory and then used for field measurements to determine the elemental composition of the mentioned particle size fractions. One of the field campaigns was carried out at a measurement site in Duesseldorf, Germany, in November 1999. As the composition of the ambient aerosols may have been influenced by a large construction site directly in the vicinity of the station during the field campaign, not only the aerosol particles, but also construction material was sampled and analyzed by TXRF. As air quality is affected by natural and anthropogenic sources, the emissions of particles ≤ 10 μm and ≤ 2.5 μm, respectively, have to be determined to estimate their contributions to the so called coarse and fine particle modes of ambient air. Therefore, an in-stack particle sampling system was developed according to the new ambient air quality standards. This PM 10/PM 2.5 cascade impactor was

Characteristics, sources and evolution of fine aerosol (PM1) at urban, coastal and forest background sites in Lithuania

NARCIS (Netherlands)

Masalaite, A.; Holzinger, R.; Remeikis, V.; Roeckmann, Thomas; Dusek, U.

The chemical and isotopic composition of organic aerosol (OA) samples collected on PM1 filters was determined as a function of desorption temperature to investigate the main sources of organic carbon and the effects of photochemical processing on atmospheric aerosol. The filter samples were

Constraining the atmospheric composition of the day-night terminators of HD 189733b: Atmospheric retrieval with aerosols

Energy Technology Data Exchange (ETDEWEB)

Lee, Jae-Min [Institute for Computational Science, University of Zürich, Winterthurerstrasse 190, CH-8057 Zürich (Switzerland); Irwin, Patrick G. J.; Fletcher, Leigh N.; Barstow, Joanna K. [Department of Atmospheric, Oceanic, and Planetary Physics, University of Oxford, OX1 3PU Oxford (United Kingdom); Heng, Kevin, E-mail: lee@physik.uzh.ch [Center for Space and Habitability, University of Bern, Sidlerstrasse 5, CH-3012 Bern (Switzerland)

2014-07-01

A number of observations have shown that Rayleigh scattering by aerosols dominates the transmission spectrum of HD 189733b at wavelengths shortward of 1 μm. In this study, we retrieve a range of aerosol distributions consistent with transmission spectroscopy between 0.3-24 μm that were recently re-analyzed by Pont et al. To constrain the particle size and the optical depth of the aerosol layer, we investigate the degeneracies between aerosol composition, temperature, planetary radius, and molecular abundances that prevent unique solutions for transit spectroscopy. Assuming that the aerosol is composed of MgSiO{sub 3}, we suggest that a vertically uniform aerosol layer over all pressures with a monodisperse particle size smaller than about 0.1 μm and an optical depth in the range 0.002-0.02 at 1 μm provides statistically meaningful solutions for the day/night terminator regions of HD 189733b. Generally, we find that a uniform aerosol layer provide adequate fits to the data if the optical depth is less than 0.1 and the particle size is smaller than 0.1 μm, irrespective of the atmospheric temperature, planetary radius, aerosol composition, and gaseous molecules. Strong constraints on the aerosol properties are provided by spectra at wavelengths shortward of 1 μm as well as longward of 8 μm, if the aerosol material has absorption features in this region. We show that these are the optimal wavelengths for quantifying the effects of aerosols, which may guide the design of future space observations. The present investigation indicates that the current data offer sufficient information to constrain some of the aerosol properties of HD189733b, but the chemistry in the terminator regions remains uncertain.

Cloud Scavenging Effects on Aerosol Radiative and Cloud-nucleating Properties - Final Technical Report

Energy Technology Data Exchange (ETDEWEB)

Ogren, John A.; Sheridan, Patrick S.; Andrews, Elisabeth

2009-03-05

The optical properties of aerosol particles are the controlling factors in determining direct aerosol radiative forcing. These optical properties depend on the chemical composition and size distribution of the aerosol particles, which can change due to various processes during the particles’ lifetime in the atmosphere. Over the course of this project we have studied how cloud processing of atmospheric aerosol changes the aerosol optical properties. A counterflow virtual impactor was used to separate cloud drops from interstitial aerosol and parallel aerosol systems were used to measure the optical properties of the interstitial and cloud-scavenged aerosol. Specifically, aerosol light scattering, back-scattering and absorption were measured and used to derive radiatively significant parameters such as aerosol single scattering albedo and backscatter fraction for cloud-scavenged and interstitial aerosol. This data allows us to demonstrate that the radiative properties of cloud-processed aerosol can be quite different than pre-cloud aerosol. These differences can be used to improve the parameterization of aerosol forcing in climate models.

Seasonal variation of spherical aerosols distribution in East Asia based on ground and space Lidar observation and a Chemical transport model

Science.gov (United States)

Hara, Y.; Yumimoto, K.; Uno, I.; Shimizu, A.; Sugimoto, N.; Ohara, T.

2009-12-01

The anthropogenic aerosols largely impact on not only human health but also global climate system, therefore air pollution in East Asia due to a rapid economic growth has been recognized as a significant environmental problem. Several international field campaigns had been conducted to elucidate pollutant gases, aerosols characteristics and radiative forcing in East Asia. (e.g., ACE-Asia, TRACE-P, ADEC, EAREX 2005). However, these experiments were mainly conducted in springtime, therefore seasonal variation of aerosols distribution has not been clarified well yet. National Institute for Environmental Studies (NIES) has been constructing a lidar networks by automated dual wavelength / polarization Mie-lidar systems to observe the atmospheric environment in Asian region since 2001. Furthermore, from June 2006, space-borne backscatter lidar, Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP), onboard NASA/CALIPSO satellite, measures continuous global aerosol and cloud vertical distribution with very high spatial resolution. In this paper, we will show the seasonal variation of aerosols distribution in East Asia based on the NIES lidar network observation, Community Multi-scale Air Quality Modeling System (CMAQ) chemical transport model simulation and CALIOP observation over the period from July 2006 to December 2008. We found that CMAQ result explains the typical seasonal aerosol characteristics by lidar observations. For example, CMAQ and ground lidar showed a summertime peak of aerosol optical thickness (AOT) at Beijing, an autumn AOT peak at Guangzhou and summertime AOT trough at Hedo, Okinawa. These characteristics are mainly controlled by seasonal variations of Asian summer/winter monsoon system. We also examined the CMAQ seasonal average aerosol extinction profiles with ground lidar and CALIOP extinction data. These comparisons clarified that the CMAQ reproduced the observed aerosol layer depth well in the downwind region. Ground lidar and CALIOP seasonal

Effect of relative humidity on soot - secondary organic aerosol mixing: A case study from the Soot Aerosol Aging Study (PNNL-SAAS)

Science.gov (United States)

Sharma, N.; China, S.; Zaveri, R. A.; Shilling, J. E.; Pekour, M. S.; Liu, S.; Aiken, A. C.; Dubey, M. K.; Wilson, J. M.; Zelenyuk, A.; OBrien, R. E.; Moffet, R.; Gilles, M. K.; Gourihar, K.; Chand, D.; Sedlacek, A. J., III; Subramanian, R.; Onasch, T. B.; Laskin, A.; Mazzoleni, C.

2014-12-01

Atmospheric processing of fresh soot particles emitted by anthropogenic as well as natural sources alters their physical and chemical properties. For example, fresh and aged soot particles interact differently with incident solar radiation, resulting in different overall radiation budgets. Varying atmospheric chemical and meteorological conditions can result in complex soot mixing states. The Soot Aerosol Aging Study (SAAS) was conducted at the Pacific Northwest National Laboratory in November 2013 and January 2014 as a step towards understanding the evolution of mixing state of soot and its impact on climate-relevant properties. Aging experiments on diesel soot were carried out in a controlled laboratory chamber, and the effects of condensation and coagulation processes were systematically explored in separate sets of experiments. In addition to online measurement of aerosol properties, aerosol samples were collected for offline single particle analysis to investigate the evolution of the morphology, elemental composition and fine structure of sample particles from different experiments. Condensation experiments focused on the formation of α-pinene secondary organic aerosol on diesel soot aerosol seeds. Experiments were conducted to study the aging of soot under dry (RH < 2%) and humid conditions (RH ~ 80%). We present an analysis of the morphology of soot, its evolution, and its correlation with optical properties, as the condensation of α-pinene SOA is carried out for the two different RH conditions. The analysis was performed by using scanning electron microscopy, transmission electron microscopy, scanning transmission x-ray microscopy and atomic force microscopy for single particle characterization. In addition, particle size, mass, composition, shape, and density were characterized in-situ, as a function of organics condensed on soot seeds, using single particle mass spectrometer.

Chemical characteristics of aerosols in MABL of Bay of Bengal and ...

Indian Academy of Sciences (India)

the water-soluble ion composition of bulk-aerosols over BoB, in contrast to Arabian Sea, arises from advective transport of continental pollutants to the. Bay region. This is further reflected in the higher abundance of OC and EC over BoB. The near quantitative Cl. −. -depletion from sea-salts by chemi- cal interaction with ...

OH-initiated Aging of Biomass Burning Aerosol during FIREX

Science.gov (United States)

Lim, C. Y.; Hagan, D. H.; Cappa, C. D.; Kroll, J. H.; Coggon, M.; Koss, A.; Sekimoto, K.; De Gouw, J. A.; Warneke, C.

2017-12-01

Biomass burning emissions represent a major source of fine particulate matter to the atmosphere, and this source will likely become increasingly important in the future due to changes in the Earth's climate. Understanding the effects that increased fire emissions have on both air quality and climate requires understanding the composition of the particles emitted, since chemical and physical composition directly impact important particle properties such as absorptivity, toxicity, and cloud condensation nuclei activity. However, the composition of biomass burning particles in the atmosphere is dynamic, as the particles are subject to the condensation of low-volatility vapors and reaction with oxidants such as the hydroxyl radical (OH) during transport. Here we present a series of laboratory chamber experiments on the OH-initiated aging of biomass burning aerosol performed at the Fire Sciences Laboratory in Missoula, MT as part of the Fire Influences on Regional and Global Environments Experiment (FIREX) campaign. We describe the evolution of biomass burning aerosol produced from a variety of fuels operating the chamber in both particle-only and gas + particle mode, focusing on changes to the organic composition. In particle-only mode, gas-phase biomass burning emissions are removed before oxidation to focus on heterogeneous oxidation, while gas + particle mode includes both heterogeneous oxidation and condensation of oxidized volatile organic compounds onto the particles (secondary organic aerosol formation). Variability in fuels and burning conditions lead to differences in aerosol loading and secondary aerosol production, but in all cases aging results in a significant and rapid increases in the carbon oxidation state of the particles.

Chemically-resolved aerosol volatility measurements from two megacity field studies

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J. A. Huffman

2009-09-01

Full Text Available The volatilities of different chemical species in ambient aerosols are important but remain poorly characterized. The coupling of a recently developed rapid temperature-stepping thermodenuder (TD, operated in the range 54–230°C with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS during field studies in two polluted megacities has enabled the first direct characterization of chemically-resolved urban particle volatility. Measurements in Riverside, CA and Mexico City are generally consistent and show ambient nitrate as having the highest volatility of any AMS standard aerosol species while sulfate showed the lowest volatility. Total organic aerosol (OA showed volatility intermediate between nitrate and sulfate, with an evaporation rate of 0.6%·K⁻¹ near ambient temperature, although OA dominates the residual species at the highest temperatures. Different types of OA were characterized with marker ions, diurnal cycles, and positive matrix factorization (PMF and show significant differences in volatility. Reduced hydrocarbon-like OA (HOA, a surrogate for primary OA, POA, oxygenated OA (OOA, a surrogate for secondary OA, SOA, and biomass-burning OA (BBOA separated with PMF were all determined to be semi-volatile. The most aged OOA-1 and its dominant ion, CO₂⁺, consistently exhibited the lowest volatility, with HOA, BBOA, and associated ions for each among the highest. The similar or higher volatility of HOA/POA compared to OOA/SOA contradicts the current representations of OA volatility in most atmospheric models and has important implications for aerosol growth and lifetime. A new technique using the AMS background signal was demonstrated to quantify the fraction of species up to four orders-of-magnitude less volatile than those detectable in the MS mode, which for OA represent ~5% of the non-refractory (NR OA signal. Our results strongly imply that all OA types should be considered

The Finokalia Aerosol Measurement Experiment – 2008 (FAME-08: an overview

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M. Pikridas

2010-07-01

Full Text Available A month (4 May to 8 June 2008 of ambient aerosol, air ion and gas phase sampling (Finokalia Aerosol Measurement Experiment 2008, FAME-08 was conducted at Finokalia, on the island of Crete, Greece. The purpose of the study was to characterize the physical and chemical properties of aged aerosol and to investigate new particle formation. Measurements included aerosol and air ion size distributions, size-resolved chemical composition, organic aerosol thermal volatility, water uptake and particle optical properties (light scattering and absorption. Statistical analysis of the aerosol mass concentration variations revealed the absence of diurnal patterns suggesting the lack of strong local sources. Sulfates accounted for approximately half of the particulate matter less than 1 micrometer in diameter (PM₁ and organics for 28%. The PM₁ organic aerosol fraction was highly oxidized with 80% water soluble. The supermicrometer particles were dominated by crustal components (50%, sea salt (24% and nitrates (16%. The organic carbon to elemental carbon (OC/EC ratio correlated with ozone measurements but with a one-day lag. The average OC/EC ratio for the study period was equal to 5.4. For three days air masses from North Africa resulted in a 6-fold increase of particulate matter less than 10 micrometers in diameter (PM₁₀ and a decrease of the OC/EC ratio by a factor of 2. Back trajectory analysis, based on FLEXPART footprint plots, identified five source regions (Athens, Greece, Africa, other continental and marine, each of which influenced the PM₁ aerosol composition and properties. Marine air masses had the lowest PM₁ concentrations and air masses from the Balkans, Turkey and Eastern Europe the highest.

Source apportionment of submicron organic aerosol collected from Atlanta, Georgia, during 2014-2015 using the aerosol chemical speciation monitor (ACSM)

Science.gov (United States)

Rattanavaraha, Weruka; Canagaratna, Manjula R.; Budisulistiorini, Sri Hapsari; Croteau, Philip L.; Baumann, Karsten; Canonaco, Francesco; Prevot, Andre S. H.; Edgerton, Eric S.; Zhang, Zhenfa; Jayne, John T.; Worsnop, Douglas R.; Gold, Avram; Shaw, Stephanie L.; Surratt, Jason D.

2017-10-01

The Aerodyne Aerosol Chemical Speciation Monitor (ACSM) was redeployed at the Jefferson Street (JST) site in downtown Atlanta, Georgia (GA) for 1 year (March 20, 2014-February 08, 2015) to chemically characterize non-refractory submicron particulate matter (NR-PM1) in near real-time and to assess whether organic aerosol (OA) types and amounts change from year-to-year. Submicron organic aerosol (OA) mass spectra were analyzed by season using multilinear engine (ME-2) to apportion OA subtypes to potential sources and chemical processes. A suite of real-time collocated measurements from the Southeastern Aerosol Research and Characterization (SEARCH) network was compared with ME-2 factor solutions to aid in the interpretation of OA subtypes during each season. OA tracers measured from high-volume filter samples using gas chromatography interfaced with electron ionization-mass spectrometry (GC/EI-MS) also aided in identifying OA sources. The initial application of ME-2 to the yearlong ACSM dataset revealed that OA source apportionment by season was required to better resolve sporadic OA types. Spring and fall OA mass spectral datasets were separated into finer periods to capture potential OA sources resulting from non-homogeneous emissions during transitioning periods. NR-PM1 was highest in summer (16.7 ± 8.4 μg m-3) and lowest in winter (8.0 ± 5.7 μg m-3), consistent with prior studies. OA dominated NR-PM1 mass (56-74% on average) in all seasons. Hydrocarbon-like OA (HOA) from primary emissions was observed in all seasons, averaging 5-22% of total OA mass. Strong correlations of HOA with carbon monoxide (CO) (R = 0.71-0.88) and oxides of nitrogen (NOx) (R = 0.55-0.79) indicated that vehicular traffic was the likely source. Biomass burning OA (BBOA) was observed in all seasons, with lower contributions (2%) in summer and higher in colder seasons (averaging 8-20% of total OA mass). BBOA correlated strongly with levoglucosan (R = 0.78-0.95) during colder seasons

Chemical compositions, methods of making the chemical compositions, and structures made from the chemical compositions

Science.gov (United States)

Yang, Lei; Cheng, Zhe; Liu, Ze; Liu, Meilin

2015-01-13

Embodiments of the present disclosure include chemical compositions, structures, anodes, cathodes, electrolytes for solid oxide fuel cells, solid oxide fuel cells, fuel cells, fuel cell membranes, separation membranes, catalytic membranes, sensors, coatings for electrolytes, electrodes, membranes, and catalysts, and the like, are disclosed.

Aerosol composition, oxidative properties, and sources in Beijing: results from the 2014 Asia-Pacific Economic Cooperation Summit study

Science.gov (United States)

Xu, W. Q.; Sun, Y. L.; Chen, C.; Du, W.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Zhao, X. J.; Zhou, L. B.; Ji, D. S.; Wang, P. C.; Worsnop, D. R.

2015-08-01

The mitigation of air pollution in megacities remains a great challenge because of the complex sources and formation mechanisms of aerosol particles. The 2014 Asia- Pacific Economic Cooperation (APEC) summit in Beijing serves as a unique experiment to study the impacts of emission controls on aerosol composition, size distributions, and oxidative properties. Herein, a high-resolution time-of-flight aerosol mass spectrometer was deployed in urban Beijing for real-time measurements of size-resolved non-refractory submicron aerosol (NR-PM1) species from 14 October to 12 November 2014, along with a range of collocated measurements. The average (±σ) PM1 was 41.6 (±38.9) μg m-3 during APEC, which was decreased by 53 % compared with that before APEC. The aerosol composition showed substantial changes owing to emission controls during APEC. Secondary inorganic aerosols (SIA = sulfate + nitrate + ammonium) showed significant reductions of 62-69 %, whereas organics presented much smaller decreases (35 %). The results from the positive matrix factorization of organic aerosols (OA) indicated that highly oxidized secondary OA (SOA) showed decreases similar to those of SIA during APEC. However, primary OA (POA) from cooking, traffic, and biomass burning sources were comparable to those before APEC, indicating the presence of strong local source emissions. The oxidation properties showed corresponding changes in response to OA composition. The average oxygen-to-carbon level during APEC was 0.36 (±0.10), which is lower than the 0.43 (±0.13) measured before APEC, demonstrating a decrease in the OA oxidation degree. The changes in size distributions of primary and secondary species varied during APEC. SIA and SOA showed significant reductions in large accumulation modes with peak diameters shifting from ~ 650 to 400 nm during APEC, whereas those of POA remained relatively unchanged. The changes in aerosol composition, size distributions, and oxidation degrees during the aging

Aerosol processing in stratiform clouds in ECHAM6-HAM

Science.gov (United States)

Neubauer, David; Lohmann, Ulrike; Hoose, Corinna

2013-04-01

Aerosol processing in stratiform clouds by uptake into cloud particles, collision-coalescence, chemical processing inside the cloud particles and release back into the atmosphere has important effects on aerosol concentration, size distribution, chemical composition and mixing state. Aerosol particles can act as cloud condensation nuclei. Cloud droplets can take up further aerosol particles by collisions. Atmospheric gases may also be transferred into the cloud droplets and undergo chemical reactions, e.g. the production of atmospheric sulphate. Aerosol particles are also processed in ice crystals. They may be taken up by homogeneous freezing of cloud droplets below -38° C or by heterogeneous freezing above -38° C. This includes immersion freezing of already immersed aerosol particles in the droplets and contact freezing of particles colliding with a droplet. Many clouds do not form precipitation and also much of the precipitation evaporates before it reaches the ground. The water soluble part of the aerosol particles concentrates in the hydrometeors and together with the insoluble part forms a single, mixed, larger particle, which is released. We have implemented aerosol processing into the current version of the general circulation model ECHAM6 (Stevens et al., 2013) coupled to the aerosol module HAM (Stier et al., 2005). ECHAM6-HAM solves prognostic equations for the cloud droplet number and ice crystal number concentrations. In the standard version of HAM, seven modes are used to describe the total aerosol. The modes are divided into soluble/mixed and insoluble modes and the number concentrations and masses of different chemical components (sulphate, black carbon, organic carbon, sea salt and mineral dust) are prognostic variables. We extended this by an explicit representation of aerosol particles in cloud droplets and ice crystals in stratiform clouds similar to Hoose et al. (2008a,b). Aerosol particles in cloud droplets are represented by 5 tracers for the

Determination of the power of multielement aerosol composition emission from distant industrial sources

International Nuclear Information System (INIS)

Popova, S.A.; Kutsenogij, K.P.; Chankina, O.V.

2008-01-01

The results from the monitoring of the temporal variability of the multielement composition of atmospheric aerosols are presented. They are used to determine the emission power of a series of elements from distant sources.

In situ chemical composition measurement of individual cloud residue particles at a mountain site, southern China

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Q. Lin

2017-07-01

Full Text Available To investigate how atmospheric aerosol particles interact with chemical composition of cloud droplets, a ground-based counterflow virtual impactor (GCVI coupled with a real-time single-particle aerosol mass spectrometer (SPAMS was used to assess the chemical composition and mixing state of individual cloud residue particles in the Nanling Mountains (1690 m a. s. l. , southern China, in January 2016. The cloud residues were classified into nine particle types: aged elemental carbon (EC, potassium-rich (K-rich, amine, dust, Pb, Fe, organic carbon (OC, sodium-rich (Na-rich and Other. The largest fraction of the total cloud residues was the aged EC type (49.3 %, followed by the K-rich type (33.9 %. Abundant aged EC cloud residues that mixed internally with inorganic salts were found in air masses from northerly polluted areas. The number fraction (NF of the K-rich cloud residues increased within southwesterly air masses from fire activities in Southeast Asia. When air masses changed from northerly polluted areas to southwesterly ocean and livestock areas, the amine particles increased from 0.2 to 15.1 % of the total cloud residues. The dust, Fe, Pb, Na-rich and OC particle types had a low contribution (0.5–4.1 % to the total cloud residues. Higher fraction of nitrate (88–89 % was found in the dust and Na-rich cloud residues relative to sulfate (41–42 % and ammonium (15–23 %. Higher intensity of nitrate was found in the cloud residues relative to the ambient particles. Compared with nonactivated particles, nitrate intensity decreased in all cloud residues except for dust type. To our knowledge, this study is the first report on in situ observation of the chemical composition and mixing state of individual cloud residue particles in China.

A seasonal time history of the size resolved composition of fine aerosol in Manchester UK

Science.gov (United States)

Choularton, Thomas; Martin, Claire; Allan, James; Coe, Hugh; Bower, Keith; Gallagher, Martin

2010-05-01

Numerous studies have been conducted in urban centres now using sophisticated instruments that measure aerosol properties needed to determine their effects on human health, air quality and climate change) showing that a significant fraction of urban aerosols (mainly from automotive sources) are composed of organic compounds with implications for human health. In this project we have produced the first seasonal aerosol composition and emission database for the City of Manchester in the UK Several recent projects have been conducted by SEAES looking at fundamental properties of urban atmospheric aerosol to understand their influence on climate. This work is now expanding through collaboration with the School of Geography & Centre for Occupational & Environmental Health to investigate urban aerosol emission impacts on human health In this paper we present a compendium of data from field campaigns in Manchester city centre over the past decade. The data are from six different campaigns, between 2001 - 2007, each campaign was between 2 weeks and 2 months long predominantly from January and June periods . The data analysis includes air parcel trajectory examination and comparisons with external data, including PM10, CO and NOx data from AURN fixed monitoring sites Six Manchester fine aerosol datasets from the past decade have been quality controlled and analysed regarding averages of the size distributions of Organic, NO3, NH4 and SO4 mass loadings. It was found that: Organic material is the largest single component of the aerosol with primary aliphatic material dominating the smallest sizes, but with oxygenated secondary organic material being important in the accumulation mode. In the accumulation mode the organic material seems to be internally mixed with sulphate and nitrate. The accumulation mode particles were effective as cloud condensation nuclei. Seasonal effects surrounding atmospheric stability and photochemistry were found to play an important role in the

Variation in global chemical composition of PM2.5: emerging results from SPARTAN

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G. Snider

2016-08-01

Full Text Available The Surface PARTiculate mAtter Network (SPARTAN is a long-term project that includes characterization of chemical and physical attributes of aerosols from filter samples collected worldwide. This paper discusses the ongoing efforts of SPARTAN to define and quantify major ions and trace metals found in fine particulate matter (PM2.5. Our methods infer the spatial and temporal variability of PM2.5 in a cost-effective manner. Gravimetrically weighed filters represent multi-day averages of PM2.5, with a collocated nephelometer sampling air continuously. SPARTAN instruments are paired with AErosol RObotic NETwork (AERONET sun photometers to better understand the relationship between ground-level PM2.5 and columnar aerosol optical depth (AOD.We have examined the chemical composition of PM2.5 at 12 globally dispersed, densely populated urban locations and a site at Mammoth Cave (US National Park used as a background comparison. So far, each SPARTAN location has been active between the years 2013 and 2016 over periods of 2–26 months, with an average period of 12 months per site. These sites have collectively gathered over 10 years of quality aerosol data. The major PM2.5 constituents across all sites (relative contribution ± SD are ammoniated sulfate (20 % ± 11 %, crustal material (13.4 % ± 9.9 %, equivalent black carbon (11.9 % ± 8.4 %, ammonium nitrate (4.7 % ± 3.0 %, sea salt (2.3 % ± 1.6 %, trace element oxides (1.0 % ± 1.1 %, water (7.2 % ± 3.3 % at 35 % RH, and residual matter (40 % ± 24 %.Analysis of filter samples reveals that several PM2.5 chemical components varied by more than an order of magnitude between sites. Ammoniated sulfate ranges from 1.1 µg m−3 (Buenos Aires, Argentina to 17 µg m−3 (Kanpur, India in the dry season. Ammonium nitrate ranged from 0.2 µg m−3 (Mammoth Cave, in summer to 6.8  µg m−3 (Kanpur, dry season. Equivalent

Physicochemical Characterization of Capstone Depleted Uranium Aerosols III: Morphologic and Chemical Oxide Analyses

International Nuclear Information System (INIS)

Krupka, Kenneth M.; Parkhurst, MaryAnn; Gold, Kenneth; Arey, Bruce W.; Jenson, Evan D.; Guilmette, Raymond A.

2009-01-01

The impact of depleted uranium (DU) penetrators against an armored target causes erosion and fragmentation of the penetrators, the extent of which is dependent on the thickness and material composition of the target. Vigorous oxidation of the DU particles and fragments creates an aerosol of DU oxide particles and DU particle agglomerations combined with target materials. Aerosols from the Capstone DU aerosol study, in which vehicles were perforated by DU penetrators, were evaluated for their oxidation states using X-ray diffraction (XRD) and particle morphologies using scanning electron microscopy/energy dispersive spectrometry (SEM/EDS). The oxidation state of a DU aerosol is important as it offers a clue to its solubility in lung fluids. The XRD analysis showed that the aerosols evaluated were a combination primarily of U3O8 (insoluble) and UO3 (relatively more soluble) phases, though intermediate phases resembling U4O9 and other oxides were prominent in some samples. Analysis of particle residues in the micrometer-size range by SEM/EDS provided microstructural information such as phase composition and distribution, fracture morphology, size distribution, and material homogeneity. Observations from SEM analysis show a wide variability in the shapes of the DU particles. Some of the larger particles appear to have been fractured (perhaps as a result of abrasion and comminution); others were spherical, occasionally with dendritic or lobed surface structures. Amorphous conglomerates containing metals other than uranium were also common, especially with the smallest particle sizes. A few samples seemed to contain small chunks of nearly pure uranium metal, which were verified by EDS to have a higher uranium content exceeding that expected for uranium oxides. Results of the XRD and SEM/EDS analyses were used in other studies described in this issue of The Journal of Health Physics to interpret the results of lung solubility studies and in selecting input parameters for

MAEROS, Multicomponent Aerosol Time Evolution

International Nuclear Information System (INIS)

1991-01-01

1 - Description of program or function: MAEROS calculates aerosol composition and mass concentration as a function of particle size and time. The processes that may be considered are coagulation due to Brownian motion, gravity, and turbulence; particle deposition due to gravitational settling, diffusion, and thermophoresis; particle growth due to condensation of a gas, typically water vapor, and time-varying sources of particles of different sizes and chemical compositions. 2 - Method of solution: The numerical technique used is based upon dividing the particle size domain into m sections and imposing the condition of mass conservation for each chemical component for the processes considered. Aerosol mass concentrations are grouped into sections (i.e., size classes) for which an average composition is determined. For m sections, a set of 2m(m+2) sectional coefficients must be calculated before integrating in time. These coefficients are determined from the basic coagulation, condensation, and deposition coefficients. Since the sectional coefficients depend on the physical properties of the containment chamber (e.g., temperature, pressure, chamber volume, and deposition surface area), they will generally need to be recalculated for a particular application. However, for a given containment chamber, the sectional coefficients will probably vary only with temperature and pressure. Consequently, the code has been developed so that sectional coefficients are stored at a user-specified upper and lower bound for both temperature and pressure, and linear interpolation is used to determine the appropriate sectional coefficients for a given temperature and pressure. A Runge-Kutta-Fehlberg method is used to integrate in time. 3 - Restrictions on the complexity of the problem - Maxima of: 20 sections, 8 components, 50 rows for plotting, 101 columns for plotting. MAEROS is limited to geometrically spaced sections in particle mass (i.e., v(m+1).GE.2v(m) is the largest particle

Aerosol characterization over the southeastern United States using high-resolution aerosol mass spectrometry: spatial and seasonal variation of aerosol composition and sources with a focus on organic nitrates

Science.gov (United States)

Xu, L.; Suresh, S.; Guo, H.; Weber, R. J.; Ng, N. L.

2015-07-01

We deployed a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and an Aerosol Chemical Speciation Monitor (ACSM) to characterize the chemical composition of submicron non-refractory particulate matter (NR-PM1) in the southeastern USA. Measurements were performed in both rural and urban sites in the greater Atlanta area, Georgia (GA), and Centreville, Alabama (AL), for approximately 1 year as part of Southeastern Center for Air Pollution and Epidemiology study (SCAPE) and Southern Oxidant and Aerosol Study (SOAS). Organic aerosol (OA) accounts for more than half of NR-PM1 mass concentration regardless of sampling sites and seasons. Positive matrix factorization (PMF) analysis of HR-ToF-AMS measurements identified various OA sources, depending on location and season. Hydrocarbon-like OA (HOA) and cooking OA (COA) have important, but not dominant, contributions to total OA in urban sites (i.e., 21-38 % of total OA depending on site and season). Biomass burning OA (BBOA) concentration shows a distinct seasonal variation with a larger enhancement in winter than summer. We find a good correlation between BBOA and brown carbon, indicating biomass burning is an important source for brown carbon, although an additional, unidentified brown carbon source is likely present at the rural Yorkville site. Isoprene-derived OA factor (isoprene-OA) is only deconvolved in warmer months and contributes 18-36 % of total OA. The presence of isoprene-OA factor in urban sites is more likely from local production in the presence of NOx than transport from rural sites. More-oxidized and less-oxidized oxygenated organic aerosol (MO-OOA and LO-OOA, respectively) are dominant fractions (47-79 %) of OA in all sites. MO-OOA correlates well with ozone in summer but not in winter, indicating MO-OOA sources may vary with seasons. LO-OOA, which reaches a daily maximum at night, correlates better with estimated nitrate functionality from organic nitrates than total nitrates. Based

The chemical composition of aerosols from Wildland fires: Current state of the science and possible new directions.

Science.gov (United States)

Wildland fire emits a substantial quantity of aerosol to the atmosphere. These aerosols typically comprise a complex mixture of organic matter and refractory elemental or black carbon with a relatively minor contribution of inorganic matter from soils and plant micronutrients. Id...

Influences of aerosol physiochemical properties and new particle formation on CCN activity from observation at a suburban site of China

Science.gov (United States)

Li, Yanan; Zhang, Fang; Li, Zhanqing; Sun, Li; Wang, Zhenzhu; Li, Ping; Sun, Yele; Ren, Jingye; Wang, Yuying; Cribb, Maureen; Yuan, Cheng

2017-05-01

With the aim of understanding the impact of aerosol particle size and chemical composition on CCN activity, the size-resolved cloud condensation nuclei (CCN) number concentration (NCCN), particle number size distribution (PSD) (10-600 nm), and bulk chemical composition of particles with a diameter China, from 22 July to 26 August 2014. The NCCN was measured at five different supersaturations (SS) ranging from 0.075%-0.76%. Diurnal variations in the aerosol number concentration (NCN), NCCN, the bulk aerosol activation ratio (AR), the hygroscopicity parameter (κchem), and the ratio of 44 mass to charge ration (m/z 44) to total organic signal in the component spectrum (f44), and the PSD were examined integrally to study the influence of particle size and chemical composition on CCN activation. We found that particle size was more related to the CCN activation ratios in the morning, whereas in the afternoon ( 1400 LST), κchem and f44 were more closely associated with the bulk AR. Assuming the internal mixing of aerosol particles, NCCN was estimated using the bulk chemical composition and real-time PSD. We found that the predicted CCN number concentrations were underestimated by 20-30% at SS case during non-NPF event. It has been found that CCN activation was restrained at the ;growth; stage during which larger particle diameters were needed to reach an activation diameter(Da), and the bulk AR decreased as well. However, during the ;leveling-off; stage, a lower Da was observed and CCN activation was greatly enhanced.

Chemical composition, mixing state, size and morphology of Ice nucleating particles at the Jungfraujoch research station, Switzerland

Science.gov (United States)

Ebert, Martin; Worringen, Annette; Kandler, Konrad; Weinbruch, Stephan; Schenk, Ludwig; Mertes, Stephan; Schmidt, Susan; Schneider, Johannes; Frank, Fabian; Nilius, Björn; Danielczok, Anja; Bingemer, Heinz

2014-05-01

An intense field campaign from the Ice Nuclei Research Unit (INUIT) was performed in January and February of 2013 at the High-Alpine Research Station Jungfraujoch (3580 m a.s.l., Switzerland). Main goal was the assessment of microphysical and chemical properties of free-tropospheric ice-nucelating particles. The ice-nucleating particles were discriminated from the total aerosol with the 'Fast Ice Nucleation CHamber' (FINCH; University Frankfurt) and the 'Ice-Selective Inlet' (ISI, Paul Scherer Institute) followed by a pumped counter-stream virtual impactor. The separated ice-nucleating particles were then collected with a nozzle-type impactor. With the 'FRankfurt Ice nuclei Deposition freezinG Experiment' (FRIDGE), aerosol particles are sampled on a silicon wafer, which is than exposed to ice-activating conditions in a static diffusion chamber. The locations of the growing ice crystals are recorded for later analysis. Finally, with the ICE Counter-stream Virtual Impactor (ICE-CVI) atmospheric ice crystals are separated from the total aerosol and their water content is evaporated to retain the ice residual particles, which are then collected also by impactor sampling. All samples were analyzed in a high-resolution scanning electron microscope. By this method, for each particle its size, morphology, mixing-state and chemical composition is obtained. In total approximately 1700 ice nucleating particles were analyzed. Based on their chemical composition, the particles were classified into seven groups: silicates, metal oxides, Ca-rich particles, (aged) sea-salt, soot, sulphates and carbonaceous matter. Sea-salt is considered as artifact and is not regarded as ice nuclei here. The most frequent ice nucleating particles/ice residuals at the Jungfraujoch station are silicates > carbonaceous particles > metal oxides. Calcium-rich particles and soot play a minor role. Similar results are obtained by quasi-parallel measurements with an online single particle laser ablation

Formation of the natural sulfate aerosol

Energy Technology Data Exchange (ETDEWEB)

Kerminen, V M; Hillamo, R; Maekinen, M; Virkkula, A; Maekelae, T; Pakkanen, T [Helsinki Univ. (Finland). Dept. of Physics

1997-12-31

Anthropogenic sulfate aerosol, together with particles from biomass burning, may significantly reduce the climatic warming due to man-made greenhouse gases. The radiative forcing of aerosol particles is based on their ability to scatter and absorb solar radiation (direct effect), and on their influences on cloud albedos and lifetimes (indirect effect). The direct aerosol effect depends strongly on the size, number and chemical composition of particles, being greatest for particles of 0.1-1 {mu}m in diameter. The indirect aerosol effect is dictated by the number of particles being able to act as cloud condensation nuclei (CCN). For sulfate particles, the minimum CCN size in tropospheric clouds is of the order of 0.05-0.2 {mu}m. To improve aerosol parameterizations in future climate models, it is required that (1) both primary and secondary sources of various particle types will be characterized at a greater accuracy, and (2) the influences of various atmospheric processes on the spatial and temporal distribution of these particles and their physico-chemical properties are known much better than at the present. In estimating the climatic forcing due to the sulfate particles, one of the major problems is to distinguish between sulfur from anthropogenic sources and that of natural origin. Global emissions of biogenic and anthropogenic sulfate pre-cursors are comparable in magnitude, but over regional scales either of these two source types may dominate. The current presentation is devoted to discussing the natural sulfate aerosol, including the formation of sulfur-derived particles in the marine environment, and the use of particulate methanesulfonic acid (MSA) as a tracer for the natural sulfate

Formation of the natural sulfate aerosol

Energy Technology Data Exchange (ETDEWEB)

Kerminen, V.M.; Hillamo, R.; Maekinen, M.; Virkkula, A.; Maekelae, T.; Pakkanen, T. [Helsinki Univ. (Finland). Dept. of Physics

1996-12-31

Anthropogenic sulfate aerosol, together with particles from biomass burning, may significantly reduce the climatic warming due to man-made greenhouse gases. The radiative forcing of aerosol particles is based on their ability to scatter and absorb solar radiation (direct effect), and on their influences on cloud albedos and lifetimes (indirect effect). The direct aerosol effect depends strongly on the size, number and chemical composition of particles, being greatest for particles of 0.1-1 {mu}m in diameter. The indirect aerosol effect is dictated by the number of particles being able to act as cloud condensation nuclei (CCN). For sulfate particles, the minimum CCN size in tropospheric clouds is of the order of 0.05-0.2 {mu}m. To improve aerosol parameterizations in future climate models, it is required that (1) both primary and secondary sources of various particle types will be characterized at a greater accuracy, and (2) the influences of various atmospheric processes on the spatial and temporal distribution of these particles and their physico-chemical properties are known much better than at the present. In estimating the climatic forcing due to the sulfate particles, one of the major problems is to distinguish between sulfur from anthropogenic sources and that of natural origin. Global emissions of biogenic and anthropogenic sulfate pre-cursors are comparable in magnitude, but over regional scales either of these two source types may dominate. The current presentation is devoted to discussing the natural sulfate aerosol, including the formation of sulfur-derived particles in the marine environment, and the use of particulate methanesulfonic acid (MSA) as a tracer for the natural sulfate

Aerosol composition of urban plumes passing over a rural monitoring site

International Nuclear Information System (INIS)

Ellestad, T.G.

1980-01-01

A field study conducted at a ground site 100 km north of St. Louis, Mo., to measure the aerosol composition and gaseous concentrations of urban plumes passing the site is discussed. Coarse and fine aerosol elemental concentrations, height scattering, meteorological data and concentrations of SO 2 , CO, O 3 , and NO-NO/sub x/ were measured and then analyzed together with data from associate investigators on fluorocarbon-11, total hydrocarbons, and size distributions. The results show that: (1) gaseous and elemental aerosol concentrations at the ground site 100 km from the St. Louis urban area were clearly influenced by the St. Louis urban plume, (2) the urban plumes of Chicago and Indianapolis, 350 km from the ground site, may have been detected, (3) sulfur compounds, presumably sulfates, accounted for 30-40% of the mass loading within the St. Louis urban plume, and resided almost entirely within the size range below 2.5 microns, (4) the most reliable urban-plume tracers in this study were fine Pb, fluorocarbon-11, total nonmethane hydrocarbons, and CO, and (5) over a period of several days, there may have been a regional buildup of fine S, light scattering, aerosol mass, O 3 , and NO/sub x/ and, to a lesser extent, CO and fluorocarbon-11

GEM-AQ/EC, an on-line global multi-scale chemical weather modelling system: model development and evaluation of global aerosol climatology

Directory of Open Access Journals (Sweden)

S. L. Gong

2012-09-01

Full Text Available A global air quality modeling system GEM-AQ/EC was developed by implementing tropospheric chemistry and aerosol processes on-line into the Global Environmental Multiscale weather prediction model – GEM. Due to the multi-scale features of the GEM, the integrated model, GEM-AQ/EC, is able to investigate chemical weather at scales from global to urban domains. The current chemical mechanism is comprised of 50 gas-phase species, 116 chemical and 19 photolysis reactions, and is complemented by a sectional aerosol module CAM (The Canadian Aerosol Module with 5 aerosols types: sulphate, black carbon, organic carbon, sea-salt and soil dust. Monthly emission inventories of black carbon and organic carbon from boreal and temperate vegetation fires were assembled using the most reliable areas burned datasets by countries, from statistical databases and derived from remote sensing products of 1995–2004. The model was run for ten years from from 1995–2004 with re-analyzed meteorology on a global uniform 1° × 1° horizontal resolution domain and 28 hybrid levels extending up to 10 hPa. The simulating results were compared with various observations including surface network around the globe and satellite data. Regional features of global aerosols are reasonably captured including emission, surface concentrations and aerosol optical depth. For various types of aerosols, satisfactory correlations were achieved between modeled and observed with some degree of systematic bias possibly due to large uncertainties in the emissions used in this study. A global distribution of natural aerosol contributions to the total aerosols is obtained and compared with observations.

Chemical composition of aerosol, sea fog, and rainwater in the marine boundary layer of the northwestern North Pacific and its marginal seas

Science.gov (United States)

Sasakawa, Motoki; Uematsu, Mitsuo

2002-12-01

Samples of aerosol, sea fog, and rainwater were collected during a research cruise in the northwestern North Pacific, the Sea of Okhotsk, and the Sea of Japan in the summer of 1998. High concentrations of NO3-, nss-SO42- and NH4+ in aerosol over the Sea of Japan suggest that anthropogenic substances were transported to this region. Although the Sea of Okhotsk was covered with a clean marine air mass, the concentration of nss-SO42- was comparatively high in the aerosol samples. This nss-SO42- is probably of marine biogenic origin. The pH values of fogwater samples were measured to be fogwater collected over the Sea of Japan were higher than those in the other regions, suggesting that the sea fog scavenged anthropogenic substances. The concentration of nss-SO42- in fogwater over the Sea of Okhotsk was equivalent to that over the Sea of Japan, probably because nss-SO42- and SO2 of marine biogenic origin were scavenged by the sea fog over the Sea of Okhotsk. The pH values of rainwater samples ranged from 6.1 to 7.2 during the cruise, and acidification of the rain was not significant. The concentrations of nss-Ca2+ in the rainwater were higher than those of the fogwater. This suggests that the rain-scavenged continental CaCO3 may have existed above the lower marine boundary layer, where sea fog appeared. Comparisons of the composition of aerosol and fogwater indicated that coarse particles, such as sea salts predominantly act as condensation nuclei of sea fog droplets rather than fine particles such as (NH4)2SO4.

Boundary layer aerosol size distribution, mass concentration and mineralogical composition in Morocco and at Cape Verde Islands during SAMUM I-II

Science.gov (United States)

Kandler, K.; Lieke, K.

2009-04-01

The Saharan Mineral Dust Experiment (SAMUM) is dedicated to the understanding of the radiative effects of mineral dust. Two major field experiments were performed: A first joint field campaign took place at Ouarzazate and near Zagora, southern Morocco, from May 13 to June 7, 2006. Aircraft and ground based measurements of aerosol physical and chemical properties were carried out to collect a data set of surface and atmospheric columnar information within a major dust source. This data set combined with satellite data provides the base of the first thorough columnar radiative closure tests in Saharan dust. A second field experiment was conducted during January-February 2008, in the Cape Verde Islands region, where about 300 Tg of mineral dust are transported annually from Western Africa across the Atlantic towards the Caribbean Sea and the Amazon basin. Along its transport path, the mineral dust is expected to influence significantly the radiation budget - by direct and indirect effects - of the subtropical North Atlantic. We are lacking a radiative closure in the Saharan air plume. One focus of the investigation within the trade wind region is the spatial distribution of mixed dust/biomass/sea salt aerosol and their physical and chemical properties, especially with regard to radiative effects. We report on measurements of size distributions, mass concentrations and mineralogical composition conducted at the Zagora (Morocco) and Praia (Cape Verde islands) ground stations. The aerosol size distribution was measured from 20 nm to 500

Characterization of a large biogenic secondary organic aerosol event from eastern Canadian forests

Science.gov (United States)

Slowik, J. G.; Stroud, C.; Bottenheim, J. W.; Brickell, P. C.; Chang, R. Y.-W.; Liggio, J.; Makar, P. A.; Martin, R. V.; Moran, M. D.; Shantz, N. C.; Sjostedt, S. J.; van Donkelaar, A.; Vlasenko, A.; Wiebe, H. A.; Xia, A. G.; Zhang, J.; Leaitch, W. R.; Abbatt, J. P. D.

2010-03-01

Measurements of aerosol composition, volatile organic compounds, and CO are used to determine biogenic secondary organic aerosol (SOA) concentrations at a rural site 70 km north of Toronto. These biogenic SOA levels are many times higher than past observations and occur during a period of increasing temperatures and outflow from Northern Ontario and Quebec forests in early summer. A regional chemical transport model approximately predicts the event timing and accurately predicts the aerosol loading, identifying the precursors as monoterpene emissions from the coniferous forest. The agreement between the measured and modeled biogenic aerosol concentrations contrasts with model underpredictions for polluted regions. Correlations of the oxygenated organic aerosol mass with tracers such as CO support a secondary aerosol source and distinguish biogenic, pollution, and biomass burning periods during the field campaign. Using the Master Chemical Mechanism, it is shown that the levels of CO observed during the biogenic event are consistent with a photochemical source arising from monoterpene oxidation. The biogenic aerosol mass correlates with satellite measurements of regional aerosol optical depth, indicating that the event extends across the eastern Canadian forest. This regional event correlates with increased temperatures, indicating that temperature-dependent forest emissions can significantly affect climate through enhanced direct optical scattering and higher cloud condensation nuclei numbers.

Vacuum FTIR study on the hygroscopicity of magnesium acetate aerosols

Science.gov (United States)

Wang, Na; Cai, Chen; He, Xiang; Pang, Shu-Feng; Zhang, Yun-Hong

2018-03-01

Hygroscopicity and volatility of secondary organic aerosol (SOA) are two important properties, which determine the composition, concentration, size, phase state of SOA and thus chemical and optical properties for SOA. In this work, magnesium acetate (Mg(Ac)2) aerosol was used as a simple SOA model in order to reveal relationship between hygroscopicity and volatility. A novel approach was set up based on a combination of a vacuum FTIR spectrometer and a home-made relative humidity (RH) controlling system. The striking advantage of this approach was that the RH and the compositions of aerosols could be obtained from a same IR spectrum, which guaranteed the synchronism between RH and spectral features on a sub-second scale. At the constant RH of 90% and 80% for 3000 s, the water content within Mg(Ac)2 aerosol particles decreased about 19.0% and 9.4% while there were 13.4% and 6.0% of acetate loss. This was attributed to a cooperation between volatile of acetic acid and Mg2 + hydrolysis in Mg(Ac)2 aerosols, which greatly suppressed the hygroscopicity of Mg(Ac)2 aerosols. When the RH changed with pulsed mode between 70% and 90%, hygroscopicity relaxation was observed for Mg(Ac)2 aerosols. Diffuse coefficient of water in the relaxation process was estimated to be 5 × 10- 12 m2·s- 1 for the Mg(Ac)2 aerosols. Combining the IR spectra analysis, the decrease in the diffuse coefficient of water was due to the formation of magnesium hydroxide accompanying acetic acid evaporation in the aerosols.

Light absorption of secondary organic aerosol: Composition and contribution of nitro-aromatic compounds

Science.gov (United States)

Secondary organic aerosol (SOA) might affect the atmospheric radiation balance through absorbing light at shorter visible and UV wavelengths. However, the composition and optical properties of light-absorbing SOA is poorly understood. In this work, SOA filter samples were collect...

Radioactive aerosols of the object 'Ukryttya' (a review). Part 4.2. Sources and generation of radioactive aerosols during technogenic activities in 1987 - 2005

International Nuclear Information System (INIS)

Ogorodnikov, B.I.; Pazukhin, Eh.M.

2006-01-01

The sources of radioactive aerosol formation were considered at operation. It is shown that concentrations, radionuclide composition, size distribution, transfer and transformation in environment depended on physical and chemical processes proceeding within reactor breakdown, man-caused activity into premises of the object 'Shelter' and near ChNPP. 34 refs.; 7 figs.; 11 tab

Water-soluble components in PM10 aerosols over an urban and a suburban site in the city of Sfax (Tunisia)

OpenAIRE

AZRI, C.; MABROUK, C.; ABIDA, H.; MEDHIOUB, K.

2010-01-01

This study examines the influence of source and meteorological factors on the physico-chemical characteristics of atmospheric aerosols collected at two sampling sites, urban and suburban, in the city of Sfax (Tunisia) during the year of 2004. Atmospheric aerosols were further analyzed for their chemical composition and spatio-temporal evolution was investigated. Based on particle content distribution, the species studied were classified into distinct groups with different content and temporal...

A unified approach to infrared aerosol remote sensing and type specification

Directory of Open Access Journals (Sweden)

L. Clarisse

2013-02-01

Full Text Available Atmospheric aerosols impact air quality and global climate. Space based measurements are the best way to observe their spatial and temporal distributions, and can also be used to gain better understanding of their chemical, physical and optical properties. Aerosol composition is the key parameter affecting the refractive index, which determines how much radiation is scattered and absorbed. Composition of aerosols is unfortunately not measured by state of the art satellite remote sounders. Here we use high resolution infrared measurements for aerosol type differentiation, exploiting, in that part of spectrum, the dependency of their refractive index on wavelength. We review existing detection methods and present a unified detection method based on linear discrimination analysis. We demonstrate this method on measurements of the Infrared Atmospheric Sounding Interferometer (IASI and five different aerosol types, namely volcanic ash, windblown sand, sulfuric acid droplets, ammonium sulfate and smoke particles. We compare these with traditional MODIS AOD measurements. The detection of the last three types is unprecedented in the infrared in nadir mode, but is very promising, especially for sulfuric acid droplets which are detected in the lower troposphere and up to 6 months after injection in the upper troposphere/lower stratosphere.

Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the UK

Science.gov (United States)

McMeeking, G. R.; Morgan, W. T.; Flynn, M.; Highwood, E. J.; Turnbull, K.; Haywood, J.; Coe, H.

2011-05-01

Black carbon (BC) aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2) measurements of refractory BC (rBC) mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the UK. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM). We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS) and used positive matrix factorization to separate hydrocarbon-like (HOA) and oxygenated organic aerosols (OOA). We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NOx) ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NOx and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA) did change for different air masses, with lower SSA observed in

Computing Equilibrium Chemical Compositions

Science.gov (United States)

Mcbride, Bonnie J.; Gordon, Sanford

1995-01-01

Chemical Equilibrium With Transport Properties, 1993 (CET93) computer program provides data on chemical-equilibrium compositions. Aids calculation of thermodynamic properties of chemical systems. Information essential in design and analysis of such equipment as compressors, turbines, nozzles, engines, shock tubes, heat exchangers, and chemical-processing equipment. CET93/PC is version of CET93 specifically designed to run within 640K memory limit of MS-DOS operating system. CET93/PC written in FORTRAN.

Aerosol composition and its application in air pollution monitoring

International Nuclear Information System (INIS)

Sadasivan, S.; Negi, B.S.; Meenakshy, V.; Nambi, K.S.V.

1994-01-01

Aerosol composition measurements have been carried out in our laboratory using nuclear and related techniques. A brief overview of results from the earlier studies and the scope of the present project are outlined. The analytical procedures in use along with the systems available are detailed. Changes envisaged in sampling and analysis are briefly discussed. Results of two case studies relating to air pollution which are investigated using INAA/EDXRF are presented. The work plan under the CRP is outlined. (author). 11 refs, 2 figs, 5 tabs

Tracing of aerosol sources in an urban environment using chemical, Sr isotope, and mineralogical characterization.

Science.gov (United States)

Duarte, Regina M B O; Matos, João T V; Paula, Andreia S; Lopes, Sónia P; Ribeiro, Sara; Santos, José Francisco; Patinha, Carla; da Silva, Eduardo Ferreira; Soares, Rosário; Duarte, Armando C

2017-04-01

In the framework of two national research projects (ORGANOSOL and CN-linkAIR), fine particulate matter (PM 2.5 ) was sampled for 17 months at an urban location in the Western European Coast. The PM 2.5 samples were analyzed for organic carbon (OC), water-soluble organic carbon (WSOC), elemental carbon (EC), major water-soluble inorganic ions, mineralogical, and for the first time in this region, strontium isotope ( 87 Sr/ 86 Sr) composition. Organic matter dominates the identifiable urban PM 2.5 mass, followed by secondary inorganic aerosols. The acquired data resulted also in a seasonal overview of the carbonaceous and inorganic aerosol composition, with an important contribution from primary biomass burning and secondary formation processes in colder and warmer periods, respectively. The fossil-related primary EC seems to be continually present throughout the sampling period. The 87 Sr/ 86 Sr ratios were measured on both the labile and residual PM 2.5 fractions as well as on the bulk PM 2.5 samples. Regardless of the air mass origin, the residual fractions are more radiogenic (representative of a natural crustal dust source) than the labile fractions, whose 87 Sr/ 86 Sr ratios are comparable to that of seawater. The 87 Sr/ 86 Sr ratios and the mineralogical composition data further suggest that sea salt and mineral dust are important primary natural sources of fine aerosols throughout the sampling period.

Contrasting organic aerosol particles from boreal and tropical forests during HUMPPA-COPEC-2010 and AMAZE-08 using coherent vibrational spectroscopy

Directory of Open Access Journals (Sweden)

C. J. Ebben

2011-10-01

Full Text Available We present the vibrational sum frequency generation spectra of organic particles collected in a boreal forest in Finland and a tropical forest in Brazil. These spectra are compared to those of secondary organic material produced in the Harvard Environmental Chamber. By comparing coherent vibrational spectra of a variety of terpene and olefin reference compounds, along with the secondary organic material synthesized in the environmental chamber, we show that submicron aerosol particles sampled in Southern Finland during HUMPPA-COPEC-2010 are composed to a large degree of material similar in chemical composition to synthetic α-pinene-derived material. For material collected in Brazil as part of AMAZE-08, the organic component is found to be chemically complex in the coarse mode but highly uniform in the fine mode. When combined with histogram analyses of the isoprene and monoterpene abundance recorded during the HUMPPA-COPEC-2010 and AMAZE-08 campaigns, the findings presented here indicate that if air is rich in monoterpenes, submicron-sized secondary aerosol particles that form under normal OH and O₃ concentration levels can be described in terms of their hydrocarbon content as being similar to α-pinene-derived model secondary organic aerosol particles. If the isoprene concentration dominates the chemical composition of organic compounds in forest air, then the hydrocarbon component of secondary organic material in the submicron size range is not simply well-represented by that of isoprene-derived model secondary organic aerosol particles but is more complex. Throughout the climate-relevant size range of the fine mode, however, we find that the chemical composition of the secondary organic particle material from such air is invariant with size, suggesting that the particle growth does not change the chemical composition of the hydrocarbon component of the particles in a significant way.

MATRIX-VBS (v1.0): Implementing an Evolving Organic Aerosol Volatility in an Aerosol Microphysics Model

Science.gov (United States)

Gao, Chloe Y.; Tsigaridis, Kostas; Bauer, Susanne E.

2017-01-01

The gas-particle partitioning and chemical aging of semi-volatile organic aerosol are presented in a newly developed box model scheme, where its effect on the growth, composition, and mixing state of particles is examined. The volatility-basis set (VBS) framework is implemented into the aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state), which resolves mass and number aerosol concentrations and in multiple mixing-state classes. The new scheme, MATRIX-VBS, has the potential to significantly advance the representation of organic aerosols in Earth system models by improving upon the conventional representation as non-volatile particulate organic matter, often also with an assumed fixed size distribution. We present results from idealized cases representing Beijing, Mexico City, a Finnish forest, and a southeastern US forest, and investigate the evolution of mass concentrations and volatility distributions for organic species across the gas and particle phases, as well as assessing their mixing state among aerosol populations. Emitted semi-volatile primary organic aerosols evaporate almost completely in the intermediate-volatility range, while they remain in the particle phase in the low-volatility range. Their volatility distribution at any point in time depends on the applied emission factors, oxidation by OH radicals, and temperature. We also compare against parallel simulations with the original scheme, which represented only the particulate and non-volatile component of the organic aerosol, examining how differently the condensed-phase organic matter is distributed across the mixing states in the model. The results demonstrate the importance of representing organic aerosol as a semi-volatile aerosol, and explicitly calculating the partitioning of organic species between the gas and particulate phases.

Physicochemical characterization of Capstone depleted uranium aerosols III: morphologic and chemical oxide analyses.

Science.gov (United States)

Krupka, Kenneth M; Parkhurst, Mary Ann; Gold, Kenneth; Arey, Bruce W; Jenson, Evan D; Guilmette, Raymond A

2009-03-01

The impact of depleted uranium (DU) penetrators against an armored target causes erosion and fragmentation of the penetrators, the extent of which is dependent on the thickness and material composition of the target. Vigorous oxidation of the DU particles and fragments creates an aerosol of DU oxide particles and DU particle agglomerations combined with target materials. Aerosols from the Capstone DU aerosol study, in which vehicles were perforated by DU penetrators, were evaluated for their oxidation states using x-ray diffraction (XRD), and particle morphologies were examined using scanning electron microscopy/energy dispersive spectroscopy (SEM/EDS). The oxidation state of a DU aerosol is important as it offers a clue to its solubility in lung fluids. The XRD analysis showed that the aerosols evaluated were a combination primarily of U3O8 (insoluble) and UO3 (relatively more soluble) phases, though intermediate phases resembling U4O9 and other oxides were prominent in some samples. Analysis of particle residues in the micrometer-size range by SEM/EDS provided microstructural information such as phase composition and distribution, fracture morphology, size distribution, and material homogeneity. Observations from SEM analysis show a wide variability in the shapes of the DU particles. Some of the larger particles were spherical, occasionally with dendritic or lobed surface structures. Others appear to have fractures that perhaps resulted from abrasion and comminution, or shear bands that developed from plastic deformation of the DU material. Amorphous conglomerates containing metals other than uranium were also common, especially with the smallest particle sizes. A few samples seemed to contain small bits of nearly pure uranium metal, which were verified by EDS to have a higher uranium content exceeding that expected for uranium oxides. Results of the XRD and SEM/EDS analyses were used in other studies described in this issue of Health Physics to interpret the

Chemical composition of Chinese palm fruit and chemical properties ...

African Journals Online (AJOL)

... chemical properties and could be used as edible oils and for industrial applications. ... on it, which can provide useful information for Chinese oil palm industry. Key words: Chemical composition, palm fruit, palm oil, palm kernel oil, chemical ...

The composition and variability of atmospheric aerosol over Southeast Asia during 2008

Directory of Open Access Journals (Sweden)

W. Trivitayanurak

2012-01-01

Full Text Available We use a nested version of the GEOS-Chem global 3-D chemistry transport model to better understand the composition and variation of aerosol over Borneo and the broader Southeast Asian region in conjunction with aircraft and satellite observations. Our focus on Southeast Asia reflects the importance of this region as a source of reactive organic gases and aerosols from natural forests, biomass burning, and food and fuel crops. We particularly focus on July 2008 when the UK BAe-146 research aircraft was deployed over northern Malaysian Borneo as part of the ACES/OP3 measurement campaign. During July 2008 we find using the model that Borneo (defined as Borneo Island and the surrounding Indonesian islands was a net exporter of primary organic aerosol (42 kT and black carbon aerosol (11 kT. We find only 13% of volatile organic compound oxidation products partition to secondary organic aerosol (SOA, with Borneo being a net exporter of SOA (15 kT. SOA represents approximately 19% of the total organic aerosol over the region. Sulphate is mainly from aqueous-phase oxidation (68%, with smaller contributions from gas-phase oxidation (15% and advection into the regions (14%. We find that there is a large source of sea salt, as expected, but this largely deposits within the region; we find that dust aerosol plays only a relatively small role in the aerosol burden. In contrast to coincident surface measurements over Northern Borneo that find a pristine environment with evidence for substantial biogenic SOA formation we find that the free troposphere is influenced by biomass burning aerosol transported from the northwest of the Island and further afield. We find several transport events during July 2008 over Borneo associated with elevated aerosol concentrations, none of which coincide with the aircraft flights. We use MODIS aerosol optical depths (AOD data and the model to put the July campaign into a longer temporal perspective. We find that Borneo is where

The composition and variability of atmospheric aerosol over Southeast Asia during 2008

Science.gov (United States)

Trivitayanurak, W.; Palmer, P. I.; Barkley, M. P.; Robinson, N. H.; Coe, H.; Oram, D. E.

2012-01-01

We use a nested version of the GEOS-Chem global 3-D chemistry transport model to better understand the composition and variation of aerosol over Borneo and the broader Southeast Asian region in conjunction with aircraft and satellite observations. Our focus on Southeast Asia reflects the importance of this region as a source of reactive organic gases and aerosols from natural forests, biomass burning, and food and fuel crops. We particularly focus on July 2008 when the UK BAe-146 research aircraft was deployed over northern Malaysian Borneo as part of the ACES/OP3 measurement campaign. During July 2008 we find using the model that Borneo (defined as Borneo Island and the surrounding Indonesian islands) was a net exporter of primary organic aerosol (42 kT) and black carbon aerosol (11 kT). We find only 13% of volatile organic compound oxidation products partition to secondary organic aerosol (SOA), with Borneo being a net exporter of SOA (15 kT). SOA represents approximately 19% of the total organic aerosol over the region. Sulphate is mainly from aqueous-phase oxidation (68%), with smaller contributions from gas-phase oxidation (15%) and advection into the regions (14%). We find that there is a large source of sea salt, as expected, but this largely deposits within the region; we find that dust aerosol plays only a relatively small role in the aerosol burden. In contrast to coincident surface measurements over Northern Borneo that find a pristine environment with evidence for substantial biogenic SOA formation we find that the free troposphere is influenced by biomass burning aerosol transported from the northwest of the Island and further afield. We find several transport events during July 2008 over Borneo associated with elevated aerosol concentrations, none of which coincide with the aircraft flights. We use MODIS aerosol optical depths (AOD) data and the model to put the July campaign into a longer temporal perspective. We find that Borneo is where the model

Composition and sources of winter and summertime aerosols at Ny Alesund, Spitsbergen

International Nuclear Information System (INIS)

Maenhaut, W.; Cornille, P.; Pacyna, J.M.

1991-01-01

Filter samples of < 2.5 μm aerosol were collected in (late) winter of 1983, 1984, 1986, and 1987 and in the summer of 1984, 1986, and 1987 at Ny Alesund, Spitsbergen, and analyzed for over 40 elements by a combination of INAA and PIXE. The data sets of the various sampling campaigns and the combined winter and combined summer data were examined by receptor modeling, including absolute principal component analysis (APCA), chemical mass balance (CMB) and multiple linear regression (MLR) techniques. APCA yielded four components, both for the winter and for the summer aerosol. For the winter aerosol, the components were identified as a general pollution component, crustal dust, sea-salt, and a halogen (Br,I) component. The CMB and MLR calculations were used to obtain source (source region) apportionments for the anthropogenic trace elements and for sulfate. For the summer, about 50% of the sulfate was attributed to a marine biogenic source

PM2.5 Chemical Composition at a Rural Background Site in Central Europe, Including Correlation and Air Mass Back Trajectory Analysis.

Czech Academy of Sciences Publication Activity Database

Schwarz, Jaroslav; Cusack, Michael; Karban, Jindřich; Chalupníčková, E.; Havránek, Vladimír; Smolík, Jiří; Ždímal, Vladimír

176-177, JUL 1 (2016), s. 108-120 ISSN 0169-8095 R&D Projects: GA ČR(CZ) GAP209/11/1342; GA MŠk(CZ) LM2011019 EU Projects: European Commission(XE) 262254 - ACTRIS Institutional support: RVO:67985858 ; RVO:61389005 Keywords : rural aerosol * PM2.5 * chemical composition Subject RIV: CF - Physical ; Theoretical Chemistry; BG - Nuclear, Atomic and Molecular Physics, Colliders (UJF-V) Impact factor: 3.778, year: 2016

Water soluble organic aerosols in the Colorado Rocky Mountains, USA: composition, sources and optical properties

OpenAIRE

Xie, Mingjie; Mladenov, Natalie; Williams, Mark W.; Neff, Jason C.; Wasswa, Joseph; Hannigan, Michael P.

2016-01-01

Atmospheric aerosols have been shown to be an important input of organic carbon and nutrients to alpine watersheds and influence biogeochemical processes in these remote settings. For many remote, high elevation watersheds, direct evidence of the sources of water soluble organic aerosols and their chemical and optical characteristics is lacking. Here, we show that the concentration of water soluble organic carbon (WSOC) in the total suspended particulate (TSP) load at a high elevation site in...

Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the United Kingdom

Science.gov (United States)

McMeeking, G. R.; Morgan, W. T.; Flynn, M.; Highwood, E. J.; Turnbull, K.; Haywood, J.; Coe, H.

2011-09-01

Black carbon (BC) aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2) measurements of refractory BC (rBC) mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the United Kingdom. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM). We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS) and used positive matrix factorization to separate hydrocarbon-like (HOA) and oxygenated organic aerosols (OOA). We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NOx) ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NOx and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA) did change for different air masses, with lower SSA

Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the United Kingdom

Directory of Open Access Journals (Sweden)

G. R. McMeeking

2011-09-01

Full Text Available Black carbon (BC aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2 measurements of refractory BC (rBC mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the United Kingdom. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA operated by the Facility for Airborne Atmospheric Measurements (FAAM. We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS and used positive matrix factorization to separate hydrocarbon-like (HOA and oxygenated organic aerosols (OOA. We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NO_x ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NO_x and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA did change for

Laboratory Studies of Planetary Hazes: composition of cool exoplanet atmospheric aerosols with very high resolution mass spectrometry

Science.gov (United States)

Moran, Sarah E.; Horst, Sarah; He, Chao; Flandinet, Laurene; Moses, Julianne I.; Orthous-Daunay, Francois-Regis; Vuitton, Veronique; Wolters, Cedric; Lewis, Nikole

2017-10-01

We present first results of the composition of laboratory-produced exoplanet haze analogues. With the Planetary HAZE Research (PHAZER) Laboratory, we simulated nine exoplanet atmospheres of varying initial gas phase compositions representing increasing metallicities (100x, 1000x, and 10000x solar) and exposed them to three different temperature regimes (600, 400, and 300 K) with two different “instellation” sources (a plasma source and a UV lamp). The PHAZER exoplanet experiments simulate a temperature and atmospheric composition phase space relevant to the expected planetary yield of the Transiting Exoplanet Survey Satellite (TESS) mission as well as recently discovered potentially habitable zone exoplanets in the TRAPPIST-1, LHS-1140, and Proxima Centauri systems. Upon exposure to the energy sources, all of these experiments produced aerosol particles, which were collected in a dry nitrogen glove box and then analyzed with an LTQ Orbitrap XL™ Hybrid Ion Trap-Orbitrap Mass Spectrometer utilizing m/z ranging from 50 to 1000. The collected aerosol samples were found to contain complex organics. Constraining the composition of these aerosols allows us to better understand the photochemical and dynamical processes ongoing in exoplanet atmospheres. Moreover, these data can inform our telescope observations of exoplanets, which is of critical importance as we enter a new era of exoplanet atmosphere observation science with the upcoming launch of the James Webb Space Telescope. The molecular makeup of these haze particles provides key information for understanding exoplanet atmospheric spectra, and constraining the structure and behavior of clouds, hazes, and other aerosols is at the forefront of exoplanet atmosphere science.

Dust Composition in Climate Models: Current Status and Prospects

Science.gov (United States)

Pérez García-Pando, C.; Miller, R. L.; Perlwitz, J. P.; Kok, J. F.; Scanza, R.; Mahowald, N. M.

2015-12-01

Mineral dust created by wind erosion of soil particles is the dominant aerosol by mass in the atmosphere. It exerts significant effects on radiative fluxes, clouds, ocean biogeochemistry, and human health. Models that predict the lifecycle of mineral dust aerosols generally assume a globally uniform mineral composition. However, this simplification limits our understanding of the role of dust in the Earth system, since the effects of dust strongly depend on the particles' physical and chemical properties, which vary with their mineral composition. Hence, not only a detailed understanding of the processes determining the dust emission flux is needed, but also information about its size dependent mineral composition. Determining the mineral composition of dust aerosols is complicated. The largest uncertainty derives from the current atlases of soil mineral composition. These atlases provide global estimates of soil mineral fractions, but they are based upon massive extrapolation of a limited number of soil samples assuming that mineral composition is related to soil type. This disregards the potentially large variability of soil properties within each defined soil type. In addition, the analysis of these soil samples is based on wet sieving, a technique that breaks the aggregates found in the undisturbed parent soil. During wind erosion, these aggregates are subject to partial fragmentation, which generates differences on the size distribution and composition between the undisturbed parent soil and the emitted dust aerosols. We review recent progress on the representation of the mineral and chemical composition of dust in climate models. We discuss extensions of brittle fragmentation theory to prescribe the emitted size-resolved dust composition, and we identify key processes and uncertainties based upon model simulations and an unprecedented compilation of observations.

Characterization of distinct Arctic aerosol accumulation modes and their sources

Science.gov (United States)

Lange, R.; Dall'Osto, M.; Skov, H.; Nøjgaard, J. K.; Nielsen, I. E.; Beddows, D. C. S.; Simo, R.; Harrison, R. M.; Massling, A.

2018-06-01

In this work we use cluster analysis of long term particle size distribution data to expand an array of different shorter term atmospheric measurements, thereby gaining insights into longer term patterns and properties of Arctic aerosol. Measurements of aerosol number size distributions (9-915 nm) were conducted at Villum Research Station (VRS), Station Nord in North Greenland during a 5 year record (2012-2016). Alongside this, measurements of aerosol composition, meteorological parameters, gaseous compounds and cloud condensation nuclei (CCN) activity were performed during different shorter occasions. K-means clustering analysis of particle number size distributions on daily basis identified several clusters. Clusters of accumulation mode aerosols (main size modes > 100 nm) accounted for 56% of the total aerosol during the sampling period (89-91% during February-April, 1-3% during June-August). By association to chemical composition, cloud condensation nuclei properties, and meteorological variables, three typical accumulation mode aerosol clusters were identified: Haze (32% of the time), Bimodal (14%) and Aged (6%). In brief: (1) Haze accumulation mode aerosol shows a single mode at 150 nm, peaking in February-April, with highest loadings of sulfate and black carbon concentrations. (2) Accumulation mode Bimodal aerosol shows two modes, at 38 nm and 150 nm, peaking in June-August, with the highest ratio of organics to sulfate concentrations. (3) Aged accumulation mode aerosol shows a single mode at 213 nm, peaking in September-October and is associated with cloudy and humid weather conditions during autumn. The three aerosol clusters were considered alongside CCN concentrations. We suggest that organic compounds, that are likely marine biogenic in nature, greatly influence the Bimodal cluster and contribute significantly to its CCN activity. This stresses the importance of better characterizing the marine ecosystem and the aerosol-mediated climate effects in the

Characteristics and composition of atmospheric aerosols in Phimai, central Thailand during BASE-ASIA

Science.gov (United States)

Li, Can; Tsay, Si-Chee; Hsu, N. Christina; Kim, Jin Young; Howell, Steven G.; Huebert, Barry J.; Ji, Qiang; Jeong, Myeong-Jae; Wang, Sheng-Hsiang; Hansell, Richard A.; Bell, Shaun W.

2013-10-01

Comprehensive measurements of atmospheric aerosols were made in Phimai, central Thailand (15.183°N, 102.565°E, elevation: 206 m) during the BASE-ASIA field experiment from late February to early May in 2006. The observed aerosol loading was sizable for this rural site (mean aerosol scattering: 108 ± 64 Mm-1; absorption: 15 ± 8 Mm-1; PM10 concentration: 33 ± 17 μg m-3), and dominated by submicron particles. Major aerosol compounds included carbonaceous (OC: 9.5 ± 3.6 μg m-3; EC: 2.0 ± 2.3 μg m-3) and secondary species (SO42-: 6.4 ± 3.7 μg m-3, NH4+: 2.2 ± 1.3 μg m-3). While the site was seldom under the direct influence of large forest fires to its north, agricultural fires were ubiquitous during the experiment, as suggested by the substantial concentration of K+ (0.56 ± 0.33 μg m-3). Besides biomass burning, aerosols in Phimai during the experiment were also strongly influenced by industrial and vehicular emissions from the Bangkok metropolitan region and long-range transport from southern China. High humidity played an important role in determining the aerosol composition and properties in the region. Sulfate was primarily formed via aqueous phase reactions, and hygroscopic growth could enhance the aerosol light scattering by up to 60%, at the typical morning RH level of 85%. The aerosol single scattering albedo demonstrated distinct diurnal variation, ranging from 0.86 ± 0.04 in the evening to 0.92 ± 0.02 in the morning. This experiment marks the first time such comprehensive characterization of aerosols was made for rural central Thailand. Our results indicate that aerosol pollution has developed into a regional problem for northern Indochina, and may become more severe as the region's population and economy continue to grow.

Investigation of short and long term trends in chemical composition of Eastern Mediterranean aerosols

International Nuclear Information System (INIS)

2011-01-01

A collaborative study was started with the Middle East Technical University, Environmental Engineering Department in 2004 in order to determine the transport of air pollutants and their deposition rates to Eastern Mediterranean with the ultimate aim of filling the gaps in knowledge on the current status of Eastern Mediterranean air quality profile. Collection sufficient amount of representative samples, analyzes of the collected samples with high accuracy and precision and interpretation of generated data are crucial efforts. To attain this goal, EDXRF spectrometer, which is a rapid, reliable and sensitive analytical instrument, located at our center was employed in analysis of the collected samples after calibration with 'NIST 2783 Air Particles on Filter'. The effectiveness of the control strategies taken on the emissions was discussed by investigating the short and long term variations in the chemical composition of samples collected between 1993 and 2001 at Antalya station. In this context, generated data set was studied for short (daily) term, seasonal and long term variations. It has been found that short term variations in the concentrations of pollutants in short time scale are highly episodic. The concentration of measured pollutants was changed 10-20 folds in the subsequent two days. The most important factors affecting the chemical composition of pollutants in short time interval are meteorological factors such as precipitation and variations observed at the emission strength of pollutants. The declined in Pb concentrations at the Antalya station was attributed to observed decrease in Pb emissions in Europe after the introduction of leaded gasoline. Highest summer averages were reported for anthropogenic pollutants in summer months. Aegean Sea (Izmir-Aliaga) studies of the project will be completed this year

NOAA's National Air Quality Prediction and Development of Aerosol and Atmospheric Composition Prediction Components for NGGPS

Science.gov (United States)

Stajner, I.; McQueen, J.; Lee, P.; Stein, A. F.; Wilczak, J. M.; Upadhayay, S.; daSilva, A.; Lu, C. H.; Grell, G. A.; Pierce, R. B.

2017-12-01

NOAA's operational air quality predictions of ozone, fine particulate matter (PM2.5) and wildfire smoke over the United States and airborne dust over the contiguous 48 states are distributed at http://airquality.weather.gov. The National Air Quality Forecast Capability (NAQFC) providing these predictions was updated in June 2017. Ozone and PM2.5 predictions are now produced using the system linking the Community Multiscale Air Quality model (CMAQ) version 5.0.2 with meteorological inputs from the North American Mesoscale Forecast System (NAM) version 4. Predictions of PM2.5 include intermittent dust emissions and wildfire emissions from an updated version of BlueSky system. For the latter, the CMAQ system is initialized by rerunning it over the previous 24 hours to include wildfire emissions at the time when they were observed from the satellites. Post processing to reduce the bias in PM2.5 prediction was updated using the Kalman filter analog (KFAN) technique. Dust related aerosol species at the CMAQ domain lateral boundaries now come from the NEMS Global Aerosol Component (NGAC) v2 predictions. Further development of NAQFC includes testing of CMAQ predictions to 72 hours, Canadian fire emissions data from Environment and Climate Change Canada (ECCC) and the KFAN technique to reduce bias in ozone predictions. NOAA is developing the Next Generation Global Predictions System (NGGPS) with an aerosol and gaseous atmospheric composition component to improve and integrate aerosol and ozone predictions and evaluate their impacts on physics, data assimilation and weather prediction. Efforts are underway to improve cloud microphysics, investigate aerosol effects and include representations of atmospheric composition of varying complexity into NGGPS: from the operational ozone parameterization, GOCART aerosols, with simplified ozone chemistry, to CMAQ chemistry with aerosol modules. We will present progress on community building, planning and development of NGGPS.

Ubiquitous influence of wildfire emissions and secondary organic aerosol on summertime atmospheric aerosol in the forested Great Lakes region

Science.gov (United States)

Gunsch, Matthew J.; May, Nathaniel W.; Wen, Miao; Bottenus, Courtney L. H.; Gardner, Daniel J.; VanReken, Timothy M.; Bertman, Steven B.; Hopke, Philip K.; Ault, Andrew P.; Pratt, Kerri A.

2018-03-01

Long-range aerosol transport affects locations hundreds of kilometers from the point of emission, leading to distant particle sources influencing rural environments that have few major local sources. Source apportionment was conducted using real-time aerosol chemistry measurements made in July 2014 at the forested University of Michigan Biological Station near Pellston, Michigan, a site representative of the remote forested Great Lakes region. Size-resolved chemical composition of individual 0.5-2.0 µm particles was measured using an aerosol time-of-flight mass spectrometer (ATOFMS), and non-refractory aerosol mass less than 1 µm (PM1) was measured with a high-resolution aerosol mass spectrometer (HR-AMS). The field site was influenced by air masses transporting Canadian wildfire emissions and urban pollution from Milwaukee and Chicago. During wildfire-influenced periods, 0.5-2.0 µm particles were primarily aged biomass burning particles (88 % by number). These particles were heavily coated with secondary organic aerosol (SOA) formed during transport, with organics (average O/C ratio of 0.8) contributing 89 % of the PM1 mass. During urban-influenced periods, organic carbon, elemental carbon-organic carbon, and aged biomass burning particles were identified, with inorganic secondary species (ammonium, sulfate, and nitrate) contributing 41 % of the PM1 mass, indicative of atmospheric processing. With current models underpredicting organic carbon in this region and biomass burning being the largest combustion contributor to SOA by mass, these results highlight the importance for regional chemical transport models to accurately predict the impact of long-range transported particles on air quality in the upper Midwest, United States, particularly considering increasing intensity and frequency of Canadian wildfires.

The impact of changing surface ocean conditions on the dissolution of aerosol iron

Science.gov (United States)

Fishwick, Matthew P.; Sedwick, Peter N.; Lohan, Maeve C.; Worsfold, Paul J.; Buck, Kristen N.; Church, Thomas M.; Ussher, Simon J.

2014-11-01

The proportion of aerosol iron (Fe) that dissolves in seawater varies greatly and is dependent on aerosol composition and the physicochemical conditions of seawater, which may change depending on location or be altered by global environmental change. Aerosol and surface seawater samples were collected in the Sargasso Sea and used to investigate the impact of these changing conditions on aerosol Fe dissolution in seawater. Our data show that seawater temperature, pH, and oxygen concentration, within the range of current and projected future values, had no significant effect on the dissolution of aerosol Fe. However, the source and composition of aerosols had the most significant effect on the aerosol Fe solubility, with the most anthropogenically influenced samples having the highest fractional solubility (up to 3.2%). The impact of ocean warming and acidification on aerosol Fe dissolution is therefore unlikely to be as important as changes in land usage and fossil fuel combustion. Our experimental results also reveal important changes in the size distribution of soluble aerosol Fe in solution, depending on the chemical conditions of seawater. Under typical conditions, the majority (77-100%) of Fe released from aerosols into ambient seawater existed in the colloidal (0.02-0.4 µm) size fraction. However, in the presence of a sufficient concentration of strong Fe-binding organic ligands (10 nM) most of the aerosol-derived colloidal Fe was converted to soluble Fe (<0.02 µm). This finding highlights the potential importance of organic ligands in retaining aerosol Fe in a biologically available form in the surface ocean.

Case studies on the chemical composition of fogwater: The influence of local gaseous emissions

Science.gov (United States)

Johnson, C. Annette; Sigg, Laura; Zobrist, Jürg

In order to study the mechanisms governing the composition of fogwater, sequential samples were taken during two fog events over several hours and analyzed chemically. In addition, preliminary measurements of gases (HCl, HNO 3, NH 3) and aerosols (H 2SO 4, NH 4NO 3, NH 4Cl and ammonium sulfates) were made. The uptake of gaseous HCl in the fog droplets was a major source of acidity: in extreme cases pH values of 2.08 and 1.94 and Cl - concentrations up to 10 -2 M were observed. HCl originated from a local source, most probably a refuse incinerator from which plumes of the stack gas reached the sampling site. The NH +4, NO -3 and SO -24 concentrations (in the range of 0.1-2 mrnol l-1) were regulated by the inputs of aerosols and the liquid water content of the fog. The contribution of dissolved S(IV) (0.06-0.27 mmol l-1) to the total aqueous sulfur varied with time, according to the pH-dependent solubility of SO 2 and to oxidation reactions.

Properties of aerosols and formation mechanisms over southern China during the monsoon season

Science.gov (United States)

Chen, Weihua; Wang, Xuemei; Blake Cohen, Jason; Zhou, Shengzhen; Zhang, Zhisheng; Chang, Ming; Chan, Chuen-Yu

2016-10-01

Measurements of size-resolved aerosols from 0.25 to 18 µm were conducted at three sites (urban, suburban and background sites) and used in tandem with an atmospheric transport model to study the size distribution and formation of atmospheric aerosols in southern China during the monsoon season (May-June) in 2010. The mass distribution showed the majority of chemical components were found in the smaller size bins (water and anticorrelated with atmospheric SO2, hinting at aqueous-phase reactions being the main formation pathway. Nitrate was the only major species that showed a bimodal distribution at the urban site and was dominated by the coarse mode in the other two sites, suggesting that an important component of nitrate formation is chloride depletion of sea salt transported from the South China Sea. In addition to these aqueous-phase reactions and interactions with sea salt aerosols, new particle formation, chemical aging, and long-range transport from upwind urban or biomass burning regions was also found to be important in at least some of the sites on some of the days. This work therefore summarizes the different mechanisms that significantly impact the aerosol chemical composition during the monsoon over southern China.

Influence of particle size and chemistry on the cloud nucleating properties of aerosols

Directory of Open Access Journals (Sweden)

P. K. Quinn

2008-02-01

Full Text Available The ability of an aerosol particle to act as a cloud condensation nuclei (CCN is a function of the size of the particle, its composition and mixing state, and the supersaturation of the cloud. In-situ data from field studies provide a means to assess the relative importance of these parameters. During the 2006 Texas Air Quality – Gulf of Mexico Atmospheric Composition and Climate Study (TexAQS-GoMACCS, the NOAA RV Ronald H. Brown encountered a wide variety of aerosol types ranging from marine near the Florida panhandle to urban and industrial in the Houston-Galveston area. These varied sources provided an opportunity to investigate the role of aerosol sources and chemistry in the potential activation of particles to form cloud droplets. Measurements were made of CCN concentrations, aerosol chemical composition in the size range relevant for particle activation in warm clouds, and aerosol size distributions. Variability in aerosol composition was parameterized by the mass fraction of Hydrocarbon-like Organic Aerosol (HOA for particle diameters less than 200 nm (vacuum aerodynamic. The HOA mass fraction in this size range was lowest for marine aerosol and highest for aerosol sampled close to anthropogenic sources. Combining all data from the experiment reveals that composition (defined by HOA mass fraction explains 40% of the variance in the critical diameter for particle activation at the instrumental supersaturation (S of 0.44%. Correlations between HOA mass fraction and aerosol mean diameter show that these two parameters are essentially independent of one another for this data set. We conclude that, based on the variability of the HOA mass fraction observed during TexAQS-GoMACCS, variability in particle composition played a significant role in determining the fraction of particles that could activate to form cloud droplets. Using a simple model based on Köhler theory and the assumption that HOA is insoluble, we estimate the

Wintertime water-soluble aerosol composition and particle water content in Fresno, California

Science.gov (United States)

Parworth, Caroline L.; Young, Dominique E.; Kim, Hwajin; Zhang, Xiaolu; Cappa, Christopher D.; Collier, Sonya; Zhang, Qi

2017-03-01

The composition and concentrations of water-soluble gases and ionic aerosol components were measured from January to February 2013 in Fresno, CA, with a particle-into-liquid sampler with ion chromatography and annular denuders. The average (±1σ) ionic aerosol mass concentration was 15.0 (±9.4) µg m-3, and dominated by nitrate (61%), followed by ammonium, sulfate, chloride, potassium, nitrite, and sodium. Aerosol-phase organic acids, including formate and glycolate, and amines including methylaminium, triethanolaminium, ethanolaminium, dimethylaminium, and ethylaminium were also detected. Although the dominant species all came from secondary aerosol formation, there were primary sources of ionic aerosols as well, including biomass burning for potassium and glycolate, sea spray for sodium, chloride, and dimethylamine, and vehicles for formate. Particulate methanesulfonic acid was also detected and mainly associated with terrestrial sources. On average, the molar concentration of ammonia was 49 times greater than nitric acid, indicating that ammonium nitrate formation was limited by nitric acid availability. Particle water was calculated based on the Extended Aerosol Inorganics Model (E-AIM) thermodynamic prediction of inorganic particle water and κ-Köhler theory approximation of organic particle water. The average (±1σ) particle water concentration was 19.2 (±18.6) µg m-3, of which 90% was attributed to inorganic species. The fractional contribution of particle water to total fine particle mass averaged at 36% during this study and was greatest during early morning and night and least during the day. Based on aqueous-phase concentrations of ions calculated by using E-AIM, the average (±1σ) pH of particles in Fresno during the winter was estimated to be 4.2 (±0.2).

The Atmospheric Aerosols And Their Effects On Cloud Albedo And Radiative Forcing

International Nuclear Information System (INIS)

Stefan, S.; Iorga, G.; Zoran, M.

2007-01-01

The aim of this study is to provide results of the theoretical experiments in order to improve the estimates of indirect effect of aerosol on the cloud albedo and consequently on the radiative forcing. The cloud properties could be changed primarily because of changing of both the aerosol type and concentration in the atmosphere. Only a part of aerosol interacts effectively with water and will, in turn, determine the number concentration of cloud droplets (CDNC). We calculated the CDNC, droplet effective radius (reff), cloud optical thickness (or), cloud albedo and radiative forcing, for various types of aerosol. Our results show into what extent the change of aerosol characteristics (number concentration and chemical composition) on a regional scale can modify the cloud reflectivity. Higher values for cloud albedo in the case of the continental (urban) clouds were obtained

Modelling of primary aerosols in the chemical transport model MOCAGE: development and evaluation of aerosol physical parameterizations

Directory of Open Access Journals (Sweden)

B. Sič

2015-02-01

Full Text Available This paper deals with recent improvements to the global chemical transport model of Météo-France MOCAGE (Modèle de Chimie Atmosphérique à Grande Echelle that consists of updates to different aerosol parameterizations. MOCAGE only contains primary aerosol species: desert dust, sea salt, black carbon, organic carbon, and also volcanic ash in the case of large volcanic eruptions. We introduced important changes to the aerosol parameterization concerning emissions, wet deposition and sedimentation. For the emissions, size distribution and wind calculations are modified for desert dust aerosols, and a surface sea temperature dependant source function is introduced for sea salt aerosols. Wet deposition is modified toward a more physically realistic representation by introducing re-evaporation of falling rain and snowfall scavenging and by changing the in-cloud scavenging scheme along with calculations of precipitation cloud cover and rain properties. The sedimentation scheme update includes changes regarding the stability and viscosity calculations. Independent data from satellites (MODIS, SEVIRI, the ground (AERONET, EMEP, and a model inter-comparison project (AeroCom are compared with MOCAGE simulations and show that the introduced changes brought a significant improvement on aerosol representation, properties and global distribution. Emitted quantities of desert dust and sea salt, as well their lifetimes, moved closer towards values of AeroCom estimates and the multi-model average. When comparing the model simulations with MODIS aerosol optical depth (AOD observations over the oceans, the updated model configuration shows a decrease in the modified normalized mean bias (MNMB; from 0.42 to 0.10 and a better correlation (from 0.06 to 0.32 in terms of the geographical distribution and the temporal variability. The updates corrected a strong positive MNMB in the sea salt representation at high latitudes (from 0.65 to 0.16, and a negative MNMB in

Halogenation processes of secondary organic aerosol and implications on halogen release mechanisms

Directory of Open Access Journals (Sweden)

J. Ofner

2012-07-01

Full Text Available Reactive halogen species (RHS, such as X·, X₂ and HOX containing X = chlorine and/or bromine, are released by various sources like photo-activated sea-salt aerosol or from salt pans, and salt lakes. Despite many studies of RHS reactions, the potential of RHS reacting with secondary organic aerosol (SOA and organic aerosol derived from biomass-burning (BBOA has been neglected. Such reactions can constitute sources of gaseous organohalogen compounds or halogenated organic matter in the tropospheric boundary layer and can influence physicochemical properties of atmospheric aerosols.

Model SOA from α-pinene, catechol, and guaiacol was used to study heterogeneous interactions with RHS. Particles were exposed to molecular chlorine and bromine in an aerosol smog-chamber in the presence of UV/VIS irradiation and to RHS, released from simulated natural halogen sources like salt pans. Subsequently, the aerosol was characterized in detail using a variety of physicochemical and spectroscopic methods. Fundamental features were correlated with heterogeneous halogenation, which results in new functional groups (FTIR spectroscopy, changes UV/VIS absorption, chemical composition (ultrahigh resolution mass spectroscopy (ICR-FT/MS, or aerosol size distribution. However, the halogen release mechanisms were also found to be affected by the presence of organic aerosol. Those interaction processes, changing chemical and physical properties of the aerosol are likely to influence e.g. the ability of the aerosol to act as cloud condensation nuclei, its potential to adsorb other gases with low-volatility, or its contribution to radiative forcing and ultimately the Earth's radiation balance.

Seasonal variability of aerosol concentration and size distribution in Cape Verde using a continuous aerosol optical spectrometer

Directory of Open Access Journals (Sweden)

Casimiro Adrião Pio

2014-05-01

Full Text Available One year of, almost continuous, measurements of aerosol optical properties and chemical composition were performed at the outskirts of Praia, Santiago Island, Cape Verde, within the framework of CV-DUST (Atmospheric aerosol in Cape Verde region: seasonal evaluation of composition, sources and transport research project, during 2011. This article reports the aerosol number and mass concentration measurements using a GRIMM Optical Aerosol Spectrometer that provides number size discrimination into 31 size ranges from 0.25 to 32 µm. Time series of 5 min average PM10 concentrations revealed peak values higher than 1000 µg.m-3 during winter dust storm events originating over Northern Africa. The 24 hours average concentrations exceeded the World Health Organization (WHO guidelines for PM2.5 and PM10 in 20% and 30% of the 2001 days, respectively. Annual average mass concentrations (±standard deviation for PM1, PM2.5 and PM10 were 5±5, 19±21 and 48±64 µg.m-3, respectively. The annual PM2.5 and PM10 values were also above the limits prescribed by the WHO (10 and 20 µg.m-3, respectively. The aerosol mass size distribution revealed two main modes for particles smaller than 10 µm: a fine mode (0.7-0.8 µm, which possibly results of gas to particle conversion processes; and a coarse mode with maxima at 3-4 µm, which is associated with desert dust and sea salt sources. Within the coarse mode two sub-modes with maxima at 5-6 µm and 10-12 µm were frequently present.

Changes in the physico-chemical properties of Amazonian aerosols from background conditions due to urban impacts in Central Amazonia.

Science.gov (United States)

Artaxo, P.; Barbosa, H. M.; Brito, J.; Carbone, S.; Fiorese, C.; Andre, B.; Rizzo, L. V.; Ditas, F.; Pöhlker, C.; Pöhlker, M. L.; Saturno, J.; Holanda, B. A.; Wang, J.; Souza, R. A. F. D.; Machado, L.; Andreae, M. O.; Martin, S. T.

2016-12-01

The GoAmazon 2014/15 experiment (Observations and Modeling of the Green Ocean Amazon) was a great opportunity to study how urbanization can change aerosol properties under pristine conditions in a tropical rain forest. The experiment took place from January 2014 to December 2015 in the vicinity of Manaus, Brazil, where several sampling stations were operated. Natural biogenic aerosol properties were studied in 3 sampling stations upwind of Manaus (ATTO (T0a), ZF2 (T0z) and EMBRAPA (T0e)). Urban impacted aerosols were analysed in two downwind sampling stations at Tiwa (T2) and Manacapuru (T3). Properties analysed were size distribution, scattering and absorption, composition, vertical profiles and others. Remote sensing measurements were done using AERONET and MODIS, while extensive ground based measurements were done in all sampling stations. Remote sensing measurements shows important changes in aerosol optical depth (AOD), especially in the aerosol absorption component. It was also observed a reduction in cloud droplet size downwind of Manaus for liquid phase clouds. Changes in particle number and size were also very significant, that reflected in changes in the aerosol radiative forcing (RF) before and after Manaus plume. In the dry season, an average RF of -24 w/m² was observed upwind, while -17 w/m² was observed downwind, due to large scale biomass burning aerosols. Single scattering albedo (SSA) at 550 nm changed from a high value of 0.96 upwind to 0.84 downwind due to the increase in absorbing aerosols in the wet season. In the dry season, SSA at 550nm changed from 0.95 to 0.87. Aerosol composition showed a large dominance of organic aerosols for all sites, accounting for 65-75% of PM1 non refractory aerosol. Most of these were secondary organic aerosol (SOA), with very low sulfate and nitrate concentrations. The influence of the Manaus plume on aerosol properties was more intense during the wet season, because in the dry season a significant amount of

Probing functional groups at the gas-aerosol interface using heterogeneous titration reactions: a tool for predicting aerosol health effects?

Science.gov (United States)

Setyan, Ari; Sauvain, Jean-Jacques; Guillemin, Michel; Riediker, Michael; Demirdjian, Benjamin; Rossi, Michel J

2010-12-17

The complex chemical and physical nature of combustion and secondary organic aerosols (SOAs) in general precludes the complete characterization of both bulk and interfacial components. The bulk composition reveals the history of the growth process and therefore the source region, whereas the interface controls--to a large extent--the interaction with gases, biological membranes, and solid supports. We summarize the development of a soft interrogation technique, using heterogeneous chemistry, for the interfacial functional groups of selected probe gases [N(CH(3))(3), NH(2)OH, CF(3)COOH, HCl, O(3), NO(2)] of different reactivity. The technique reveals the identity and density of surface functional groups. Examples include acidic and basic sites, olefinic and polycyclic aromatic hydrocarbon (PAH) sites, and partially and completely oxidized surface sites. We report on the surface composition and oxidation states of laboratory-generated aerosols and of aerosols sampled in several bus depots. In the latter case, the biomarker 8-hydroxy-2'-deoxyguanosine, signaling oxidative stress caused by aerosol exposure, was isolated. The increase in biomarker levels over a working day is correlated with the surface density N(i)(O3) of olefinic and/or PAH sites obtained from O(3) uptakes as well as with the initial uptake coefficient, γ(0), of five probe gases used in the field. This correlation with γ(0) suggests the idea of competing pathways occurring at the interface of the aerosol particles between the generation of reactive oxygen species (ROS) responsible for oxidative stress and cellular antioxidants.

Where and What Is Pristine Marine Aerosol?

Science.gov (United States)

Russell, L. M.; Frossard, A. A.; Long, M. S.; Burrows, S. M.; Elliott, S.; Bates, T. S.; Quinn, P.

2014-12-01

The sources and composition of atmospheric marine aerosol particles have been measured by functional group composition (from Fourier transform infrared spectroscopy) to identify the organic composition of the pristine primary marine (ocean-derived) particles as 65% hydroxyl, 21% alkane, 6% amine, and 7% carboxylic acid functional groups [Frossard et al., 2014a,b]. Pristine but non-primary components from photochemical reactions (likely from biogenic marine vapor emissions) add carboxylic acid groups. Non-pristine contributions include shipping effluent in seawater and ship emissions, which add additional alkane groups (up to 70%), and coastal or continental emissions mix in alkane and carboxylic acid groups. The pristine primary marine (ocean-derived) organic aerosol composition is nearly identical to model generated primary marine aerosol particles from bubbled seawater, indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. While the seawater organic functional group composition was nearly invariant across all three ocean regions studied and the ratio of organic carbon to sodium (OC/Na+) in the generated primary marine aerosol particles remained nearly constant over a broad range of chlorophyll-a concentrations, the generated primary marine aerosol particle alkane group fraction increased with chlorophyll-a concentrations. In addition, the generated primary marine aerosol particles have a hydroxyl group absorption peak location characteristic of monosaccharides and disaccharides, where the seawater hydroxyl group peak location is closer to that of polysaccharides. References Cited Frossard, Amanda A., Lynn M. Russell, Paola Massoli, Timothy S. Bates, and Patricia K. Quinn, "Side-by-Side Comparison of Four Techniques Explains the Apparent Differences in the Organic Composition of Generated and Ambient Marine Aerosol Particles," Aerosol Science and Technology - Aerosol Research Letter

Molecular Diversity of Sea Spray Aerosol Particles: Impact of Ocean Biology on Particle Composition and Hygroscopicity

Energy Technology Data Exchange (ETDEWEB)

Cochran, Richard E.; Laskina, Olga; Trueblood, Jonathan; Estillore, Armando D.; Morris, Holly S.; Jayarathne, Thilina; Sultana, Camile M.; Lee, Christopher; Lin, Peng; Laskin, Julia; Laskin, Alexander; Dowling, Jackie; Qin, Zhen; Cappa, Christopher; Bertram, Timothy; Tivanski, Alexei V.; Stone, Elizabeth; Prather, Kimberly; Grassian, Vicki H.

2017-05-01

The impact of sea spray aerosol (SSA) on climate depends on the size and chemical composition of individual particles that make-up the total SSA ensemble. While the organic fraction of SSA has been characterized from a bulk perspective, there remains a lack of understanding as to the composition of individual particles within the SSA ensemble. To better understand the molecular components within SSA particles and how SSA composition changes with ocean biology, simultaneous measurements of seawater and SSA were made during a month-long mesocosm experiment performed in an ocean-atmosphere facility. Herein, we deconvolute the composition of freshly emitted SSA devoid of anthropogenic and terrestrial influences by characterizing classes of organic compounds as well as specific molecules within individual SSA particles. Analysis of SSA particles show that the diversity of molecules within the organic fraction varies between two size fractions (submicron and supermicron) with contributions from fatty acids, monosaccharides, polysaccharides and siliceous material. Significant changes in the distribution of these compounds within individual particles are observed to coincide with the rise and fall of phytoplankton and bacterial populations within the seawater. Furthermore, water uptake is impacted as shown by hygroscopicity measurements of model systems composed of representative organic compounds. Thus, the how changes in the hygroscopic growth of SSA evolves with composition can be elucidated. Overall, this study provides an important connection between biological processes that control the composition of seawater and changes in single particle composition which will enhances our ability to predict the impact of SSA on climate.

Combustion aerosols from potassium-containing fuels

Energy Technology Data Exchange (ETDEWEB)

Balzer Nielsen, Lars

1999-12-31

The scope of the work presented in this thesis is the formation and evolution of aerosol particles in the submicron range during combustion processes, in particular where biomass is used alone or co-fired with coal. An introduction to the formation processes of fly ash in general and submicron aerosol in particular during combustion is presented, along with some known problems related to combustion of biomass for power generation. The work falls in two parts. The first is the design of a laboratory setup for investigation of homogeneous nucleation and particle dynamics at high temperature. The central unit of the setup is a laminar flow aerosol condenser (LFAC), which essentially is a 173 cm long tubular furnace with an externally cooled wall. A mathematical model is presented which describes the formation and evolution of the aerosol in the LFAC, where the rate of formation of new nuclei is calculated using the so-called classical theory. The model includes mass and energy conservation equations and an expression for the description of particle growth by diffusion. The resulting set of nonlinear second-order partial differential equations are solved numerically using the method of orthogonal collocation. The model is implemented in the FORTRAN code MONAERO. The second part of this thesis describes a comprehensive investigation of submicron aerosol formation during co-firing of coal and straw carried out at a 380 MW{sub Th} pulverized coal unit at Studstrup Power Plant, Aarhus. Three types of coal are used, and total boiler load and straw input is varied systematically. Straw contains large amounts of potassium, which is released during combustion. Submicron aerosol is sampled between the two banks of the economizer at a flue gas temperature of 350 deg. C using a novel ejector probe. The aerosol is characterized using the SMPS system and a Berner-type low pressure impactor. The chemical composition of the particles collected in the impactor is determined using

Combustion aerosols from potassium-containing fuels

International Nuclear Information System (INIS)

Balzer Nielsen, Lars

1998-01-01

The scope of the work presented in this thesis is the formation and evolution of aerosol particles in the submicron range during combustion processes, in particular where biomass is used alone or co-fired with coal. An introduction to the formation processes of fly ash in general and submicron aerosol in particular during combustion is presented, along with some known problems related to combustion of biomass for power generation. The work falls in two parts. The first is the design of a laboratory setup for investigation of homogeneous nucleation and particle dynamics at high temperature. The central unit of the setup is a laminar flow aerosol condenser (LFAC), which essentially is a 173 cm long tubular furnace with an externally cooled wall. A mathematical model is presented which describes the formation and evolution of the aerosol in the LFAC, where the rate of formation of new nuclei is calculated using the so-called classical theory. The model includes mass and energy conservation equations and an expression for the description of particle growth by diffusion. The resulting set of nonlinear second-order partial differential equations are solved numerically using the method of orthogonal collocation. The model is implemented in the FORTRAN code MONAERO. The second part of this thesis describes a comprehensive investigation of submicron aerosol formation during co-firing of coal and straw carried out at a 380 MW Th pulverized coal unit at Studstrup Power Plant, Aarhus. Three types of coal are used, and total boiler load and straw input is varied systematically. Straw contains large amounts of potassium, which is released during combustion. Submicron aerosol is sampled between the two banks of the economizer at a flue gas temperature of 350 deg. C using a novel ejector probe. The aerosol is characterized using the SMPS system and a Berner-type low pressure impactor. The chemical composition of the particles collected in the impactor is determined using chemical

Combustion aerosols from potassium-containing fuels

Energy Technology Data Exchange (ETDEWEB)

Balzer Nielsen, Lars

1998-12-31

The scope of the work presented in this thesis is the formation and evolution of aerosol particles in the submicron range during combustion processes, in particular where biomass is used alone or co-fired with coal. An introduction to the formation processes of fly ash in general and submicron aerosol in particular during combustion is presented, along with some known problems related to combustion of biomass for power generation. The work falls in two parts. The first is the design of a laboratory setup for investigation of homogeneous nucleation and particle dynamics at high temperature. The central unit of the setup is a laminar flow aerosol condenser (LFAC), which essentially is a 173 cm long tubular furnace with an externally cooled wall. A mathematical model is presented which describes the formation and evolution of the aerosol in the LFAC, where the rate of formation of new nuclei is calculated using the so-called classical theory. The model includes mass and energy conservation equations and an expression for the description of particle growth by diffusion. The resulting set of nonlinear second-order partial differential equations are solved numerically using the method of orthogonal collocation. The model is implemented in the FORTRAN code MONAERO. The second part of this thesis describes a comprehensive investigation of submicron aerosol formation during co-firing of coal and straw carried out at a 380 MW{sub Th} pulverized coal unit at Studstrup Power Plant, Aarhus. Three types of coal are used, and total boiler load and straw input is varied systematically. Straw contains large amounts of potassium, which is released during combustion. Submicron aerosol is sampled between the two banks of the economizer at a flue gas temperature of 350 deg. C using a novel ejector probe. The aerosol is characterized using the SMPS system and a Berner-type low pressure impactor. The chemical composition of the particles collected in the impactor is determined using